Ma muli o nā pilikia o ke kaiapuni a me ka hoʻololi ʻana o ka ikehu, hoʻemi ʻia ka electrochemical CO2 (ECR) i nā wahie multicarbon (C2+) i hoʻohui ʻia (C2+) a me nā kemika, me ka hoʻohana ʻana i ka uila hiki ke hoʻololi ʻia, ke hāʻawi nei i kahi hopena lōʻihi e pani ai i ka pōʻai kalapona me nā pono waiwai hoʻohui pū kekahi.Eia nō naʻe, ʻo ka hoʻopili ʻana i ka electrocatalytic C─C i loko o nā electrolytes wai he paʻakikī paʻakikī ma muli o ke koho haʻahaʻa, hana, a me ka paʻa.ʻO ka hoʻolālā ʻana o nā catalysts a me nā reactors ke kī i ka hoʻoponopono ʻana i kēlā mau pilikia.Hōʻuluʻulu mākou i ka holomua hou i ka hoʻokō ʻana i ka hui C─C maikaʻi ma o ECR, me ka manaʻo nui i nā hoʻolālā i ka electrocatalysts a me ka electrocatalytic electrode/reactor design, a me kā lākou mau hana pili.Eia kekahi, kūkākūkā ʻia nā bottlenecks o kēia manawa a me nā manawa e hiki mai ana no ka hoʻokumu huahana C2 +.Manaʻo mākou e hāʻawi i kahi loiloi kikoʻī o nā hoʻolālā hoʻohui C─C hou i ke kaiāulu no ka hoʻomohala hou a me ka hoʻoikaika ʻana i ka ʻike kumu a me nā noi ʻenehana.

ʻO ka hoʻokuʻu nui ʻana o ka carbon dioxide (CO2) i loko o ka lewa ua hoʻoulu i nā hopena kūlohelohe koʻikoʻi a ke hōʻike nei hoʻi i kahi hoʻoweliweli koʻikoʻi a hiki ʻole ke hoʻohuli ʻia i nā hui kanaka (1, 2).I ka piʻi nui ʻana o ka manaʻo CO2 o ka lewa mai ka 270 ppm (mau ʻāpana o ka miliona) i ka 1800s mua a hiki i 401.3 ppm i Iulai 2015, ua loaʻa ka manaʻo o ka honua holoʻokoʻa no ka hana hou ʻana i ka wāwae kalapona i hoʻoiho ʻia e nā hana kanaka (3, 4).No ka hoʻomaopopo ʻana i ka loop loop pili no ka carbon footprint, hoʻokahi ala hiki ke hoʻololi i ka hilinaʻi o ka ikehu o kēia manawa a me nā ʻoihana kemika mai nā wahie fossil i nā kumu hou e like me ka lā a me ka makani (5-8).Eia nō naʻe, ʻo ka hapa o ka ikehu mai kēlā mau kumu hoʻohou i kaupalena ʻia i 30% ma muli o ko lākou ʻano intermittent, ke ʻole e loaʻa nā ala no ka mālama ʻana i ka ikehu nui (9).No laila, ma ke ʻano he ʻokoʻa, ʻoi aku ka maʻalahi o ka hopu ʻana i CO2 mai nā kumu kiko e like me nā mea kanu mana, a ukali ʻia e ka hoʻololi ʻana i nā meaʻai kemika a me nā wahie (9-12).ʻO ka Electrocatalytic CO2 reduction (ECR) me ka hoʻohana ʻana i ka uila hiki ke hōʻike ʻia i kahi hopena lōʻihi nani ma muli o nā kūlana hana maʻalahi e pono ai no ka hoʻololi ʻana, kahi e hiki ai ke hana i nā huahana i hoʻohui ʻia (13).E like me ka mea i hōʻike ʻia ma ke kiʻi 1, ma kēia kaʻina hana, hoʻololi ka electrochemical electrolyzer i ka CO2 a me ka wai i kemika a me nā wahie i hoʻohana ʻia e ka uila hiki ke hoʻololi ʻia.Hiki ke hoʻopaʻa ʻia ka wahie i ka wā lōʻihi a hiki ke puʻunaue ʻia a hoʻopau ʻia paha, e hāʻawi ana i ka CO2 i ka ʻōpala nui, e hopu ʻia a hāʻawi ʻia i ka reactor e pani i ka loop.Eia kekahi, hiki ke hoʻohana ʻia nā meaʻai kemika liʻiliʻi-mole [e laʻa, carbon monoxide (CO) a me ka formate] mai ECR i mea maka no ka hoʻohui ʻana i nā kemika paʻakikī.

Hiki ke loaʻa nā wahie a me nā kemika mai ka ECR me ka pōʻaiapuni kalapona pani ʻia e nā kumu ikehu hou e like me ka lā, ka makani, a me ka wai.Hoʻokani ka ʻenekinia kelepona a me ka ʻenehana catalyst i nā kuleana koʻikoʻi e hāpai i ka koho, hana, a me ka pono no ka hoʻololi ʻana o CO2 i nā huahana C2+ i hoʻohui ʻia me ka nui o ka ikehu kiʻekiʻe.

Eia naʻe, ʻo CO2 kahi molekele laina kūpaʻa me ka paʻa C═O ikaika (750 kJ mol−1) (14), e paʻakikī ana i ka hoʻololi electrochemical.No laila, pono ia i kahi pale ho'āla kiʻekiʻe, kahi e alakaʻi ai i nā overpotentials nui (15).Eia kekahi, ʻo ka ECR i loko o kahi electrolyte wai e pili ana i nā kaʻina hoʻololi multi-electron/proton me nā ʻano like ʻole o nā mea waena a me nā huahana (16-18), e paʻakikī loa ia.Hōʻuluʻulu ka Papa 1 i ka hapalua electrochemical thermodynamic reactions o nā huahana ECR nui, me CO, methane (CH4), methanol (CH3OH), formic acid (HCOOH), ethylene (C2H4), ethanol (CH3CH2OH), a pēlā aku, me ko lākou e pili ana i nā pono redox maʻamau (19).Ma keʻano laulā, i ka wā o ke kaʻina hana ECR, hoʻomaka mua nā molekala CO2 i ka adsorption a me ka pilina me nā ʻātoma ma ka ʻili catalyst e hana i *CO2−, a ukali ʻia e nā ʻano hoʻololi stepwise o nā protons a / a i ʻole nā ​​​​electrons i nā huahana hope loa.No ka laʻana, ua manaʻo ʻia e hana ʻia ʻo CH4 ma o kēia mau ala: CO2 → *COOH → *CO → *CHO → *CH2O → *CH3O → CH4 + *O → CH4 + *OH → CH4 + H2O (20).

Hōʻuluʻulu ka Figure 2A i ka maikaʻi o Faradaic (FE) ma lalo o nā kumukūʻai hana like ʻole (ka nui o kēia manawa) no nā electrocatalysts ECR i hōʻike ʻia, e hōʻike ana i ka koho huahana o ka hopena (21-43).ʻOiai, hiki i nā electrocatalysts hou ke hoʻololi i ka CO2 i nā huahana C1 (CO a i ʻole formate) me ka 95% FE ma lalo o ka nui o ka hana kiʻekiʻe (> 20 mA cm−2 no ka H-type cell a me> 100 mA cm− 2 no ka cell flow) (9, 21, 22, 25, 28, 44, 45), ka mea koho loa (> 90%) a me ka hana pono o nā kinikini multicarbon (C2+) i loaʻa ʻaʻole i ʻike ʻia i kēia manawa.ʻO kēia ma muli o ka hoʻohui ʻana i nā huahana C2+ e pono ai ka hōʻea ʻana a me ka adsorption o kekahi mau molekala CO2 i ka ʻili, ka hoʻololi stepwise, a me ke kūlana spatial (13).No ke kiko'ī, e like me ka mea i hōʻike ʻia ma ka Fig. 2B, ʻo nā hopena hope o nā *CO intermediates e hoʻoholo i nā huahana C2+ hope o ECR.Ma keʻano laulā, kaʻana like ʻo C2H6 a me CH3COO− i ka *CH2 waena, i hana ʻia mai nā ʻanuʻu hoʻololi electron-coupled proton o *CO.Hāʻawi ka protonation hou aʻe o *CH2 i ka *CH3 waena, e alakaʻi ana i ka hoʻokumu ʻana o C2H6 ma o *CH3 dimerization.ʻAʻole like me ka hanauna C2H6, hoʻokumu ʻia ʻo CH3COO− e ka hoʻokomo ʻana o CO i loko o *CH2.ʻO ka *CO dimerization ka pae hoʻoholo helu no ka hoʻokumu ʻana o C2H4, CH3CH2OH, a me n-propanol (n-C3H7OH).Ma hope o ke kaʻina o ka hoʻololi electron a me nā ʻanuʻu protonation, hoʻokumu ka *CO─CO dimer i ka *CH2CHO waena, kahi e hana ai ma ke ʻano he koho koho no C2H4 a me C2H5OH.Eia hou, ua ʻike ʻia ʻo ka hoʻemi ʻana i ka *CH2CHO i ka C2H4 he haʻahaʻa haʻahaʻa o ka ikehu ma mua o ka hoʻololi ʻana *CH3CHO i C2H5OH (46), hiki ke wehewehe i ka FE kiʻekiʻe no C2H4 ma luna o C2H5OH ma ka hapa nui o nā catalysts keleawe.Eia kekahi, hiki i nā mea waena C2 paʻa ke hoʻololi i n-C3H7OH ma o ka hoʻokomo CO.ʻO ke ala paʻakikī a hiki ʻole ke hoʻopaʻa ʻia i ka wā o ka hoʻokumu ʻana o ke kemika C2+ ma muli o ka nui o nā permutations i nā wahi protonation, me ka hiki ke komo ʻana o ka pae nonelectrochemical (19, 47).No laila, ʻo ka hoʻolālā ʻana o nā electrocatalysts koho nui he mea pono no ka hoʻokumu ʻana o ka huahana C2 + kikoʻī ma ka hua kiʻekiʻe.Ma kēia loiloi, manaʻo mākou e hōʻike i ka holomua hou o nā hoʻolālā i ka hoʻolālā electrocatalyst no ka hoʻokumu huahana C2 + koho ma o ECR.Hāʻawi pū mākou i kahi hōʻuluʻulu o nā ʻike o nā mīkini pili.E hoʻoikaika pū ʻia ka hoʻolālā electrode a me ka reactor e hōʻike pehea e hoʻokō ai i ka hana kūpono, kūpaʻa, a me ka nui o ka ECR.Eia kekahi, e kūkākūkā mākou i nā pilikia i koe a me nā manawa e hiki mai ana no ka hoʻololi electrochemical o CO2 i nā kemika C2 + i hoʻohui ʻia.

(A) ʻO ka FE ma lalo o nā kumukūʻai hana like ʻole (ka nui o kēia manawa) no nā electrocatalysts ECR i hōʻike ʻia (21-43, 130).(B) ʻO nā ala C2+ hiki loa i ka wā ECR.Hoʻopuka hou ʻia me ka ʻae mai ka American Chemical Society (47).

ʻO ka hoʻololi electrocatalytic o CO2 i loko o nā wahie kemika a me nā meaʻai meaʻai he ʻenehana hiki ke hoʻokō i kahi pōʻai ikehu kalapona-neutral (11).Eia nō naʻe, mamao loa ka FE o nā huahana C2+ mai ka hoʻohana pono ʻana, kahi e hiki ai i nā catalysts hou ke hana i nā huahana C2 me kahi o 60% FE (13, 33), aʻo ka hana C3 i kaupalena ʻia ma lalo o 10% FE (48, 49).ʻO ka hoʻohui hoʻohaʻahaʻa ʻana o nā huahana CO2 i C2+ e pono ai nā catalysts heterogeneous me nā waiwai morphological a me nā mea uila (50, 51).Pono ka ʻili catalytic e wāwahi i nā pilina scaling ma waena o nā mea waena (47, 52, 53).Eia kekahi, no ka hoʻokō ʻana i ka hoʻokumu ʻana i ka paʻa C─C, pono e hoʻokokoke ka hopena i hoʻopili ʻia ma ka ʻili catalyst.Eia kekahi, pono e hoʻomalu maikaʻi ʻia ke ala mai ka intermediate adsorbed mua i kahi huahana C2+ kikoʻī ma muli o nā ʻanuʻu hoʻololi electron kōkua proton.Ke noʻonoʻo nei i ka paʻakikī kiʻekiʻe o ka hoʻemi ʻana o CO2 i nā huahana C2 +, pono e hoʻopili pono ʻia nā electrocatalysts e hoʻonui i ka koho.Wahi a nā ʻano waena a me nā haku mele, hoʻokaʻawale mākou i nā huahana C2+ i nā hydrocarbon multicarbon a me nā oxygenates (4, 54).No ka hoʻokokoke ʻana i nā electrocatalysts maikaʻi loa no ka hana mole C2+ kikoʻī, ua hōʻike ʻia kekahi mau hoʻolālā hoʻolālā catalyst, e like me ka heteroatom doping, crystal facet regulation, alloy/dealloying, oxidation state tuning, a me ka mana ligand surface, ua hōʻike ʻia (35, 41, 55-61) .Pono ka hoʻolālā maikaʻi e noʻonoʻo pono i nā hopena i ʻōlelo ʻia a hoʻonui i nā pono.A i ʻole, ʻo ka hoʻomaopopo ʻana i ke kumu o ka pūnaewele hoʻoikaika e alakaʻi i kahi ʻano catalytic kūʻokoʻa e hoʻomālamalama hou aku i ka hoʻolālā catalyst pololei no ka hui ʻana o C─C.No laila, pehea e hoʻolālā ai i ka catalyst ECR e pili ana i nā huahana kikoʻī (multicarbon hydrocarbons a me oxygenates) a me nā hana pili e kūkākūkā ʻia ma kēia ʻāpana.

