Discover the SciOpen Platform and Achieve Your Research Goals with Ease.
Search articles, authors, keywords, DOl and etc.
To improve the electrocatalytic conversion of carbon dioxide (CO2) into C2+ products (such as ethylene (C2H4) and ethanol (CH3CH2OH), etc.) is of great importance, but remains challenging. Herein, we proposed a strategy that directs the C–C coupling pathway through enriching and confining the carbon monoxide (CO) intermediate to internal pores of Cu nanocubes, for electrocatalytic reduction of CO2 into C2+ chemicals. In H-type cell, the Faraday efficiency (FE) for ethylene and ethanol reaches 70.3% at −1.28 V versus the reversible hydrogen electrode (vs. RHE), with a current density of 47.9 mA·cm−2. In flow cell, the total current density is up to 340.3 mA·cm−2 at −2.38 V (vs. RHE) and the FE for C2+ products is 67.4%. Experimental and theoretical studies reveal that both the CO intermediate adsorption and C–C coupling reaction on such an internal porous catalyst are facilitated, thus improving CO2-to-C2+ conversion efficiency.
Huo, H.; Wang, J.; Fan, Q. K.; Hu, Y. J.; Yang, J. Cu-MOFs derived porous Cu nanoribbons with strengthened electric field for selective CO2 electroreduction to C2+ fuels. Adv. Energy Mater. 2021, 11, 2102447.
Yao, K. L.; Li, J.; Wang, H. B.; Lu, R. H.; Yang, X. T.; Luo, M. C.; Wang, N.; Wang, Z. Y.; Liu, C. X.; Jing, T. et al. Mechanistic insights into OC–COH coupling in CO2 electroreduction on fragmented copper. J. Am. Chem. Soc. 2022, 144, 14005–14011.
Chen, X. Y.; Chen, J. F.; Alghoraibi, N. M.; Henckel, D. A.; Zhang, R. X.; Nwabara, U. O.; Madsen, K. E.; Kenis, P. J. A.; Zimmerman, S. C.; Gewirth, A. A. Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes. Nat. Catal. 2021, 4, 20–27.
Zhang, B. X.; Zhang, J. L.; Hua, M. L.; Wan, Q.; Su, Z. Z.; Tan, X. N.; Liu, L. F.; Zhang, F. Y.; Chen, G.; Tan, D. X. et al. Highly electrocatalytic ethylene production from CO2 on nanodefective Cu nanosheets. J. Am. Chem. Soc. 2020, 142, 13606–13613.
Zhong, D. Z.; Zhao, Z. J.; Zhao, Q.; Cheng, D. F.; Liu, B.; Zhang, G.; Deng, W. Y.; Dong, H.; Zhang, L.; Li, J. K. et al. Coupling of Cu(100) and (110) facets promotes carbon dioxide conversion to hydrocarbons and alcohols. Angew. Chem., Int. Ed. 2021, 60, 4879–4885.
Zhu, Q. G.; Sun, X. F.; Yang, D. X.; Ma, J.; Kang, X. C.; Zheng, L. R.; Zhang, J.; Wu, Z. H.; Han, B. X. Carbon dioxide electroreduction to C2 products over copper-cuprous oxide derived from electrosynthesized copper complex. Nat. Commun. 2019, 10, 3851.
Ma, W. C.; Xie, S. J.; Liu, T. T.; Fan, Q. Y.; Ye, J. Y.; Sun, F. F.; Jiang, Z.; Zhang, Q. H.; Cheng, J.; Wang, Y. Electrocatalytic reduction of CO2 to ethylene and ethanol through hydrogen-assisted C–C coupling over fluorine-modified copper. Nat. Catal. 2020, 3, 478–487.
Christensen, O.; Zhao, S. Q.; Sun, Z. Z.; Bagger, A.; Lauritsen, J. V.; Pedersen, S. U.; Daasbjerg, K.; Rossmeisl, J. Can the CO2 reduction reaction be improved on Cu: Selectivity and intrinsic activity of functionalized Cu surfaces. ACS Catal. 2022, 12, 15737–15749.
