文献类型：期刊文献

英文题名：Synergistic Effect of Atomically Dispersed Ni-Zn Pair Sites for Enhanced CO2 Electroreduction

作者：Li, Youzhi[1];Wei, Bo[2,3];Zhu, Minghui[4];Chen, Jiacheng[4];Jiang, Qike[5];Yang, Bin[1];Hou, Yang[1];Lei, Lecheng[1];Li, Zhongjian[1];Zhang, Ruifeng[2,3];Lu, Yingying[1]

机构：[1]Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China;[2]Beihang Univ, Sch Mat Sci & Engn, Ctr Integrated Computat Mat Engn, Beijing 100191, Peoples R China;[3]Beihang Univ, Sch Mat Sci & Engn, Key Lab High Temp Struct Mat & Coatings Technol, Beijing 100191, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[5]Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China

年份：2021

卷号：33

期号：41

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20213510844405);WOS:【SCI-EXPANDED(收录号:WOS:000691791100001)】；

基金：Y.L. and B.W. contributed equally to this work. This work was supported by the Zhejiang University. Y.L. acknowledges support of the National Key R&D Program of China (2018YFA0209600) and the Natural Science Foundation of China (22022813, 21878268). Q.J. acknowledges the financial support from the DNL Cooperation Fund, CAS (DNL201903) and the National Natural Science Foundation of China (No. 51701201). R.Z. acknowledges the support of the National Key Research and Development Program of China (No. 2017YFB0702100), Part of the DFT calculations were performed using the computational resources provided by the School of Materials Science and Engineering, Beihang University. The authors thank Prof. Liang Zhang from the Institute of Functional Nano & Soft Materials, Soochow University for support of original EXAFS data.

语种：英文

外文关键词：atomic-level Ni-Zn pair sites; enhanced CO; (2) electroreduction; mechanistic understanding; synergistic effects; thermodynamic pathways; kinetic pathways

摘要：Dual-atom catalysts have the potential to outperform the well-established single-atom catalysts for the electrochemical conversion of CO2. However, the lack of understanding regarding the mechanism of this enhanced catalytic process prevents the rational design of high-performance catalysts. Herein, an obvious synergistic effect in atomically dispersed Ni-Zn bimetal sites is observed. In situ characterization combined with density functional theory (DFT) calculations reveals that heteronuclear coordination modifies the d-states of the metal atom, narrowing the gap between the d-band centre (epsilon(d)) of the Ni (3d) orbitals and the Fermi energy level (E-F) to strengthen the electronic interaction at the reaction interface, resulting in a lower free energy barrier (Delta G) in the thermodynamic pathway and a reduced activation energy (E-a) as well as fortified metal-C bonding in the kinetic pathway. Consequently, a CO faradaic efficiency of >90% is obtained across a broad potential window from -0.5 to -1.0 V (vs RHE), reaching a maximum of 99% at -0.8 V, superior to that of the Ni/Zn single-metal sites.