ʻO C2+ hydrocarbons, e like me C2H4, he mau kemika nexus no nā ʻoihana kemika like ʻole, e like me ka hana polyethylene (62, 63).Ma waho aʻe o kēia, hiki ke hoʻohana pololei ʻia e like me ka wahie no ka wili a i ʻole ka hui ʻana i loko o ke kinoea maoli (12).Ua hoʻohana ʻia ka Hydrogenation o CO (Fischer-Tropsch synthesis) a me CO2 no ka hana ʻana i nā hydrocarbons C2+ no ka manawa lōʻihi ma ka ʻenehana ʻoihana akā hoʻokūkū ʻia e ka hoʻohana ʻana i ka ikehu kiʻekiʻe a me ka hopena o ke kaiapuni (64).Ma kahi ʻokoʻa loa, hāʻawi ka hoʻemi ʻana o ka electrochemical CO2 me ka hoʻohana ʻana i ka ikehu hou i kahi ala maʻemaʻe a ʻoi aku ka hoʻomau.Ua hoʻoikaika nui ʻia e hoʻomohala i nā electrocatalysts maikaʻi i ka C2+ hydrocarbons (32, 33, 65–70).

Ua noiʻi nui ʻia nā bimetallic electrocatalysts e wāwahi i ka pilina scaling i ka wā o ka hoʻololi electrochemical CO2, hiki ke hoʻopaʻa i ke kī waena a hoʻohaʻahaʻa i ka overpotential a, no laila, hoʻonui i ka koho (71-74).ʻOiai ua hōʻike ʻia kahi pūʻulu o nā mea hao e like me Au-Cu, Ag-Cu, Au-Pd, a me Cu-Pt no ka hana kiʻekiʻe C1 ma o ka hoʻopaʻa ʻana i ka waena koʻikoʻi (73, 75), ʻike ʻia ka hopena alloy i ka C2+ hydrocarbon. e paʻakikī loa (76).No ka laʻana, i loko o ka ʻōnaehana Cu-Ag bimetallic, hiki ke hoʻopaʻa maʻalahi i ka hāʻawi ʻana i ka huahana ma ke kani ʻana i ka ratio atomic surface o Ag a me Cu (77).ʻOi aku ka maikaʻi o ka hāpana Cu-waiwai o ka ʻili no ka hana hydrocarbon, ʻoiai nā huahana o ka ʻili Ag-waiwai kekahi e noho aliʻi ʻia e CO, e hōʻike ana i ke koʻikoʻi o ka lākiō atomika no nā electrocatalysts ECR alloyed.ʻO ka hopena geometric i hoʻokumu ʻia e ka hoʻonohonoho atomic kūloko hiki ke hoʻopilikia nui i ka ikaika paʻa o nā mea waena.Ua hōʻike ʻo Gewirth a me nā hoa hana (36) ua hōʻike ʻia nā huila Cu-Ag mai ka electrodeposition hoʻohui ʻia i hoʻohui ʻia i ka ~ 60% FE no C2H4 i kahi electrolyzer kahe alkaline (Fig. 3, A a me B).I kēia hihia, hiki ke hoʻokō ʻia ka koho C2H4 i hoʻopaʻa ʻia e ka morphology a me ka hoʻokau ʻana iā Ag-loading.Ua manaʻo ʻia nā pūnaewele Ag i ke kuleana o ka mea hoʻolaha no ka hoʻokumu ʻana o CO i ka wā ECR.A laila, hiki i ka loaʻa maikaʻi loa o ka CO intermediate ke kōkua i ka hui ʻana o C─C i ka Cu e pili ana.Ma waho aʻe, hiki iā Ag ke hoʻoikaika i ka hoʻokumu ʻana o Cu2O i ka wā o ka Cu-Ag catalyst synthesis (Fig. 3C), e hopena i ka hoʻonui ʻana i ka hana hana C2H4.Ke wehe nei kēia synergy i nā mea hou no ka hoʻomohala ʻana i nā catalysts hui pū C─C.Eia kekahi, ʻo ke ʻano hui ʻana o nā metala like ʻole i ka ʻōnaehana alloy hiki ke hoʻoholo i ka hāʻawi ʻana i nā huahana ECR.Ke hoʻohana nei i ka Pd-Cu alloy ma ke ʻano he laʻana (Fig. 3D), Kenis a me nā hoa hana (71) i hōʻike i ka hiki ke hāʻawi i kahi catalyst Pd-Cu i hoʻokaʻawale ʻia i ka koho kiʻekiʻe loa (~ 50%) no C2H4 i hoʻohālikelike ʻia me kāna kauoha a me ka pilikia. nā hoa like.Wahi a ka manaʻo d-band, ʻo ka mea maʻamau, ʻo ka metala hoʻololi me kahi kikowaena d-band haʻahaʻa e hōʻike ana i ka nawaliwali o ka hoʻopaʻa ʻana o nā kikowaena in situ i hana ʻia ma nā ʻili metala (78).ʻOiai ʻo Pd-Cu alloy i hoʻokaʻawale ʻia e hōʻike i ka koho catalytic like a me ka hana no CO me Cu nanoparticles (NPs), hāʻawi ʻo ia i ka ikaika hoʻopaʻa ʻokoʻa loa i nā mea waena e ka Pd tuning.E like me ka mea i hōʻike ʻia ma ka Fig. 3E, ua hōʻike ʻia ka huila Cu-Pd i hoʻokaʻawale ʻia i ka haʻahaʻa haʻahaʻa, ʻoiai ʻo Cu NP ka mea kiʻekiʻe loa.Manaʻo ʻia ʻo ka hui Cu-Pd i hoʻokaʻawale ʻia i ka pae i loaʻa ka ikaika hoʻopaʻa haʻahaʻa loa no ka waena CO.Hōʻike kēia nānā ʻana i ka hopena geometric a me ka hoʻolālā ʻana i ʻoi aku ka nui ma mua o ka hopena uila no ka hoʻomaikaʻi ʻana i ka koho hydrocarbon i ka hihia hoʻokaʻawale Cu-Pd i hoʻokaʻawale ʻia.I kēia lā, ʻo ke keleawe maʻemaʻe a i ʻole nā ​​​​mea hoʻohui keleawe e hōʻike ana i ka koho maikaʻi a me ka hana no ka hoʻemi electrochemical o CO2 i C2+ hydrocarbons.No laila, pono e hoʻomohala i kahi electrocatalyst hou no ka C2+ hydrocarbon production mai ECR.Hoʻoulu ʻia e ka hydrogenation CO2, ua hōʻike ʻia kahi noiʻi mua e hiki ke hoʻohana ʻia ka huila Ni-Ga me nā ʻāpana like ʻole no ka hanauna C2H4 (79).Ua hōʻike ʻia e hiki i ke kiʻi Ni5Ga3 ke hōʻemi i ka CO2 i ka C2H4 a me ka ethane (C2H6).ʻOiai ʻoi aku ka liʻiliʻi o ka FE e pili ana i ka C2+ hydrocarbons ma mua o 5%, hiki iā ia ke wehe i nā laina hou no ka nānā ʻana i ka electrocatalyst i ka hui ʻana o C─C ma muli o ka hopena alloy.

(A i C) Cu-Ag bimetallic catalysts fabriced e additive-mana electrodeposition: (A) scanning electron microscopy (SEM) o Cu uwea, Cu-Ag poly, a me Cu-Ag uea a me (B) pili C2H4 FE.(C) EXAFS ua hōʻike ʻia ua hui like ʻia ka uea Cu-Ag a ua hōʻike ʻia ʻo Cu(I) oxide.Hoʻopuka hou ʻia (A) a (C) me ka ʻae mai ka American Chemical Society (36).(D a me E) Nā mea hoʻoheheʻe Cu-Pd me nā ʻano hui like ʻole: (D) Kiʻi kiʻi, nā kiʻi microscopy electron transmission (TEM), a me ka ikehu-dispersive spectroscopy element palapala 'āina o nā ʻāpana Cu-Pd i hoʻokaʻawale ʻia, hoʻokaʻawale ʻia a me ka (E) ) ili valence band photoemission spectra a me d-band kikowaena (ke kupaa laina) o Cu-Pd alloys pili i ka Fermi pae.Hoʻopuka hou ʻia (D) a me (E) me ka ʻae mai ka American Chemical Society (71).ʻau, ʻokoʻa ʻokoʻa.

Ma waho aʻe o ka hopena alloy, ʻo ka hoʻopunipuni ʻana i nā mokuʻāina oxidation kekahi kumu nui e hoʻokō i ka hana o nā electrocatalysts, hiki ke hoʻopilikia i ka ʻōnaehana uila kūloko o ka mea.ʻO ka laʻana mua no ka hoʻopaʻa ʻana o ka catalyst ka hoʻohana ʻana i nā mea i loaʻa i ka oxide.Hiki i ke koena o ka oxygen ma ka ʻili a i ʻole ka lalo o ka catalyst ma hope o ka hōʻemi in situ ke hoʻoponopono i ke kūlana oxidation o ke kikowaena metala.No ka laʻana, ua hōʻike ʻo Cu plasma-oxidized i ʻoi aku ma mua o 60% selectivity i ka C2H4, i hāʻawi ʻia i ka hoʻohaʻahaʻa-kū kūʻē Cu + (37).No ka hōʻoia ʻana ʻo Cu + ke kī nui no ke koho kiʻekiʻe o ka ethylene, ua hana mākou i nā hoʻokolohua mana me ka hoʻohana ʻana i ka plasma like ʻole (Fig. 4A).Ua hōʻike hou ʻia ka spectroscopy absorption x-ray paʻakikī i ke koena o ke koena o ka ʻāpana o ka ʻili o ka ʻili (sub) paʻa i ke kūlana hoʻemi, me ka nui o nā ʻano Cu+ i koe ma hope o 1 hola o ka hōʻemi ʻana i nā mea hiki ke kiʻekiʻe o −1.2 V versus reversible hydrogen electrode (RHE).Eia kekahi, ua hōʻoia hou ʻia ka electroredeposition o ke keleawe mai kahi sol-gel copper oxychloride e hiki ke hoʻomaikaʻi i ke koho ʻana o C2H4 (61).Ua nānā ʻia ke kūlana hoʻokahe ʻana o kahi mea hoʻoheheʻe keleawe ma lalo o nā mea hiki ke hoʻohana ʻia me ka hoʻohana ʻana i ka spectroscopy absorption x-ray i hoʻoholo ʻia i ka manawa.ʻO ke kaʻina hoʻololi mua mai Cu2+ a i Cu+ he wikiwiki loa;akā naʻe, ʻoi aku ka lohi o ka hoʻemi electrochemical o nā ʻano Cu + i Cu0.Ma kahi o 23% o nā ʻano Cu+ e mau ana ma hope o 1-hola hoʻemi mau ma lalo o −1.2 V versus RHE (Fig. 4B).Ua hōʻike ʻia nā haʻawina mechanistic e alakaʻi ana ka pilina ma waena o Cu+ a me Cu0 i ka huki ʻana i ka electrostatic ma waena o nā intermediates mai ka mea i hoʻopiʻi maikaʻi ʻia ka C atom o *CO@Cu+, ʻoiai ʻo *CO@Cu0 ua hoʻopiʻi maikaʻi ʻia (80), ʻo ia hoʻi, hoʻoikaika i ka ʻO ka hoʻokumu ʻana i ka paʻa C─C a pēlā e hana ai i nā hydrocarbons C2+.Ma waho aʻe o nā mea i loaʻa i ka oxide, ua hoʻohana ʻia ke keleawe nitride (Cu3N) no ka hoʻokō ʻana i nā ʻano Cu+ i lalo o ka ʻili e hoʻemi i ka pale ikehu dimerization o *CO (81).Eia kekahi, i ka hoʻohālikelike ʻia me Cu i loaʻa i ka oxide, ʻoi aku ka paʻa o nā ʻano Cu3N i loaʻa iā Cu + (Fig. 4C).Ma muli o ka hopena, hōʻike ka nitride copper catalyst i kahi FE o 39 ± 2% no C2H4, ʻoi aku ka maikaʻi o ka Cu maʻemaʻe (~ 23%) a me Cu (~28%).Hoʻohālikelike i ka ʻōnaehana catalytic Cu +/Cu i ʻōlelo ʻia ma luna, ua hoʻohana ʻia ka boron ma ke ʻano he heteroatom dopant e hoʻolauna a hoʻopaʻa i ka Cuδ + (41).Hiki ke hoʻomalu ʻia ka awelika o ka oxidation state o ke keleawe mai +0.25 a +0.78 ma o ka hoʻololi ʻana i ka neʻe o ka boron dopant.Ua hōʻike ʻia ka nui o nā mokuʻāina i ka neʻe ʻana o nā electrons mai ke keleawe a i ka boron, e alakaʻi ana i kahi pae keleawe i hoʻoiho ʻia i ka dopant.Ua hōʻike mai ke keleawe boron-doped i ka hoʻonui ʻana i ka ikehu hoʻokumu o *CHO intermediate a, no laila, hoʻopaʻa i ke ala pane i nā huahana C1.Eia hou, hiki iā ia ke hoʻonui i ke koho ʻana i nā hydrocarbon multicarbon ma ka hoʻemi ʻana *CO dimerization reaction energy (Fig. 4D).Ma ka optimizing i ka awelika o ka ʻili o ke keleawe, hiki ke loaʻa kahi C2 FE kiʻekiʻe o ~ 80% me ~ 53% C2H4 ma lalo o ka awelika copper oxidation state o +0.35 (Fig. 4E).I kēia lā, ua ʻike ʻia nā pūnaewele ikaika ma ke keleawe ʻo Cu0, Cuδ+, a me / a i ʻole kā lākou interface no ECR ma nā haʻawina like ʻole (39, 41, 42, 81, 82).Eia naʻe, he aha ke kahua paʻa e hoʻopaʻapaʻa mau ʻia nei.ʻOiai ʻo ka heteroatom doping-induced Cuδ+ catalysts i hōʻike ʻia e ikaika loa no ka ECR i nā huahana C2+, pono e noʻonoʻo ʻia ka hopena synergistic mai nā hemahema i hana ʻia a me nā pilina.No laila, pono e hoʻomohala ʻia nā ʻōnaehana o ka operando no ka ʻike ʻana i ke kikowaena ikaika ma ka ʻili keleawe a nānā i ka hiki ke hoʻololi ʻia i loko o nā wahi hana ma lalo o nā kūlana pane.Ma waho aʻe, ʻo ka paʻa o ke keleawe i hoʻopiʻi maikaʻi ʻia kekahi mea hopohopo ma lalo o nā kūlana hoʻemi electrochemical.He mea paʻakikī ke ʻano o ka hana ʻana i nā catalysts me nā pūnaewele Cuδ+ paʻa.