Wu, Z. Z.; Zhang, X. L.; Niu, Z. Z.; Gao, F. Y.; Yang, P. P.; Chi, L. P.; Shi, L.; Wei, W. S.; Liu, R.; Chen, Z. et al. Identification of Cu(100)/Cu(111) interfaces as superior active sites for CO dimerization during CO2 electroreduction. J. Am. Chem. Soc. 2022, 144, 259–269.
Luo, H. Q.; Li, B.; Ma, J. G.; Cheng, P. Surface modification of nano-Cu2O for controlling CO2 electrochemical reduction to ethylene and syngas. Angew. Chem., Int. Ed. 2022, 61, e202116736.
Sha, Y. F.; Zhang, J. L.; Cheng, X. Y.; Xu, M. Z.; Su, Z. Z.; Wang, Y. Y.; Hu, J. Y.; Han, B. X.; Zheng, L. R. Anchoring ionic liquid in copper electrocatalyst for improving CO2 conversion to ethylene. Angew. Chem., Int. Ed. 2022, 61, e202200039.
Wang, P. T.; Yang, H.; Tang, C.; Wu, Y.; Zheng, Y.; Cheng, T.; Davey, K.; Huang, X. Q.; Qiao, S. Z. Boosting electrocatalytic CO2-to-ethanol production via asymmetric C–C coupling. Nat. Commun. 2022, 13, 3754.
Morales-Guio, C. G.; Cave, E. R.; Nitopi, S. A.; Feaster, J. T.; Wang, L.; Kuhl, K. P.; Jackson, A.; Johnson, N. C.; Abram, D. N.; Hatsukade, T. et al. Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst. Nat. Catal. 2018, 1, 764–771.
Liang, Z. Q.; Zhuang, T. T.; Seifitokaldani, A.; Li, J.; Huang, C. W.; Tan, C. S.; Li, Y.; De Luna, P.; Dinh, C. T.; Hu, Y. F. et al. Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2. Nat. Commun. 2018, 9, 3828.
Zhou, Y. S.; Che, F. L.; Liu, M.; Zou, C. Q.; Liang, Z. Q.; De Luna, P.; Yuan, H. F.; Li, J.; Wang, Z. Q.; Xie, H. P. et al. Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons. Nat. Chem. 2018, 10, 974–980.
De Luna, P.; Quintero-Bermudez, R.; Dinh, C. T.; Ross, M. B.; Bushuyev, O. S.; Todorović, P.; Regier, T.; Kelley, S. O.; Yang, P. D.; Sargent, E. H. Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction. Nat. Catal. 2018, 1, 103–110.
Gao, D. F.; Zegkinoglou, I.; Divins, N. J.; Scholten, F.; Sinev, I.; Grosse, P.; Cuenya, B. R. Plasma-activated copper nanocube catalysts for efficient carbon dioxide electroreduction to hydrocarbons and alcohols. ACS Nano 2017, 11, 4825–4831.
Wakerley, D.; Lamaison, S.; Ozanam, F.; Menguy, N.; Mercier, D.; Marcus, P.; Fontecave, M.; Mougel, V. Bio-inspired hydrophobicity promotes CO2 reduction on a Cu surface. Nat. Mater. 2019, 18, 1222–1227.
Niu, Z. Z.; Gao, F. Y.; Zhang, X. L.; Yang, P. P.; Liu, R.; Chi, L. P.; Wu, Z. Z.; Qin, S.; Yu, X. X.; Gao, M. R. Hierarchical copper with inherent hydrophobicity mitigates electrode flooding for high-rate CO2 electroreduction to multicarbon products. J. Am. Chem. Soc. 2021, 143, 8011–8021.
Liu, C. X.; Zhang, M. L.; Li, J. W.; Xue, W. Q.; Zheng, T. T.; Xia, C.; Zeng, J. Nanoconfinement engineering over hollow multi-shell structured copper towards efficient electrocatalytical C–C coupling. Angew. Chem., Int. Ed. 2022, 61, e202113498.
