文献类型：期刊文献

英文题名：Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO2RR

作者：Huang, Kai[1,2];Li, Ru[1,2];Qi, Haodong[1,2];Yang, Shuai[3];An, Shuhao[1,2];Lian, Cheng[1,2,4];Xu, Qing[5];Liu, Honglai[1,2,4];Hu, Jun[1,2]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Joint Int Res Lab Precis Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China;[4]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[5]Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China

年份：2024

卷号：14

期号：11

起止页码：8889

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20242216175611);WOS:【SCI-EXPANDED(收录号:WOS:001233756000001)】；

基金：The authors acknowledge the financial support from the National Natural Science Foundation of China (Nos. 22250005, 22278126, 22308095, and 52303288), the Youth Innovation Promotion Association of Chinese Academy of Sciences (E324441401), the Fundamental Research Funds for the Central Universities, the China Postdoctoral Science Foundation (2022M720049, 2023M732318), and the financial support of the SINOPEC. The authors would also like to thank beamline BL14W1 at SSRF for the beam time allocation and assistance.

语种：英文

外文关键词：dual-atomic metal catalyst; sulfur modulating; electrocatalytic CO2 reduction; bidentate configuration; current density

摘要：The formation of dual-atom catalysts or heteroatom ligand modulation is the most promising strategy for optimizing single-atom catalysts (SACs) for the more efficient conversion of CO2 to valuable chemicals. However, heteroatom ligands introduced into the dual-atomic sites are expected but still under-explored. In this study, a dual-atom Fe-Ni pair electrocatalyst with N- and S-coordination in porous carbon nanosheets was conceptually predicted for electrocatalytic CO2 reduction to CO (CO2RR). In contrast to SACs and traditional diatomic catalysts (DACs), joined S-coordination can balance the cooperative activities of Fe and Ni sites, making the CO2 adsorption configuration bidentate at both Fe-Ni sites. This regulation leads to a substantial change in CO* adsorption from Fe to Ni sites, facilitating CO desorption and boosting the electrocatalytic CO2RR. Experimental results demonstrate that the obtained FeNi-NSC catalyst achieves high selectivity with the Faradaic efficiencies for CO of 96.1%, and a remarkable activity with the turnover frequency of 6526.9 h(-1) at -1.0 V, which were over 4.5 and 2.5 times of those from the single Fe or Ni sites. This work gives us insight into designing highly effective catalysts guided by theoretical calculation.