(A) Hōʻuluʻulu manaʻo o ka C2H4 selectivity o nā ʻokoʻa plasma-activated copper catalysts.Hoʻopuka hou ʻia me ka ʻae mai ka Nature Publishing Group (37).ʻO nā pā kauā, 500 nm.(B) Ka ratio o Cu oxidation states pili i ka manawa pane ma −1.2 V versus RHE ma electroredeposited copper.Hoʻopuka hou ʻia me ka ʻae mai ka Nature Publishing Group (61).(C) Lakiō o nā ʻano Cu+ me kahi hana o ka manawa pane ma −0.95 V me RHE ma Cu-on-Cu3N a i ʻole Cu-on-Cu2O.Hoʻopuka hou ʻia me ka ʻae mai ka Nature Publishing Group (81).(D) Hiki i ka Boron doping ke hoʻololi i ka awelika adsorption ikehu o CO ma ka ʻili keleawe a hoʻohaʻahaʻa i ka ikehu dimerization CO─CO.ʻO 1[B], 2[B], 3[B], 4[B], a me 8[B] e pili ana i ka neʻe ʻana o ka boron doping ma lalo o ka ʻāina i loko o nā mea hoʻoheheʻe keleawe, ʻo ia ka 1/16, 1/8, 3/ 16, 1/4, a me 1/2.(E) ʻO ka pilina ma waena o ke kūlana oxidation a me FE o nā huahana C2 a i ʻole C1 i loko o nā catalysts keleawe-doped boron.Hoʻopuka hou ʻia (D) a me (E) me ka ʻae mai ka Nature Publishing Group (41).(F) Nā kiʻi SEM o nā pepa keleawe me nā mānoanoa like ʻole o nā kiʻi ʻoniʻoni Cu2O ma mua (luna) a ma hope (lalo) ECR.Hoʻopuka hou ʻia me ka ʻae mai ka American Chemical Society (83).

Ma waho aʻe o ka hoʻolālā uila, hiki i nā mea i loaʻa i ka oxide ke alakaʻi i ka morphology a i ʻole ka hoʻomohala ʻana i ka wā o ke kaʻina hoʻemi in situ.Mai ka hiʻohiʻona o ka morphology a i ʻole ka hoʻolālā ʻana, ua hoʻokumu ʻia ka hana electrochemical i hoʻonui ʻia o nā electrocatalysts i loaʻa i ka oxide i ka hoʻokumu ʻana i nā palena palaoa ikaika, nā kihi, a me nā ʻanuʻu (83-85).Ua hōʻike ʻo Yeo a me nā hoa hana (83) i ka hui ʻana C─C koho i nā kiʻi ʻoniʻoni Cu2O electrodeposited me nā mānoanoa like ʻole (Fig. 4F).Ma kahi Raman spectroscopy i hōʻike ʻia ua hoʻemi ʻia ka ʻili o nā kiʻiʻoniʻoni Cu2O i Cu0 paʻa paʻa i ka wā ECR (83).ʻO ka hopena, ua hōʻoia ʻia ʻo Cu0 metala ma ke ʻano he catalytic active center ma kahi o Cu+ species a i ʻole ka Cu+/Cu0 interface.Ma ke kaʻina hana o ka hoʻemi ʻana i ka Cu2O i Cu0 metala, ʻike ʻia ka ʻili o ka mea hoʻoheheʻe i loko o ke kahua i nā ʻanuʻu, nā ʻaoʻao, a me nā ʻanuʻu.Ua hōʻike ʻia he ʻoi aku ka ikaika o nā ʻanuʻu a me nā ʻaoʻao i hana ʻia ma mua o nā ʻanuʻu, mai ko lākou hoʻopaʻa ikaika ʻana me *CO, hiki ke hoʻoheheʻe hou i ka *CO i *CHO a i ʻole *CH2O.Ma waho aʻe, he mea hoʻolaha nā ʻāpana Cu e hoʻoikaika i ka hoʻokumu ʻana *CHO a me *CH2O.ʻO ka hana mua i manaʻo ʻia ʻoi aku ka maikaʻi o nā mea waena o *CHO a me *CH2O no ka hui ʻana o C─C ma mua o *CO i nā kinetics (86).Ma ka hoʻoponopono ʻana i ka morphology ili, hiki ke hoʻonui ʻia ka ikaika chemisorption o nā *CHO a me *CH2O intermediates.Ma kēia haʻawina, ua ʻike nā mea kākau i ka emi ʻana o ka FE o C2H4 mai 40 a 22% ke hoʻonui lākou i ka mānoanoa o Cu2O kiʻi lahilahi mai 0.9 a 8.8 μm.Loaʻa kēia ma muli o ka hoʻonui ʻia o Cu2O i hoʻonui ʻia me ka hoʻonui ʻana i ka mānoanoa Cu2O.Hiki i kēia mau ʻātoma undercoordinated ke hoʻopaʻa ikaika me H a, no laila, ʻoi aku ka makemake no ka hoʻololi hydrogen ma mua o ka hui ʻana o C─C.Ua hōʻike kēia hana e hiki i ka mea hoʻoheheʻe keleawe i loaʻa mai ka oxide ke hoʻoikaika nui i ka koho C2H4 ma o ka hana hou ʻana o ka morphology ma mua o ka hoʻokomo ʻana i nā ʻano Cuδ+ i hoʻopaʻa ʻia.Me ka hoʻohana ʻana i nā catalysts i loaʻa i ka oxide, ua koho ʻia ka ethane (C2H6) me ke kōkua o ka palladium(II) chloride (PdCl2) additive i ka electrolyte (34).Ua hōʻike ʻia he kuleana koʻikoʻi ka PdClx i hoʻopili ʻia ma ka ʻili o Cu2O i loaʻa i kahi hana koʻikoʻi no ka ulu ʻana o C2H6.ʻO ke kikoʻī, ua hoʻemi mua ʻia ka CO2 i C2H4 ma nā wahi Cu2O i loaʻa iā Cu2O, a laila e hoʻoheheʻe ʻia ka C2H4 i hoʻokumu ʻia me ke kōkua o PdClx adsorbed e hana i ka C2H6.Ua hoʻonui ka FE o C2H6 mai <1 a i 30.1% me ke kōkua o PdCl2.Hōʻike kēia hana i ka hui pū ʻana o ka catalyst ECR i wehewehe maikaʻi ʻia a me ka hoʻohui electrolyte hiki ke wehe i nā manawa hou no ka hana huahana C2+ kikoʻī.

ʻO ka Morphology a/a i ʻole ka hoʻoponopono hoʻonohonoho ʻana he hoʻolālā ʻē aʻe e hoʻololi i ka koho catalytic a me ka hana.Ua hōʻike nui ʻia ka hoʻomalu ʻana i ka nui, ke ʻano, a me nā hiʻohiʻona o ka catalyst no ka hoʻomaikaʻi ʻana i ka hana ECR (58, 87, 88).No ka laʻana, makemake nui ʻia ka ʻaoʻao Cu(100) no ka hanauna C2H4, ʻoiai ʻo ka huahana i mana mai ka Cu(111) catalyst ʻo ia ka methane (CH4) (87).Ma kahi noiʻi o Cu nanocrystals me nā ʻano like ʻole a me nā nui, ua hōʻike ʻo Buonsanti a me nā hoa hana (58) i ka hilinaʻi nui nonmonotonic o ka C2H4 selectivity i nā nanocrystals copper cube-shaped (Fig. 5A).ʻO ka mea maʻamau, ua hōʻike nā cubic Cu nanocrystals i ka hana C2H4 kiʻekiʻe a me ke koho ʻana ma mua o nā nanocrystals Cu spherical ma muli o ka predominance o ka (100) facet.Hiki ke hāʻawi i ka hana kiʻekiʻe aʻe ka nui aniani liʻiliʻi o cubic Cu ma muli o ka piʻi ʻana o ka neʻe ʻana o nā kahua ʻili haʻahaʻa, e like me nā kihi, nā ʻanuʻu, a me nā kinks.Eia nō naʻe, ʻoi aku ka ikaika o ka chemisorption o nā pae haʻahaʻa i hui pū ʻia me ka H2 a me ka koho kiʻekiʻe o CO, e hopena i ka haʻahaʻa o ka hydrocarbon FE.Ma ka ʻaoʻao ʻē aʻe, ua emi ka lakio o nā pae ʻaoʻao i nā kahua mokulele me ka hoʻonui ʻana i ka nui o nā ʻāpana, e pili pū ana i ka hana o ka hana C2H4.Ua hōʻike nā mea kākau i nā nanocubes keleawe waena me ka lōʻihi 44-nm i hōʻike ʻia i ka koho C2H4 kiʻekiʻe loa ma muli o ke kaulike i hoʻopaʻa ʻia ma waena o ka nui o ka nui a me ka mānoanoa o nā pae lihi.Eia kekahi, hiki i ka morphology ke hoʻopili i ka pH kūloko a me ka halihali lehulehu i ka wā ECR.Ua hōʻike ʻia ʻo ka pH kūloko kiʻekiʻe ma kahi kokoke i ka ʻili catalyst, ka mea i hoʻokumu ʻia e ka in situ i hoʻokumu ʻia OH−, e hoʻopau i ke ala hoʻopili proton.ʻO ka hopena, hiki ke hoʻonui ʻia ka hoʻokumu ʻana o ka hydrocarbon C2+ ma o *CO dimerization, a hiki ke kāohi ʻia ka CH4 i hana ʻia ma o *COH intermediate.Ua hōʻike ʻia nā ʻāpana nanowire keleawe (Fig. 5B) e hoʻonui i ka pH kūloko (68).Ma ke ʻano he electrolyte i hoʻohana mau ʻia, e hoʻopau koke ʻo CO2 saturated potassium bicarbonate (KHCO3) i ka OH− (HCO3− + OH− = CO32− + H2O) a e emi iho ka pH kūloko.Me kahi microstructure elongated, hiki ke hoʻohaʻahaʻa ʻia ka diffusion o HCO3− i loko o ka Cu nanowire arrays i hiki ke hoʻopau ʻia ka hopena neutralization no ka OH− kūloko i kekahi degere.Ma ke kumu o kahi loina like, ua hōʻike ʻia nā mesopores keleawe me nā mesopores i hoʻomalu pono ʻia (Fig. 5C) i hoʻonui ʻia FE no ka hana C2H4 a i ʻole C2H6 (32).Ua hōʻike ʻia e hiki ke hoʻonui ʻia ka pH kūloko i ka ʻili electrode ma ka hōʻemi ʻana i ka laula pore, e hoʻemi ana i ka huahana C1 FE a hoʻonui i ka huahana C2 FE.Ma waho aʻe o ka hoʻonui ʻana i ka hohonu o ka pore, hiki ke hoʻopaʻa ʻia ka huahana hōʻemi nui mai C2H4 a i C2H6.ʻO ka FE o C2H6 he kiʻekiʻe e like me 46%.No ka mea ua hoʻopaʻa ʻia nā kemika i loko o nā pores i ka wā ECR, ua wehewehe ʻia ka manawa lōʻihi o ka mālama ʻana i nā kikowaena koʻikoʻi i hoʻokumu ʻia e nā pores hohonu ke kumu nui o ke koho kiʻekiʻe i ka saturated C2 hydrocarbon.Ua hōʻike pū ʻia nā Cu nanofibers i loaʻa iā CuI i ke koho kiʻekiʻe i ka C2H6 (FE = 30% ma -0.735 V versus RHE) (89).ʻO ka anisotropic morphology a me ke kiʻekiʻe o ka ʻili o nā Cu nanofibers i loaʻa i ka CuI hiki ke hoʻomaikaʻi i ka hana paʻa o ka H2 i hoʻopaʻa ʻia a pēlā e hoʻonui ai i ka FE o C2H6.

