文献类型：期刊文献

英文题名：Selective methane electrosynthesis enabled by a hydrophobic carbon coated copper core-shell architecture

作者：Zhang, Xin Yu[1];Li, Wen Jing[1];Wu, Xue Feng[1];Liu, Yuan Wei[1];Chen, Jiacheng[2];Zhu, Minhui[2];Yuan, Hai Yang[1];Dai, Sheng[3];Wang, Hai Feng[4,5];Jiang, Zheng[6];Liu, Peng Fei[1];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Adv Mat & Feringa Nobel Prize Scientist J, Sch Chem & Mol Engn, Inst Fine Chem, 130 Meilong Rd, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[6]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, 239 Zhangheng Rd, Shanghai 201204, Peoples R China

年份：2022

卷号：15

期号：1

起止页码：234

外文期刊名：ENERGY & ENVIRONMENTAL SCIENCE

收录：;EI(收录号：20220611612539);WOS:【SCI-EXPANDED(收录号:WOS:000724279300001)】；

基金：This work was financially supported by the National Natural Science Funds for Distinguished Young Scholars (51725201), the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), the Innovation Program of Shanghai Municipal Education Commission (E00014), the National Natural Science Foundation of China (51902105, 21902048), the Fundamental Research Funds for the Central Universities (JKD01211519), the Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400) and the Shanghai Sailing Program (19YF1411600). The authors acknowledge the support by Shanghai Rising-star Program (20QA1402400). Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry. The authors also thank the crew of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF) and the 1W1B beamline of Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analyses.

语种：英文

外文关键词：Computer architecture - Electrocatalysts - Carbon dioxide - Architecture - Pollution control - Shells (structures) - Surface waters - Density functional theory

摘要：The electrosynthesis of valuable chemicals via carbon dioxide reduction reaction (CO2RR) has provided a promising way to address global energy and sustainability problems. However, the selectivity and activity of deep-reduction products (DRPs) still remain as big challenges. Here, a copper-carbon-based catalyst with a hydrophobic core-shell architecture has been constructed and was found to exhibit excellent DRPs of methane generation with a faradaic efficiency of 81 +/- 3% in a neutral medium and a maximum partial current density of -434 mA cm(-2) in a flow cell configuration, which is among the best of CO2-to-CH4 electrocatalysts. Density functional theory calculations suggest that the hydrophobic structure decreasing the water coverage on the catalyst surface can promote the protonation of the *CO intermediate and block CO production, further favoring the generation of methane. These results provide a new insight into the electrosynthesis of DRPs via constructing a hydrophobic core-shell architecture for tuning the surface water coverage.