Lv, J. J.; Jouny, M.; Luc, W.; Zhu, W. L.; Zhu, J. J.; Jiao, F. Highly porous copper electrocatalyst for carbon dioxide reduction. Adv. Mater. 2018, 30, 1803111.
Li, C. W.; Ciston, J.; Kanan, M. W. Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper. Nature 2014, 508, 504–507.
Yang, K. D.; Ko, W. R.; Lee, J. H.; Kim, S. J.; Lee, H.; Lee, M. H.; Nam, K. T. Morphology-directed selective production of ethylene or ethane from CO2 on a Cu mesopore electrode. Angew. Chem., Int. Ed. 2017, 56, 796–800.
Jung, H.; Lee, S. Y.; Lee, C. W.; Cho, M. K.; Won, D. H.; Kim, C.; Oh, H. S.; Min, B. K.; Hwang, Y. J. Electrochemical fragmentation of Cu2O nanoparticles enhancing selective C–C coupling from CO2 reduction reaction. J. Am. Chem. Soc. 2019, 141, 4624–4633.
Li, M. H.; Ma, Y. Y.; Chen, J.; Lawrence, R.; Luo, W.; Sacchi, M.; Jiang, W.; Yang, J. P. Residual chlorine induced cationic active species on a porous copper electrocatalyst for highly stable electrochemical CO2 reduction to C2+. Angew. Chem., Int. Ed. 2021, 60, 11487–11493.
Sang, J. Q.; Wei, P. F.; Liu, T. F.; Lv, H. F.; Ni, X. M.; Gao, D. F.; Zhang, J. W.; Li, H. F.; Zang, Y. P.; Yang, F. et al. A reconstructed Cu2P2O7 catalyst for selective CO2 electroreduction to multicarbon products. Angew. Chem., Int. Ed. 2022, 61, e202114238.
Nam, D. H.; Bushuyev, O. S.; Li, J.; De Luna, P.; Seifitokaldani, A.; Dinh, C. T.; De Arquer, F. P. G.; Wang, Y. H.; Liang, Z. Q.; Proppe, A. H. et al. Metal-organic frameworks mediate Cu coordination for selective CO2 electroreduction. J. Am. Chem. Soc. 2018, 140, 11378–11386.
Wang, Y. H.; Wang, Z. Y.; Dinh, C. T.; Li, J.; Ozden, A.; Kibria, M. G.; Seifitokaldani, A.; Tan, C. S.; Gabardo, C. M.; Luo, M. C. et al. Catalyst synthesis under CO2 electroreduction favours faceting and promotes renewable fuels electrosynthesis. Nat. Catal. 2020, 3, 98–106.
Verma, S.; Hamasaki, Y.; Kim, C.; Huang, W. X.; Lu, S.; Jhong, H. R. M.; Gewirth, A. A.; Fujigaya, T.; Nakashima, N.; Kenis, P. J. A. Insights into the low overpotential electroreduction of CO2 to CO on a supported gold catalyst in an alkaline flow electrolyzer. ACS Energy Lett. 2018, 3, 193–198.
Zhan, C.; Dattila, F.; Rettenmaier, C.; Bergmann, A.; Kühl, S.; García-Muelas, R.; López, N.; Cuenya, B. R. Revealing the CO coverage-driven C–C coupling mechanism for electrochemical CO2 reduction on Cu2O nanocubes via operando Raman spectroscopy. ACS Catal. 2021, 11, 7694–7701.
Li, F. W.; Li, Y. C.; Wang, Z. Y.; Li, J.; Nam, D. H.; Lum, Y.; Luo, M. C.; Wang, X.; Ozden, A.; Hung, S. F. et al. Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces. Nat. Catal. 2020, 3, 75–82.
Carmo, M.; Fritz, D. L.; Mergel, J.; Stolten, D. A comprehensive review on PEM water electrolysis. Int. J. Hydrogen Energy 2013, 38, 4901–4934.