(A i ka C) Morphology a i ʻole nā ​​hopena hoʻolālā.(A) Ka mānoanoa o nā ʻātoma (koi hema) a me ka lakio o nā mana ma nā pae lihi (Nedge) i nā ʻātoma ma ka mokulele (100) (N100) (axis ʻākau) e pili ana i ka lōʻihi lihi (d).Hoʻopuka hou ʻia me ka ʻae ʻia mai John Wiley a me Sons (58).(B) Hoʻololi ka pH i ke ʻano o ka morphology.Hoʻopuka hou ʻia me ka ʻae mai John Wiley a me Sons (68).(C) Ke koho huahana o ke keleawe mesopore me ka nui o ka pore a me ka hohonu.Hoʻopuka hou ʻia me ka ʻae ʻia mai John Wiley a me Sons (32).(D i H) Nā hopena Ligand.(D a me E) ECR ma ka copper nanowire (Cu NW) me nā ʻano amino acids (D) a i ʻole modifiers (E) ma −1.9 V. Hoʻopuka hou ʻia me ka ʻae mai ka Royal Society of Chemistry (35).(F) Ka nui o ka hana ana o C2H4 i loko o nā electrolytes halide like ʻole me nā mea hiki ke hoʻopili like ʻia ma Cu(35).Hoʻopuka hou ʻia me ka ʻae mai ka American Chemical Society (91).NHE, hydrogen electrode maʻamau.(G) FE o C2H4 a me CO i loko o nā manaʻo like ʻole o KOH electrolytes a me (H) Tafel slope o C2H4 i nā ʻokoʻa like ʻole o KOH electrolytes.(G) a me (H) i hana hou ʻia mai ka ʻAhahui ʻAmelika no ka holomua o ka ʻepekema (AAAS) (33).

ʻO ka hoʻololi ʻana i ka ʻili o ka Catalyst me ka hoʻohana ʻana i nā molekole liʻiliʻi kekahi hoʻolālā kaulana e hoʻomaikaʻi i ka hana electrochemical o ECR.Hiki i kēia hoʻolālā ke hoʻoikaika i ka microenvironment kokoke i ka ʻili catalyst, hiki ke hoʻopaʻa i nā mea waena ma muli o ka pilina ma waena o ka ligand surface a me ka waena.Ua hōʻike ʻia ʻo Amine ma ke ʻano he mea hoʻololi e hāpai i ka ECR (35).ʻO nā ʻakika amino like ʻole, me ka glycine (Gly), dl-alanine (Ala), dl-leucine (Leu), dl-tryptophan (Tyr), dl-arginine (Arg), a me dl-tryptophan (Trp), ua noiʻi ʻia i e aʻo i kā lākou hopena ma nā nanowires keleawe (35).E like me ka mea i hōʻike ʻia ma ka Fig. 5D, hiki i nā ligands amino acid-based a pau ke hoʻomaikaʻi i ke koho ʻana o C2+ hydrocarbons.ʻO ia mea hoʻonui e hōʻike ana ʻo ─COOH a me ─NH2 hui hana i loko o ka waikawa amino ke kuleana no ka hoʻonui ʻana i ka koho o ECR.Ua hōʻike ʻia nā hōʻike mua e hoʻokō ʻia ka adsorption o nā waikawa amino ma ka ʻili Cu ma o nā hui ─COOH a me ─NH2 (35, 90).ʻO ka waikona Stearic (C17H35COOH, RCO2H), aia wale nō ka hui ─COOH, i koho ʻia e ʻike i ke kuleana o ─COOH.Ua noiʻi pū ʻia nā mea hoʻololi ʻē aʻe, e like me a-anthraquinone diazonium salt (AQ), o-nitrobenzene diazonium salt (PhNO2), a me dodecyl mercaptan (C12H25SH, RSH), ʻaʻohe ─COOH a i ʻole ─NH2.Akā naʻe, ʻaʻole maikaʻi lākou a pau no ka hoʻomaikaʻi ʻana o C2+ hydrocarbon FE (Fig. 5E).Ua hōʻike ʻia ka helu ʻana i nā hui ─NH3+ i loko o ka adsorbed zwitterionic glycine hiki ke hoʻopaʻa i ka *CHO waena ma muli o kā lākou pilina ikaika, e like me nā paʻa hydrogen.ʻO ka hoʻokomo ʻana i nā ion halide i loko o ka electrolyte kekahi ala e hoʻololi ai i nā catalysts (91, 92).E like me ka mea i hōʻike ʻia ma ka Fig. 5F, hiki ke hoʻonui nui ʻia ka helu hana C2H4 ma ka plasma-activated Cu me ke kōkua o nā mea hoʻohui halide.Ua hōʻike ʻia ʻoi aku ka ikaika o ka I− ion ma mua o Br− a me Cl−, e like me ka ikehu adsorption pili o I−, Br−, a me Cl− ma ka Cu(100) facet (91).Ma waho aʻe o nā halides, ua hōʻike pū ka ion hydroxide i kahi hopena maikaʻi i ke koho C2H4.I kēia mau lā, ua hōʻike ʻo Sargent a me nā hoa hana (33) i ka hoʻololi ʻana o CO2-to-C2H4 me ~ 70% FE me ka hoʻohana ʻana i ka electrolyte potassium hydroxide (KOH) electrolyte (a hiki i ka 10 M) i loko o kahi kahe kahe.E like me ka mea i hōʻike ʻia ma ka Fig. 5G, ʻoi aku ka haʻahaʻa o ka hiki ke hoʻomaka o CO a me C2H4 ma 10 M KOH electrolyte i hoʻohālikelike ʻia me ka 1 M KOH.Eia kekahi, ua emi iho nā pali Tafel (Fig. 5H) o ka C2H4 me ka hoʻonui o ka hydroxide concentration (135 mV decade−1 ma 1 M KOH a me 65 mV decade−1 ma 10 M KOH), e hōʻike ana i ka transmutation o ka huina holoʻokoʻa- ka hoʻoholo ʻana i ka ʻanuʻu.Ua hōʻike nā hualoaʻa ʻo Density functional theory (DFT) i ka hiki ʻana mai o nā hydroxides concentrated hiki ke hoʻohaʻahaʻa i ka ikehu hoʻopaʻa o ka waena CO a hoʻonui pū i ke kaulike ʻole ma waena o ʻelua mau kalapona kalapona i adsorbed OCCO intermediates.ʻO ka hopena, e hoʻokūpaʻa hou ʻia ka waena OCCO ma o ka huki ʻana i ka dipole ikaika, e alakaʻi ana i ka haʻahaʻa haʻahaʻa o ka ikehu hoʻāla no ka dimerization CO, a laila e hoʻomaikaʻi i ka hana holoʻokoʻa.

ʻO C2+ oxygenates e like me ka ethanol (CH3CH2OH) kekahi mahele nui o nā huahana ECR waiwai nui.ʻO ka hana ʻenehana o ka ethanol kahi kaʻina hana ikaika, a e hoʻopau pū i ka nui o ka ethylene a i ʻole nā ​​​​meaʻai mahiʻai (40).No laila, ʻo ka hana electrocatalytic o ka ethanol a i ʻole nā ​​​​oxygenates C2 + ʻē aʻe mai CO2 e hana nui i ka manaʻo waiwai a me ke kaiapuni.Ma muli o ka hāʻawi ʻana o ka ethanol generation mai ECR i kahi waena penultimate me C2H4 ʻo ia ʻo *C2H3O (43), hiki i ka hydrogenation koho o kēia waena ke hoʻololi i nā ala ECR mai C2H4 i nā ʻona (64).Eia nō naʻe, ma ka hapa nui o nā ʻōnaehana, ʻoi aku ka haʻahaʻa o ka koho i ka C2+ oxygenates ma mua o ka hydrocarbons (31, 37, 39, 41, 42, 67).No laila, ma kēia ʻāpana, e hōʻike mākou i nā hoʻolālā hoʻolālā electrocatalyst e hiki ai ke hoʻokō i ka C2 + oxygenate FE kupaianaha ma luna o 25%.

E like me ka mea i kūkākūkā ʻia ma luna, hiki i nā catalysts bimetallic i hoʻolālā maikaʻi ke hoʻomaikaʻi i ka koho a me ka hana no ka hana ʻana o ka hydrocarbon C2+.Ua hoʻohana ʻia kahi hoʻolālā like akā ʻaʻole like e hoʻomaikaʻi i ka hana electrocatalytic no C2 + oxygenates (38, 93, 94).No ka laʻana, ua hōʻike nā mea hoʻoheheʻe Cu-Cu2O i hui pū ʻia me Ag i ke koho koho ethanol, a ʻo ka ethanol FE kiʻekiʻe he 34.15% (95).ʻO ka palena biphasic i loko o ka hui Ag-Cu i hui pū ʻia, ma kahi o Ag/Cu atomic ratio, ua ʻike ʻia ʻo ia ke kumu nui no ka hana koho ʻana o ka ethanol.No ka mea, ua kokoke loa ka Cu site i ka Ag site ma ke ano i hui pu ia (Ag-Cu2OPB), ua hiki ke hoonuiia ka nui o ke kukulu ana o na ethanol intermediates no ka laana i hui pu ia me ka hoolikelike me ka mahele i hookaawale ia (Ag-Cu2OPS. ), e alakaʻi ana i kahi hana hoʻomohala ethanol maikaʻi aʻe.Ma waho aʻe o ka ethanol, ua hōʻike ʻia nā Cu-Ag bimetallic NPs e hoʻololi i ka CO2 i acetate me ka hoʻohui ʻana o benzotriazole (93).Ma −1.33 V me RHE, he 21.2% ka FE o ka acetate.ʻElua ala hoʻololi i manaʻo ʻia i kēia hihia: Hoʻokumu ʻia kekahi ma ka dimerization CO, a ʻo kekahi ma luna o ka hoʻokomo ʻana CO, e hōʻike ana i ke kuleana koʻikoʻi o ka hoʻokumu ʻana o CO intermediate ma nā kahua Ag.Ua hōʻike ʻia kahi ʻike like ma Cu-Zn catalysts (Fig. 6, A a me B) no ka hana ethanol (38).Ma ka hoʻopaʻa ʻana i ka maʻiʻo o Zn i Zn-Cu alloyed catalysts, hiki ke hoʻomalu maikaʻi ʻia ka ratio o ka ethanol me C2H4 FE ma ka laulā o 0.48 a hiki i 6, e hōʻike ana i ke koʻikoʻi o nā kahua hoʻololi CO no ka hoʻokumu ʻana o ka oxygenate C2+.Hiki i ka hana ʻana o nā mea hoʻoheheʻe i hoʻohui ʻia ke hoʻoulu i ka hopena koʻikoʻi i ka mea matrix, ʻaʻole makemake ʻia i kekahi manawa.No laila, ʻoi aku ka maikaʻi o ke ala pololei i nā catalysts bimetallic no kekahi mau huahana.Ua kūkulu ʻo Jaramillo a me nā hoa hana (96) i kahi ʻōnaehana bimetallic Au-Cu maʻalahi, i hoʻohui ʻia e ka waiho pololei ʻana o nā NP gula ma luna o ka polycrystalline Cu foil, e noiʻi i ka hopena catalysis tandem.Ua hōʻike ka bimetallic Au-Cu i ka synergistic selectivity a me ka hana i ka C2+ alcohols, outperforming maʻemaʻe keleawe a me ke gula, a me Au-Cu alloy.Hoʻohālikelike ʻia me Cu foil, ua hōʻike ka ʻōnaehana Au-Cu bimetallic i ka piʻi ʻana o ka manaʻo CO kūloko ma muli o ka loaʻa ʻana o nā Au NPs (Fig. 6C) i hana no ka hanauna CO.No ka mea ʻaʻole ikaika ke gula no ka hōʻemi ʻana i ka CO, ua hoʻonui ʻia ka nui o ka hana ʻana i ka waiʻona C2+ ma nā catalysts bimetallic Au-Cu i kahi mīkini catalysis tandem.Ma keʻano kikoʻī, hiki i nā NP gula ke hoʻoulu i ka ʻike CO kūloko kiʻekiʻe kokoke i ka ʻili Cu.Ma hope aʻe, hiki ke hoʻemi hou ʻia ka nui o nā molekala CO kūloko i nā waiʻona C2+ e Cu.

