A Supported Pd2 Dual-Atom Site Catalyst for Efficient Electrochemical CO2 Reduction

被引:282
作者
Zhang, Ningqiang [1 ]
Zhang, Xinxin [2 ]
Kang, Yikun [3 ]
Ye, Chenliang [1 ]
Jin, Rui [4 ]
Yan, Han [1 ]
Lin, Rui [1 ]
Yang, Jiarui [1 ]
Xu, Qian [1 ]
Wang, Yu [5 ]
Zhang, Qinghua [6 ]
Gu, Lin [6 ]
Liu, Licheng [2 ]
Song, Weiyu [3 ]
Liu, Jian [3 ]
Wang, Dingsheng [1 ]
Li, Yadong [1 ]
机构
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China
[3] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[4] SINOPEC Res Inst Petr Proc, Xue Yuan Rd 18, Beijing 100083, Peoples R China
[5] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[6] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金; 国家重点研发计划;
关键词
CO2 reduction reaction; dual-atom site catalyst; electron transfer; palladium; single-atom site catalysts;
D O I
10.1002/anie.202101559
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Dual-atom site catalysts (DACs) have emerged as a new frontier in heterogeneous catalysis because the synergistic effect between adjacent metal atoms can promote their catalytic activity while maintaining the advantages of single-atom site catalysts (SACs), like 100 % atomic utilization efficiency and excellent selectivity. Herein, a supported Pd-2 DAC was synthesized and used for electrochemical CO2 reduction reaction (CO2RR) for the first time. The as-obtained Pd-2 DAC exhibited superior CO2RR catalytic performance with 98.2 % CO faradic efficiency at -0.85 V vs. RHE, far exceeding that of Pd-1 SAC, and coupled with long-term stability. The density functional theory (DFT) calculations revealed that the intrinsic reason for the superior activity of Pd-2 DAC toward CO2RR was the electron transfer between Pd atoms at the dimeric Pd sites. Thus, Pd-2 DAC possessed moderate adsorption strength of CO*, which was beneficial for CO production in CO2RR.
引用
收藏
页码:13388 / 13393
页数:6
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