(A i C) Nā hopena huila.(A) FE kiʻekiʻe o ka ethanol a me C2H4 a me ka lakio FE o ka ethanol a me ka ethylene ma nā huila Cu-Zn like ʻole.(B) Māhele ʻāpana o kēia manawa o ka ethanol ma nā huila Cu-Zn like ʻole.Hoʻopuka hou ʻia (A) a me (B) me ka ʻae mai ka American Chemical Society (38).(C) ka emi ʻana o CO2 a me ka hoʻololi ʻana o CO ma ke gula, keleawe, a me ka ʻōnaehana bimetallic Au-Cu.Hoʻopuka hou ʻia me ka ʻae mai ka Nature Publishing Group (96).(D i ka L) Morphology a i ʻole nā ​​hopena hoʻolālā.(D) Hōʻike kiʻi kiʻi o ke ʻano kaʻa kaʻa kaʻa metala.(E a me F) nā kiʻi SEM o 100-cycle Cu ma mua o (E) a ma hope o (F) ka prereduction ma lalo o nā kūlana ECR.(G) TEM a me ka ʻāpana electron diffraction i koho ʻia ua hōʻike ʻia ʻo Cu(100) a me (H) ikehu manuahi no ka hoʻokumu ʻana o *OCCO a me *OCCHO ma nā ʻaoʻao Cu(100), Cu(111), a me Cu(211).Hoʻopuka hou ʻia (D) a (G) me ka ʻae ʻia mai ka Nature Publishing Group (42).(I) Ka ratio o ka oxygenates a me ka hydrocarbons ma ke ʻano he hana o ka hiki ma Cu(111), Cu(751), a me Cu(100).(J) Nā helu hui no Cu(111), Cu(100), a me Cu(751).Hoʻopuka hou ʻia (I) a me (J) me ka ʻae mai ka National Academy of Sciences (97).(K) Papahana o ke kaʻina hana hoʻololi mai Cu NPs i cubic-like keleawe.Hoʻopuka hou ʻia me ka ʻae mai ka National Academy of Sciences (98).(L) Nā kiʻi SEM o ke keleawe nanodendritic ma mua a ma hope o ECR.Hoʻopuka hou ʻia me ka ʻae mai ka American Chemical Society (99).

Ua hōʻike ʻia ka ʻike koho ʻana o nā ʻaoʻao aniani no nā electrocatalysts ma ke ʻano he ala kūpono a pololei i ka hoʻokō ʻana i ka FE i hoʻonui ʻia i nā huahana ECR kikoʻī a me kahi ala koʻikoʻi no ka ʻike kumu.He mea paʻakikī ke ʻano maʻalahi akā hiki ke hoʻonui ʻia o nā catalysts hoʻokahi-crystal.Hoʻoulu ʻia e ke kaʻina hana galvanostatic charging-discharging (GCD) no nā pila, ua hoʻomohala kā mākou hui i ke ʻano kaʻa kaʻa kaʻa metala (Fig. 6D) e hōʻike pono i ka ʻaoʻao aniani o kahi Cu catalyst (42).Ma hope o 100 mau pōʻaiapuni GCD, ua hoʻokumu ʻia kahi pūʻulu Cu nanocube nui ma luna o ka pahu Cu me nā ʻaoʻao i hōʻike ʻia (100) (Fig. 6, E a G).Ua hōʻike ʻia ka mea hoʻoheheʻe 100-cycle i kahi C2+ waiʻona FE holoʻokoʻa ma mua o 30% a me kahi ʻano waiʻona C2+ e pili ana i kēia manawa ma mua o 20 mA cm−2.Eia naʻe, ʻo ka 10-cycle Cu me ka haʻahaʻa haʻahaʻa o ka (100) facet hāʻawi wale i kahi C2+ waiʻona FE o ~10%.Ua hōʻoia ʻo DFT simulation ua ʻoi aku ka maikaʻi o nā ʻaoʻao Cu (100) a me ka paepae (211) no ka hui ʻana o C─C ma luna o Cu (111), e like me ka hōʻike ʻana ma ka Fig. 6H.Ua hoʻohana ʻia kahi kiʻi hoʻohālike, epitaxial Cu film me nā ʻaoʻao ʻokoʻa i hōʻike ʻia, no ka hoʻoholo ʻana i nā kumu o ka pūnaewele hoʻoikaika i ka C2+ oxygenate production (Fig. 6I) (97).Ma muli o ka emi ʻana o ka helu CO* dimer e pili ana i nā ʻātoma H* ma ka ʻili me ka liʻiliʻi o nā hoalauna, hiki i nā pae Cu i hoʻohui ʻia haʻahaʻa ke kāohi i ka hana ʻana o nā hydrocarbons a alakaʻi i ka C2+ oxygenate FE maikaʻi no ka mea ʻoi aku ka paʻakikī o ka hydrogenate. C─C hui pū ʻia nā kikowaena ECR ma kona ʻili (97).Ma ka epitaxial Cu film study, ua hōʻoia nā mea kākau i ka ECR ma ka Cu(751) facet i hōʻike i ka hoʻomaikaʻi ʻana i ka ratio oxygenate/hydrocarbon.Hiki ke hoʻohui ʻia kēia hoʻonui ʻana i ka ʻili Cu atom geometry o nā ʻaoʻao Cu like ʻole a me ka helu haʻahaʻa haʻahaʻa i hui pū ʻia (Fig. 6J), kahi i hui pū ai ʻo Cu atom, me ʻelua, ʻehā, a me ʻeono mau hoalauna kokoke loa ma Cu(751), Cu(100), a me Cu(111).Ua hoʻohana ʻia ke kūkulu hou ʻana i ka morphology in situ e hoʻomaikaʻi i ka C2+ oxygenate FE.Ua hoʻomohala ʻia e Yang a me nā hoa hana (98) kahi mea hoʻoheheʻe cube-like Cu, kahi i hōʻike i ka hoʻomaikaʻi ʻana i ka hana hoʻohui C─C.Ma ka kikoʻī, ua waiho ʻia ka monodisperse Cu NPs (6.7 nm) me nā ukana like ʻole ma ke kākoʻo pepa kalapona ma ke ʻano he catalyst no ECR.ʻIke ʻia, ua ʻike ʻia ka hoʻonui ʻana o FE o C2 + oxygenates me ka hoʻonui ʻana i ka hoʻouka ʻana o Cu NP.Ua hōʻike ʻia ʻo Cu NPs i hoʻopiha piha ʻia ma lalo o nā kūlana hoʻouka kiʻekiʻe i hoʻololi ʻia i loko o ka wahi i ka wā ECR, kahi i hoʻokumu ʻia ai nā morphologies like cube (Fig. 6K).Ua ʻike ʻia kēia ʻano hana hou i ʻoi aku ka hana electrocatalytically.Ua manaʻo ʻia ka loiloi Tafel ʻo ka dimerization CO ka pae hoʻoholo helu no ka hoʻokumu ʻana i ka huahana C2, akā ʻo ka n-propanol i hōʻike i kahi ala ʻokoʻa i kēia ʻōnaehana catalytic.ʻO ke keleawe nanodendritic kekahi hiʻohiʻona e hōʻike ana i ke koʻikoʻi o ka mana morphology no ka C2 + oxygenate production (99).ʻO ka pōkole, ʻo ka huina FE o ka nanodendrite keleawe i wehewehe maikaʻi ʻia (Fig. 6L) no ka waiʻona C2+ ma kahi o 25% ma −1.0 V versus RHE.Hiki ke ho'okō 'ia ka n-propanol FE o 13% ma −0.9 V. E no'ono'o ana i ka hana ki'eki'e o Cu atom, e ho'opilikia mau 'ia nā catalysts ma muli o ka ho'oha'aha'a 'ana i ka wā ECR, 'o ia ho'i ma ka overpotential ki'eki'e. kūpaʻa.Eia nō naʻe, ua hōʻike ʻia kēlā ʻano keleawe nanodendritic i ke kūpaʻa maikaʻi no ka hana ʻana i ka waiʻona, e hōʻike ana i kahi waiʻona FE o ~24% ma luna o 6 mau hola.

ʻO nā hemahema o nā electrocatalysts, e like me nā hakahaka atom a me nā dopants, e hōʻike ana i ka hiki ke hoʻopili i nā intermediates ECR unconventional a, no laila, koho koho i ke ala e pili ana i nā oxygenates (29, 43, 100).Ke lawe nei i ka *C2H3O ma ke ano he la'ana, 'o ia ka waena penultimate kūpono no ka hana 'ana i ka ethylene a me ka ethanol, ua a'o 'o Sargent a me nā hoa hana (43) i ke 'ano o nā hemahema i loko o ka pūpū Cu electrocatalyst me ka kiko'ī.Ua hōʻike manaʻo lākou ua like nā pale ikehu hopena no ka hoʻokumu ʻana i ka ethylene a me ka ethanol i ka wā mua o ka hui ʻana o C─C (0.5-V overpotential) (Fig. 7A).Ma lalo o ia ʻano, ʻo ka hoʻokomo ʻia ʻana o ka hakahaka keleawe e hoʻonui iki i ka pale ikehu no ka hoʻokumu ʻana i ka ethylene, akā ʻaʻole ia i hōʻike i ka hopena i ka hanauna ethanol (Fig. 7B).Eia naʻe, e like me ka mea i hōʻike ʻia ma ka Fig. 7C, hiki i nā catalysts keleawe me ka hakahaka a me ka dopant sulfur subsurface ke hoʻonui nui i ka pale ikehu no ke ala ethylene, me ka maikaʻi ʻole o ka thermodynamically.Eia naʻe, ua hōʻike ʻia kēlā hoʻololi ʻana i kahi hopena maikaʻi ʻole ma ke ala ethanol.Ua hōʻoia hou ʻia kēia hanana.ʻO Cu2S-Cu i hoʻonohonoho ʻia me ka nui o nā hakahaka o ka ʻili (Cu2S-Cu-V; Fig. 7D).Ua hoʻonui ʻia ka lakio o ka waiʻona i ka ethylene mai 0.18 ma nā Cu NPs ʻole a i 0.34 ma Cu2S-Cu hakahaka ʻole a laila i 1.21 ma Cu2S-Cu-V, ʻoiai ua like ka huina FE o nā huahana C2+ no nā catalysts āpau (Fig. 7E) .Ua hōʻike ʻia kēia ʻike e pili ana ka paipai ʻana i ka koho ʻana i ka waiʻona me ka hoʻopau ʻana i ka hana ethylene, e like me ka hopena DFT.Eia kekahi, ʻoi aku ka koʻikoʻi o ka ʻenehana defect no ka mea hoʻoheheʻe kalapona metala ʻole no ka mea ʻaʻole hana nā mea kalapona maʻemaʻe no ECR.Ua hoʻohana ʻia nā dopants e like me ka nitrogen a me ka boron no ka hoʻololi ʻana i ke ʻano uila o kahi catalyst-carbon (31, 43, 100).No ka laʻana, ua hoʻololi ʻia ke kiʻiʻoniʻoni nitrogen-doped nanodiamond (NDD) ma ka substrate silika e Quan et al.(29) no ka hana acetate koho mai ECR (Fig. 7F).ʻO ka hiki ke hoʻomaka o ka acetate he haʻahaʻa e like me -0.36 V versus RHE me ka hoʻohana ʻana i ka NDD catalyst, a ʻo ka FE no ka acetate i ʻoi aku ma mua o 75% i kahi pae kūpono mai -0.8 a -1.0 V versus RHE.No ka hoʻomaopopo ʻana i ke kumu o ia ʻano hoʻomaikaʻi maikaʻi loa, ua mākaukau a noiʻi ʻia nā electrodes NDD/Si ​​me nā ʻano nitrogen like ʻole a i ʻole nā ​​​​mea ʻano nitrogen (Fig. 7G).Ua hoʻoholo nā mea kākau e hiki ke hoʻopili ʻia ka hana kiʻekiʻe o ka NDD/Si ​​catalyst no ECR i kona overpotential kiʻekiʻe no ka hydrogen evolution a me N doping, kahi i hana nui ai nā ʻano N-sp3C no ka hana acetate.Ua hōʻike ʻia ka ʻikepili electrokinetic a me ka spectrum infrared in situ ʻo ke ala nui no ka hoʻokumu ʻana o ka acetate ʻo CO2 → *CO2− → *(COO)2 → CH3COO−.Ma waho aʻe o ka nitrogen, ʻo boron kekahi heteroatom i ʻimi maikaʻi ʻia e hoʻoponopono i ke ʻano uila o nanodiamond.Eia naʻe, ʻoi aku ka maikaʻi o ka hoʻemi ʻana o ka boron-doped nanodiamond (BDD) i ka CO2 i formaldehyde a i ʻole formate (101).Eia kekahi, ua hōʻike ʻo Quan a me nā hoa hana (102) i ka boron a me ka nitrogen co-doped nanodiamond (BND) i hōʻike i ka hopena synergistic ma ECR, hiki ke lanakila i ka palena o BDD a laila koho i ka ethanol.BND1, BND2, a me BND3 catalysts me ka like ole naikokene maʻiʻo a me ka like boron doping pae i hoomakaukauia.E like me ka mea i hōʻike ʻia ma ka Fig. 7H, hiki ke loaʻa ke koho kiʻekiʻe o ka ethanol a hiki i ka 93% ma ka BND3 catalyst ma −1.0 V versus RHE, nona ka doping nitrogen kiʻekiʻe.Ua hōʻike ʻia ka helu ʻana i ke kaʻina hana hoʻohui C─C ma BND i thermodynamically maikaʻi, kahi i hoʻoikaika ai ka boron atom i ka hopu ʻana o CO2 a me ka nitrogen dopant i hoʻoikaika i ka hydrogenation o waena i ka ethanol.ʻOiai ua hiki i ka heteroatom-doped nanodiamond ke hoʻololi i ka CO2 i loko o nā oxygenates multicarbon me ke koho kiʻekiʻe, ua kaupalena ʻia kāna hana ECR ma muli o ke kaʻina hana hoʻoili lohi (ʻoi aku ka nui o kēia manawa ma mua o 2 mA cm−2).ʻO nā mea i hoʻopaʻa ʻia i ka graphene he mea hiki ke hoʻopau i nā hemahema o nā mea hoʻoheheʻe daimana.ʻO ka manaʻo, ua lawe ʻia nā pae pyridinic N ma ka papa graphene ma ke ʻano he mau wahi hana no ka hui ʻana o C─C (103).Ma muli o ka hiki ʻana o ka pyridinic N ma nā wahi lihi hiki ke hoʻololi i ka CO2 i CO, hiki ke hoʻohui hou ʻia i loko o ka mole C2+ (Fig. 7I).No ka laʻana, hiki ke hoʻopaʻa ʻia ka *C2O2 waena i loko o ke kalapona nitrogen-doped kahi i hoʻopaʻa ʻia ai nā ʻātoma C ʻelua i ka pyridinic N a me kāna ʻātoma C pili, kēlā me kēia (103).Ua hōʻoia ʻia ka wanana theoretical me ka hoʻohana ʻana i nā catalysts graphene-doped graphene quantum dot (NGQD) (31).Ma hope o ka pulverization o nitrogen-doped graphene sheets (1 a 3 μm) (Fig. 7J), 1- i 3-nm NGQDs i loaʻa i loko o ka nui o ka pyridinic N ma nā wahi lihi i hoʻonui ʻia e ʻekolu kauoha o ka nui.Ma −0.78 V versus RHE, hiki ke piʻi ka FE kiʻekiʻe loa no C2+ oxygenates i 26%.Eia kekahi, e like me ka mea i hōʻike ʻia ma ka Fig. 7K, ʻo ka hapa o kēia manawa no ka C2 + oxygenates kokoke i 40 mA cm−2 ma -0.86 V versus RHE, ʻoi aku ka kiʻekiʻe ma mua o ka nanodiamond i hoʻololi ʻia.I ka hoohalike ana, N-noa graphene quantum kiko a me N-doped graphene oxide, e hoike ana i ka pae haahaa loa o ka pyridinic N, ka mea nui i hua mai H2, CO, a me ka formate.

(A i C) Gibbs ka ikehu manuahi mai *C2H3O i ka ethylene a me ka ethanol no ke keleawe, ke keleawe me ka hakahaka, a me ke keleawe me ka hakahaka keleawe a me ka sulfur ma lalo o ka ʻāina.(D) Hōʻike kiʻi kiʻi o ka Cu2S-Cu-V catalyst.(E) FE o nā waiʻona C2+ a me ka ethylene, a me ka ratio FE o nā waiʻona me nā alkenes.Hoʻopuka hou ʻia (A) a (E) me ka ʻae mai ka Nature Publishing Group (43).(F) kiʻi SEM o NDD.(G) Ka nui o ka hana ʻana o ka acetate a me ka formate ma NDD me nā ʻokoʻa o ka nitrogen.ma %, atomika %.Hoʻopuka hou ʻia (F) a me (G) me ka ʻae mai ka American Chemical Society (29).(H) FEs no NDD, BDD, a me BND ma −1.0 V. Hoʻopuka hou ʻia me ka ʻae mai John Wiley a me Sons (102).(I) Hōʻike kiʻi kiʻi o nā pūnaewele hana no ka hui ʻana o C─C ma NGQD.Ua paʻi hou ʻia (I) me ka ʻae mai ka American Chemical Society (103).(J) TEM kiʻi o NGQD.ʻO nā pā unahi, 1 nm.(K) Māhele ʻāpana o kēia manawa no nā huahana like ʻole me ka hoʻohana ʻana i nā NGQD.Hoʻopuka hou ʻia (J) a me (K) me ka ʻae ʻia mai ka Nature Publishing Group (31).

Ma waho aʻe o nā electrocatalysts, electrode a me catalytic reactor architecture design e hāʻawi i kahi ala kūpono e hoʻoikaika ai i ka hana ECR, ʻoi aku ka nui o ka hana a me ka pono o ka ikehu.Ua hana ʻia nā hoʻomaikaʻi koʻikoʻi ma ka hoʻolālā a me ka hana ʻana i nā ʻōnaehana electroreduction hou e hoʻokō ai i ka hana C2+ maikaʻi loa.Ma kēia ʻāpana, e kūkākūkā mākou i ka hoʻolālā electrode / reactor ECR i nā kikoʻī.

Hoʻohana nui ʻia nā cell type H i nā hoʻokolohua lab-scale, e noʻonoʻo ana i kā lākou hui maʻalahi, hana maʻalahi, a me ke kumu kūʻai haʻahaʻa.Hoʻolako ʻia nā keʻena me nā cathode kūʻokoʻa a me nā keʻena anode i hoʻopili ʻia e kahi membrane hoʻololi ion (104, 105).ʻO ka pōʻino mua o kēia pūnaewele H-type ka haʻahaʻa CO2 solubility i loko o ka wai electrolyte, ʻo ia wale nō ka 0.034 M ma lalo o nā kūlana ambient, e alakaʻi ana i ka hoʻemi ʻana o CO2 i kēia manawa densities o j <100 mA cm−2 (64).Eia kekahi, ʻaʻole hiki ke hoʻokō i nā koi noiʻi e ulu nei (105, 106).No ka hana hua C2+, hōʻike maʻamau nā pūnaewele ʻano-H i ka haʻahaʻa haʻahaʻa ma lalo o nā mana kiʻekiʻe, e laʻa, 32% no ka ethylene ma −0.98 V versus RHE (107), 13.1% no n-propanol ma −0.9 V versus RHE (99), a 20.4% no ka ethanol ma −0.46 V versus RHE (108), ma muli o ka hoʻokūkū koʻikoʻi o ka hydrogen evolution.

No ka hoʻoponopono ʻana i nā pilikia i luna aʻe, ua manaʻo ʻia ka reactor kahe (15, 109).I loko o nā keena kahe, hiki ke hoʻohana pono ʻia ke kahawai CO2 kinoea ma ke ʻano he mea hānai ma ka cathode, no laila ke alakaʻi nei i ka hoʻonui nui ʻana i ka diffusion a me ka helu hana (104, 110).Hōʻike ka Figure 8A i ka hoʻolālā maʻamau o ke kahe kahe, kahi i lawelawe ʻia ai kahi membrane electrolyte polymer (PEM) ma ke ʻano he mea hoʻokaʻawale electrode i hoʻopili ʻia ma waena o ʻelua kahawai kahe.Hoʻokomo ʻia ka catalyst ma luna o kahi electrode diffusion gas (GDE) e lawelawe ma ke ʻano he cathode electrode, kahi e hānai pono ʻia ai ke kinoea CO2.ʻO ka catholyte, e like me 0.5 M KHCO3, ke kahe mau nei i loko o ka ʻāpana lahilahi ma waena o ka electrode catalyst a me PEM.Eia hou, ho'olaha pinepine 'ia ka 'ao'ao anode me kahi electrolyte wai no ka ho'ololi 'ana o ka oxygen (43, 110).Ke hoʻohālikelike ʻia me nā pūnaewele H-type, hōʻike ʻia kēia mau mea kahe e pili ana i ka membrane i ka hana ECR maikaʻi loa.No ka laʻana, ua loiloi ʻo Sargent a me nā hoa hana (43) i ka hana ECR o ka mea hoʻoheheʻe Cu2S-Cu-V ma nā ʻano H-type cell a me ke kahe kahe, e like me ka mea i hōʻike ʻia ma ka Fig. 8 (B to E).Ke hoʻohana nei i nā pūnaewele H-type, ʻo ka FE kiʻekiʻe loa no nā huahana C2+ he 41% me ka huina o kēia manawa o ~30 mA cm−2 ma lalo o −0.95 V versus RHE.Eia naʻe, ua hoʻonui ʻia ka FE no nā huahana C2+ i 53% me ka nui o kēia manawa maʻalahi ma mua o 400 mA cm−2 ma lalo o −0.92 V versus RHE i kahi ʻōnaehana kahe.ʻO ia ʻano hoʻomaikaʻi koʻikoʻi me ka hoʻohana ʻana i ka reactor kahe e hiki ke hoʻohālikelike ʻia i ka hoʻonui ʻia ʻana o CO2 a me nā ʻaoʻao ʻaoʻao i hoʻopaʻa ʻia, ʻo ia ka mea i loaʻa mai ka hoʻolālā kinoea-electrolyte-catalyst triple-interface architecture.

(A) He kiʻikuhi o ka electrolyzer kahe me kahi kiʻi i hoʻonui ʻia o ka interface electrode-electrolyte.(A) ua hana hou ʻia me ka ʻae ʻia mai John Wiley a me Sons (30).(B i E) Hoʻohālikelike i ka hana ECR me ka hoʻohana ʻana i ka cell H-type a me ka cell flow.Hoʻopuka hou ʻia (B) a (E) me ka ʻae ʻia mai ka Nature Publishing Group (43).(F a i H) Hoʻohana ʻia nā electrolytes like ʻole i loko o nā keena kahe e kūʻē i ka hana ECR.Hoʻopuka hou ʻia (F) a (H) me ka ʻae ʻia mai John Wiley a me Sons (30).(I a K) Ka hoʻolālā a me ka hana paʻa o ka electrode diffusion kinoea polymer.Hoʻopuka hou ʻia (I) a (K) me ka ʻae mai AAAS (33).

ʻO ka cell gap zero kekahi papa e puka mai ana o nā electrolyzers, kahi e hoʻoneʻe hou aku ai i nā kahawai kahe i loko o nā keena kahe a kaomi i ʻelua electrodes me kahi membrane hoʻololi ion ma waena.Hiki i kēia hoʻonohonoho hoʻonohonoho ke hoʻohaʻahaʻa nui i ka hoʻoili ʻana a me ka hoʻololi ʻana o ka electron a pēlā e hoʻomaikaʻi ai i ka pono o ka ikehu, e ʻoi aku ka maʻalahi i nā noi kūpono (110).ʻO nā mea hoʻoheheʻe i hānai ʻia i ka cathode he catholyte-saturated CO2 a i ʻole kahawai CO2 humidified.Hoʻokomo pono ʻia ka mahu wai a i ʻole ka wai electrolyte i ka anode no ka hoʻokuʻu ʻana o ka proton e uku i ka uku no nā ʻano hoʻemi CO2 (111).ʻO Gutiérrez-Guerra et al.(109) loiloi i ka hana o ka Cu-AC hybrid catalyst i loko o ka zero gap cell a hōʻike i ka acetaldehyde ka huahana nui me ka koho kiʻekiʻe o 60%.Ma keʻano he mea maikaʻi'ē aʻe o kēia mea hana, he mea maʻalahi loa ke kaomi i ke kahe o ka reactant a hoʻonui nui i ka manaʻo CO2 kūloko, no laila ka hopena i nā densities nui o kēia manawa a me nā helu hopena kiʻekiʻe (110).Eia nō naʻe, ʻo ka hoʻololi ʻana i ka ion i hoʻolalelale ʻia i loko o nā cell gap zero ka mea e hoʻokahe i ka catholyte, e hoʻololi i ka pane i ka H2 evolution ma kahi o ka hoʻemi CO2 (112).No ka hoʻoponopono ʻana i kēia pilikia, ua hoʻokomo ʻo Zhou a me nā hoa hana (112, 113) i kahi papa pale me kahi electrolyte wai e kahe ana ma waena o ka cathode a me ka membrane e mālama ai i ka pH kūpono kokoke i ka cathode no ka hopena hoʻemi CO2.ʻOiai ua ʻike ʻia nā huahana C2+ like ʻole ma ke kumu o nā pūnaewele zero gap, me ka acetone, ethanol, a me ka n-propanol, haʻahaʻa mau nā FE.ʻO ka hapa nui o nā haʻawina i hōʻike ʻia e pili mau ana i nā huahana C1 e pili ana i nā helu liʻiliʻi o ka proton a me nā hoʻololi electron i ka wā o ka hoʻohaʻahaʻa ʻana.No laila, ke hoʻopaʻapaʻa ʻia nei ka hiki o ka cell gap zero no nā huahana C2+ (110).

Eia kekahi, ʻo nā cell electrolytic microfluidic (MECs) he ʻano hoʻonohonoho electrolyzer maikaʻi loa i hoʻomohala ʻia e Kenis a me nā hoa hana (39, 114).I loko o kēia hāmeʻa, hoʻololi ʻia ka membrane e kahi ākea lahilahi (<1 mm ka mānoanoa) i hoʻopiha ʻia me ke kahawai electrolyte kahe e hoʻokaʻawale i ka anode a me ka cathode.Hiki i nā molekala CO2 ke hoʻopuehu koke i loko o ke kikowaena electrode-electrolyte kokoke i ka cathode, a ʻo nā GDE paʻa ʻelua e hoʻoheheʻe ʻia e ka electrolyte kahe.Ke hoʻohālikelike ʻia i nā cell kahe e pili ana i ka membrane, ʻaʻole wale nā ​​MEC e pale i ke kumukūʻai membrane kiʻekiʻe akā e hoʻēmi pū i ka hoʻokele wai, e pili ana i ka anode maloʻo a me ka wai kahe ʻana i ka cathode i ka wā e hoʻohana ʻia ai i nā density kiʻekiʻe o kēia manawa ma muli o ka osmotic drag o nā molekole wai me. ka lawe proton mai ka anode a i ka cathode ma o ka membrane (115).E like me kā mākou e ʻike ai, ʻoiai nā mea i ʻike ʻia a me nā hoʻokō, ua loaʻa i kahi helu liʻiliʻi o nā haʻawina i loaʻa nā huahana C2+ i nā MEC mua.Ma muli paha o ka hopena "floating" i hoʻokahe maʻalahi ʻia nā protons i hana ʻia i loko o ka anode mai kahi kokoke i ka cathode a i ʻole holoi ʻia e ka electrolyte kahe, ma mua o ke komo ʻana i ka proton he nui i koi ʻia C2+.Hiki ke hōʻoia ʻia ka manaʻo e ka laʻana aʻe.Ma 2016, ua hōʻike ʻo Kenis a me nā hoa hana (31) i ka hōʻemi kūleʻa o CO2 i nā huahana C2 + ma kahi MEC i hoʻololi ʻia a me ka membrane, kahi e hiki ai i nā NGQD ke hoʻemi i nā molekala CO2 i C2 + me 55% FE (31% no ka ethylene, 14% no ka ethanol, 6% no ka acetate, a me 4% no ka n-propanol) ma kahi hiki ke hoohana ia o −0.75 V me RHE ma 1 M KOH solution.He mea nui ia e kuhikuhi i hiki i kahi kaiapuni electrolyte ke hoʻololi nui i ka koho huahana pū kekahi.No ka laʻana, ua hana ʻo Jiao a me nā hoa hana (30) i kahi nanoporous Cu catalyst a laila hoʻāʻo i kāna hana ECR me ka hoʻohana ʻana i nā electrolytes like ʻole (KHCO3, KOH, K2SO4, a me KCl) i loko o kahi MEC me ka membrane.Ua hōʻike lākou i ka hōʻemi ʻana o CO2 i ka alkaline electrolyte (KOH) e hōʻike ana i ka koho kiʻekiʻe C2 + a me ka nui o kēia manawa, e like me ka hōʻike ʻana ma ka Fig. 8 (F a me G).Ma −0.67 V versus RHE ma 1 M KOH electrolyte, hiki i ka FE i loaʻa no C2+ a hiki i 62% me kahi ʻāpana o kēia manawa o 653 mA cm−2, ʻo ia kekahi o nā densities kiʻekiʻe loa i hōʻike ʻia ma nā hoʻemi electrochemical CO2. i nā huahana C2+.ʻO Ethylene (38.6%), ethanol (16.6%), a me n-propanol (4.5%) nā huahana C2 + nui me ka liʻiliʻi o ka acetate.Ua hōʻike pū lākou he pilina ikaika ma waena o ka pH ili i helu ʻia a me FE no nā huahana C2+: ʻO ke kiʻekiʻe o ka pH ili, ʻoi aku ka kiʻekiʻe o kēia manawa a me nā hua hua C2+, e like me ka mea i hōʻike ʻia ma Fig. 8H.Ua manaʻo ʻia ka helu ʻana e hiki i nā ion OH− kokoke i ka ʻili ke hoʻoikaika ikaika i ka hui ʻana o C─C (31).

Ma waho aʻe o ka hoʻonohonoho electrolyzer, hiki i ka electrolyte i hoʻohana ʻia i nā electrolyzers like ʻole ke hoʻololi nui i nā huahana ECR hope loa.E like me kā mākou i ʻōlelo ai ma luna nei, hoʻohana mau ʻia nā hopena KOH alkaline nui i nā cell kahe me ka hana maikaʻi loa ma mua o nā cell H-type.He mea ia e hiki ai i ka KOH electrolyte ke hāʻawi i ka mana electrolyte kiʻekiʻe, e hoʻemi i ka pale ohmic ma waena o ka uhi electrolyte lahilahi ma ka catalyst a me ka electrolyte nui, a e hoʻemi hou i nā overpotentials i koi ʻia no ka hoʻokumu ʻana o C2+ (31).Ua hōʻoia hou nā hualoaʻa DFT e hiki ke hoʻohaʻahaʻa i ka hiki ʻana o nā ion OH− i ka pale ikehu no ka dimerization CO, pēlā e hoʻonui ai i ka hoʻokumu ʻana o C2+ a me ke kāohi ʻana i ka hoʻokūkū mai ka hoʻokumu ʻana o C1 a me H2 (30, 33).Eia naʻe, ʻaʻole hiki ke hoʻohana ʻia ka alkaline KOH ma ke ʻano he electrolyte i loko o nā ʻano ʻano H-type.ʻO kēia no ka mea e pane wikiwiki nā kahawai CO2 me nā hāʻina KOH a i ka hopena e hana i kahi hopena bicarbonate me ka pH kūʻokoʻa i loko o nā keena H-type (30).I loko o nā pūnaewele kahe, akā naʻe, ke hoʻopuehu ka CO2 ma o ka GDE, e hoʻopau ʻia nā molekala CO2 ma ka pae palena ʻekolu (CO2-catalyst-electrolyte) e hana koke i nā huahana i hōʻemi ʻia.Ma waho aʻe o kēia, hiki i ka hiki ke hoʻonui i ka pH a puni ka electrolyte i ka hoʻonohonoho electrolyzer paʻa, ʻoiai ka electrolyte kahe e hōʻoluʻolu i ka ʻili a e hōʻemi i ka fluctuation pH i ka electrolyte (33, 116).

E like me ka mea i ʻōlelo ʻia ma mua, ʻo ka ECR kahi hopena diffusion-controlled, hiki ke hoʻonui nui i ke kaomi hopena kiʻekiʻe i ka nui a me ka hoʻopili ʻana i ka manaʻo CO2.ʻO nā reactors kiʻekiʻe maʻamau e like me ka autoclave kila, kahi e hiki ai ke hoʻokomo i ka CO2 kiʻekiʻe (a hiki i ka 60 atm) i loko o ke kelepona, e alakaʻi ana i kahi piʻi kupaianaha o ka FE a me ka nui o C2 + (117). , 118).Ua hōʻike ʻo Sakata a me nā hoa hana (119) e hiki ke hoʻonui ʻia ka nui o kēia manawa i 163 mA cm−2 ma lalo o 30 atm ma kahi electrode Cu me ka ethylene ka huahana nui.Nui nā mea hoʻoheheʻe metala (e laʻa, Fe, Co, a me Ni), me ka hana ʻole no ka hana ʻana o C2+ ma ke kaomi ʻana, hiki ke hōʻemi i ka CO2 i ka ethylene, ethane, propane, a me nā huahana C2+ kauoha kiʻekiʻe ma nā kaomi kiʻekiʻe.Ua hōʻike ʻia ʻo ke koho ʻana o nā huahana e hilinaʻi nui ʻia i ke kaomi CO2 i ke ʻano o ka hoʻololi ʻana i ka loaʻa CO2 ma ka ʻili electrode (117, 120).Hoʻololi ʻia nā huahana nui i hoʻemi ʻia mai ka H2 a i ka hydrocarbons (C2+ i hoʻokomo ʻia) a hope loa i CO/HCOOH me ka piʻi ʻana o ke kaomi CO2.ʻO ka mea nui, pono ke nānā pono ʻia ke kaomi CO2 no ka mea ʻoi aku ka nui o ke kiʻekiʻe a i ʻole ka haʻahaʻa CO2 kaomi e hoʻoulu i ka nui a i ʻole ka palena o ka diffusion CO2, kahi e makemake ai i ka hana ʻana o CO/HCOOH a i ʻole H2.ʻO ka nui kūpono o ka CO waena a me ka nui o kēia manawa i hana ʻia ma ka ʻili electrode hiki ke hoʻomaʻamaʻa i ka hopena hoʻohui C─C a hoʻonui i ka koho huahana C2+ (119).

ʻO ka hoʻolālā ʻana i kahi electrode hou me nā hale kiʻekiʻe kahi kuhikuhi koʻikoʻi ʻē aʻe e hoʻonui ai i ka hana koho C2 +.I ka wā mua, ʻo nā electrodes hana he nonporous metala foils a loaʻa i ka sluggish mass transfer (26, 105).ʻO ka hopena, ua manaʻo ʻia ʻo GDE e hōʻoluʻolu i ka hana kelepona maikaʻi ʻole ma o ka hāʻawi ʻana i nā kahawai hydrophobic e hoʻomaʻamaʻa i ka hoʻolaha ʻana o CO2 i nā ʻāpana catalyst (121).Aia ka GDE ma'amau i ka papa catalyst (CL) a me ke kinoea diffusion layer (GDL), e like me ka mea i hō'ike 'ia ma ka 'ao'ao ha'aha'a o Fig. 8A (30, 33).ʻO ke kinoea-wai-catalyst interface i hoʻokumu ʻia ma GDE he mea koʻikoʻi e hoʻomaikaʻi i ka hana kelepona.Hiki i ka GDL i hui pū me nā mea porous (pepa kalapona maʻamau) ke hāʻawi i nā ala CO2 nui a hōʻoia i ka wikiwiki o ka hoʻoheheʻe electrolyte.Hoʻohana ʻia ʻo ia ma ke ʻano he ala kaʻa haʻahaʻa haʻahaʻa no nā protons, electrons, a me nā huahana hōʻemi mai ka CL i ka electrolyte (121).ʻO ka hoʻolei ʻana, airbrushing, a me ka electrodeposition nā ʻenehana maʻamau no ka hoʻomākaukau ʻana i nā GDE (122).Ua noiʻi nui ʻia nā Catalysts i hui pū ʻia me nā GDE i ka hoʻemi ʻana o CO2 i nā huahana C2+.ʻO ka mea nui, ua hui pū ʻia nā cell flow i ʻōlelo ʻia me ka hana maikaʻi me nā GDE.I ka makahiki 1990, ua hōʻike ʻo Sammells a me nā hoa hana (123) ua loaʻa nā GDE i uhi ʻia ʻo Cu i ka FE kiʻekiʻe o 53% no ka ethylene me kahi kiʻekiʻe kiʻekiʻe o 667 mA cm−2.ʻO ka hoʻonui ʻana i ke koho ʻana o ka ethylene a me ka ethanol he mea paʻakikī nui i hana pū ʻia ma nā catalysts hoʻokumu ʻia Cu ma muli o kā lākou mau ala ʻano like mechanistic.Eia kekahi, he mea nui e kuhikuhi aku ua ikeia ka hoouluhua kiekie a me ke koho ana o ka ethylene e hoohalikeia me ka ethanol ma Cu-based GDE (25, 36).Ua hōʻike ʻo Gewirth a me nā hoa hana (36) i kahi FE maikaʻi loa o 60% no ka ethylene a me kahi FE i hoʻopaʻa ʻia no ka ethanol o 25% ma ka electrodeposited Cu-Ag GDE, i ka wā i hiki ai ka nui o kēia manawa i ka ~300 mA cm−2 ma −0.7 V versus RHE.He hana kakaʻikahi ia i loaʻa i kahi koho kiʻekiʻe i ka nui o kēia manawa.Hōʻike kēia ʻike e hāʻawi kahi electrode i hoʻohui ʻia i ka GDE i kahi ala hoʻohiki no ka hoʻopaʻa ʻana i nā ala pane, kahi e loaʻa ai ke koho o nā huahana i hōʻemi ʻia i nā kiʻekiʻe o kēia manawa.

He mea koʻikoʻi ka paʻa o nā GDE e pono e hoʻoponopono ʻia no ka mea he mea nui ka hana paʻa i ka wā lōʻihi e ʻike ai i ka hoʻohana pono ʻana no nā cell kahe.ʻOiai ka maikaʻi o ka hana CO2-to-C2+ i loaʻa me nā GDE, ʻaʻole maikaʻi ka paʻa ʻana ma muli o ka palupalu mechanical adhesion o ka catalyst, GDL, a me nā papa binder (77, 124).Hiki ke loli ka ʻili kalapona o GDL mai ka hydrophobic a i ka hydrophilic i ka wā o ka hopena electrochemical ma muli o ka hopena oxidation i hana ʻia ma nā overpotentials kiʻekiʻe, e alakaʻi ana i ke kahe ʻana i ka GDL a keakea i nā ala hoʻoheheʻe CO2 (33).No ka hoʻoponopono ʻana i kēia pilikia, ua hoʻohui nā mea noiʻi i ka scaffold hydrophobic o polytetrafluoroethylene (PTFE) i loko o nā GDE.Hoʻohālikelike ʻia me ka hydrophilic Nafion, kahi ʻāpana PTFE hydrophobic e hāʻawi i kahi kūpaʻa lōʻihi lōʻihi (33).ʻO Sargent a me nā hoa hana (33) i hōʻuluʻulu i kahi Cu catalyst ma waena o ka PTFE a me ka carbon NPs i hoʻokaʻawale ʻia, kahi i hiki ai i ka papa hydrophobic PTFE ke hoʻoneʻe i nā NPs a me nā papa graphite, pēlā e kūkulu ai i kahi kikowaena electrode paʻa (Fig. 8, I a me J).ʻO ka hopena, ua hoʻonui ʻia ka FE no ka hana ʻana i ka ethylene i 70% ma 7 M KOH solution ma nā densities o kēia manawa o 75 a 100 mA cm−2.Ua hoʻonui ʻia ke ola o kēia mea hoʻoheheʻe kahe i ʻoi aku ma mua o 150 mau hola me ka nalo ʻole o ka ethylene selectivity, ʻo ia ka 300-paʻi ka lōʻihi ma mua o nā GDE kuʻuna, e like me ka hōʻike ʻana ma Fig. 8K.Ua hōʻike ʻia kēlā ʻano hana sandwich he hoʻolālā GDE maikaʻi loa.No ka laʻana, ua hoʻolālā ʻo Cui a me nā hoa hana (124) i kahi hale trilayer me kahi papa electrode ikaika i ʻoki ʻia e nā kiʻiʻoniʻoni polyethylene nanoporous hydrophobic ʻelua.Hiki i nā papa hydrophobic waho ke hoʻolohi i ke kahe electrolyte mai ka hoʻonā nui, e alakaʻi ana i ka pH kūpaʻa kiʻekiʻe a puni ka electrode hana.ʻO ka hoʻonui ʻana i ka wahi interlayer, hiki ke hoʻomaikaʻi i ka lawe ʻana a me ka adsorption CO2, he mea nui hoʻi i ia hoʻolālā (124).I kēia mau lā, ua hoʻohui pū ʻia nā nanotubes kalapona i loko o nā GDE ma muli o ko lākou porosity kiʻekiʻe, conductivity maikaʻi, a me ka hydrophobicity, hiki ke hoʻomaʻamaʻa i ka electron a me ka halihali lehulehu (77).

ʻOiai ka holomua ʻana o ka ECR, ʻaʻole hiki ke loaʻa nā hoʻolālā no nā kumu kūʻai haʻahaʻa, nui-nui C2+ (125).I kēia manawa, ua like nā pilikia a me nā manawa kūpono e hoʻomaopopo i nā ʻano hana o ka ECR a hoʻolaha i kēia ʻenehana hoʻohiki.

Ma ke ʻano he hopena maikaʻi e pani ai i ke kalapona kalapona a mālama i ka ikehu hiki ke hoʻololi hou ʻia, e like me ka makani a me ka lā, ua hana ʻia nā holomua nui e hoʻokō i ka hoʻololi CO2 kūpono i nā makahiki i hala.ʻOiai ua lōʻihi ka hoʻomaopopo ʻana i nā kaʻina hana e pili ana me ECR mai kona mau lā mua (126), ʻaʻole mamao loa ka hoʻopili ʻana o C─C ma o ECR i nā huahana C2+ no ka hoʻohana pono ʻana.Ma kēia loiloi, ua nānā mākou i nā kikoʻī kikoʻī i nā hoʻolālā o kēia manawa e hiki ke hoʻoikaika i ka koho a me ka helu hana no nā huahana C2+ ma o ECR, me ka hoʻokani maikaʻi-catalyst, nā hopena electrolyte, nā kūlana electrochemical, a me ka hoʻolālā electrode / reactor electrochemical.

ʻOiai ʻo ka hoʻoikaika ʻana i ka ECR, nui nā pilikia me nā catalysts o kēia manawa a me ka ʻōnaehana ECR pono e hoʻoponopono ʻia ma mua o ka kūʻai ʻana i ka ECR.ʻO ka mea mua, ma ke ʻano he mea hoʻoikaika nui e hoʻomaopopo i ka hui ʻana C─C maikaʻi, loaʻa ʻo Cu i nā pilikia paʻa koʻikoʻi, ʻoi aku ka nui o ka wai electrolyte, a hiki ʻole ke ola no 100 mau hola ma muli o ko lākou kiʻekiʻe atom mobility, particle aggregation, and structure deterioration under ECR condition.No laila, pehea e hoʻokō ai i ka paʻa o ka wā lōʻihi me ka hoʻohana ʻana i ka catalyst Cu-based he mea paʻakikī.ʻO ka hoʻopaʻa ʻana i ka mea hoʻoheheʻe Cu-based ma ke kākoʻo kikoʻī me ka hoʻopili ikaika ʻana paha he hoʻolālā hilinaʻi e mālama ai i ke ʻano catalyst/morphology a pēlā e hoʻonui ai i ke ola.Eia kekahi, me ka hoʻohana ʻana i ka electrolyte membrane polymer e hoʻololi i ka hoʻonā wai i ka wā ECR hiki paha ke hoʻomaikaʻi hou aku i ka paʻa o ka catalyst Cu-based.Eia hou, mai ke kuanaʻike o catalysts, in situ/in operando characterization a me ka theoretical modeling pono e hoʻohana 'ia e nānā a hoʻomaopopo i ka catalyst hana palaho, pela, ka huli, suppressing ka degradation a me ka make o ka catalyst i ka haʻahaʻa pae.ʻO kekahi pilikia koʻikoʻi o nā catalysts ECR e pono e kamaʻilio ʻia ʻo ia ka hana ʻana i ka protocol synthesis e hiki ai ke hana nui.No kēia hopena, ʻoi aku ka maikaʻi o ka hoʻomaʻamaʻa ʻana i nā kaʻina hana synthetic me ka hoʻohana ʻana i nā meaʻai meaʻai ākea.

ʻO ka lua, ʻo ka C2+ oxygenated mai ECR e hui pū ʻia me nā solutes (e laʻa, KHCO3 a me KOH) i loko o ka electrolyte no ka H- a i ʻole nā ​​kahe-cell reactors kuʻuna, akā naʻe, pono e hoʻokaʻawale hou a me nā kaʻina hana no ka hoʻihoʻi ʻana i ka wai maʻemaʻe. nā noi kūpono.I ka manawa like, ua hui pū ʻia nā hydrocarbons C2+ i hoʻololi ʻia me H2 a me ke koena CO2.No laila, pono ke kaʻina hana hoʻokaʻawale nui no ka ʻenehana ECR o kēia manawa, kahi mea e pale hou ai iā ECR mai ka hoʻohana pono ʻana.No laila, pehea e hana pololei ai a hoʻomau i ka hoʻoheheʻe ʻana i ka wahie wai maʻemaʻe a me nā hydrocarbons kinoea maʻemaʻe, ʻoi aku ka nui o nā huahana kiʻekiʻe, makemake nui ʻia no ka hoʻohana pono ʻana o ECR.No laila mākou e wānana i ka piʻi nui ʻana o ka hoʻokumu pololei ʻana o nā huahana maʻemaʻe ma o ECR i ka wā e hiki mai ana, hiki ke lawe i ka ʻenehana ECR kokoke loa i ka mākeke (127).

ʻO ke kolu, ʻoiai ka hoʻokumu ʻana o nā mea paʻa C─O a me C─H, e like me ka ethanol, acetic acid, a me ka ethylene, i ka ʻenehana ECR i aʻo nui ʻia, ʻo ka ʻimi ʻana i nā ʻano huahana ʻē aʻe he mea nui no ka ʻenehana ECR a hōʻike i ka hoihoi waiwai.Eia kekahi laʻana, i kēia manawa, ua hōʻikeʻo Han a me nā hoa hana (128) i ka hanaʻana o 2-bromoethnol e ECR.ʻO ka hoʻokumu ʻana i loko o ka paʻa C─Br e hoʻololi i ka huahana mai ka ethanol a i ka 2-bromoethnol, kahi mea nui i kūkulu ʻia i ka synthesis kemika a me ka lāʻau lapaʻau a hōʻike i ka waiwai hoʻohui kiʻekiʻe.No laila, ma waho aʻe o nā huahana C2+ i aʻo maikaʻi ʻia, ke manaʻoʻiʻo nei mākou ʻo ka huli ʻana i nā huahana ʻē aʻe i ʻimi ʻole ʻia e like me ka oxalic acid (129) a me ka synthesis o nā molekala C2+ paʻakikī e like me nā pūhui cyclic kahi ala hoʻohiki ʻē aʻe no ka noiʻi ECR e hiki mai ana.

ʻO ka mea hope akā ʻaʻole ka mea liʻiliʻi loa, pono e hoʻohana nui ʻia nā hoʻolālā electrode hou a me ka reactor e like me GDE waiʻole, ke kahe wai-wai, a me ka cell PEM no ka hoʻonui ʻana i ka helu hana ECR i ka pae kalepa (>200 mA cm−2).Eia nō naʻe, ʻike mau ʻia ka ʻokoʻa nui i ka hana electrocatalytic i ka wā e hoʻohana ʻia ai nā electrocatalysts i ka hoʻāʻo ʻana o ke kelepona piha.No laila, pono e hana ʻia nā haʻawina hoʻonaʻauao e hōʻemi i ka ʻokoʻa ma waena o nā haʻawina hapalua-cell a me ka hoʻohana ʻana i nā hāmeʻa piha piha e lawe i ka ECR mai ka hoʻāʻo lab-scale i ka hoʻohana pono.

I ka hōʻuluʻulu ʻana, hāʻawi ka hoʻemi electrochemical CO2 i ka manawa kūpono no mākou e hoʻoponopono i ka pilikia kaiapuni mai nā kinoea ʻōmaʻomaʻo i hoʻokuʻu ʻia e nā hana kanaka.Hōʻike pū ia i ka hiki ke hoʻokō i nā wahie maʻemaʻe a me nā kemika me ka hoʻohana ʻana i ka ikehu hou.ʻOiai e mau ana nā pilikia he nui no ka ʻenehana ECR i kēia manawa, ʻoi aku hoʻi no ke kaʻina hana hoʻohui C─C, ua manaʻo ʻia me ka hoʻomau ʻana o ka noiʻi a me ka hoʻomohala ʻana i ka catalyst optimization a me ka cell perfection, ʻo ka hiʻohiʻona o kahi electrolysis CO2 honua maoli no ka wahie maʻemaʻe. a e hoʻokō ʻia nā kemika i ka wā e hiki mai ana.

He ʻatikala wehe ʻia kēia i hāʻawi ʻia ma lalo o nā ʻōlelo o ka laikini Creative Commons Attribution-NonCommercial, e ʻae ana i ka hoʻohana ʻana, ka hoʻohele ʻana, a me ka hana hou ʻana ma nā ʻano mea like ʻole, inā ʻaʻole no ka pono kālepa ka hopena o ka hoʻohana ʻana a hāʻawi ʻia ka hana kumu i kūpono. haʻi ʻia.

MANAʻO: Ke noi wale nei mākou i kāu leka uila i ʻike ka mea āu e paipai nei i ka ʻaoʻao ua makemake ʻoe e ʻike lākou, ʻaʻole ia he leka uila.ʻAʻole mākou e hopu i kahi leka uila.

© 2020 ʻAhahui ʻAmelika no ka holomua o ka ʻepekema.Ua mālama ʻia nā kuleana āpau.He hoa pili ʻo AAAS no HINARI, AGORA, OARE, CHORUS, CLOCKSS, CrossRef a me COUNTER.Science Advances ISSN 2375-2548.