A universal ligand mediated method for large scale synthesis of transition metal single atom catalysts

被引:601
作者
Yang, Hongzhou [1 ,2 ]
Shang, Lu [1 ]
Zhang, Qinghua [3 ]
Shi, Run [1 ]
Waterhouse, Geoffrey I. N. [4 ]
Gu, Lin [3 ,5 ]
Zhang, Tierui [1 ,2 ]
机构
[1] Chinese Acad Sci, Key Lab Photochem Convers & Optoelect Mat, Tech Inst Phys & Chem, Beijing 100190, Peoples R China
[2] Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Inst Phys, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China
[4] Univ Auckland, Sch Chem Sci, Auckland 1142, New Zealand
[5] Songshan Lake Mat Lab, Dongguan 523808, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
ORGANIC FRAMEWORKS; REDUCTION; IDENTIFICATION; CARBON; COPPER; SITES; CO2;
D O I
10.1038/s41467-019-12510-0
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
There is interest in metal single atom catalysts due to their remarkable activity and stability. However, the synthesis of metal single atom catalysts remains somewhat ad hoc, with no universal strategy yet reported that allows their generic synthesis. Herein, we report a universal synthetic strategy that allows the synthesis of transition metal single atom catalysts containing Cr, Mn, Fe, Co, Ni, Cu, Zn, Ru, Pt or combinations thereof. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure spectroscopy confirm that the transition metal atoms are uniformly dispersed over a carbon black support. The introduced synthetic method allows the production of carbon-supported metal single atom catalysts in large quantities (>1 kg scale) with high metal loadings. A Ni single atom catalyst exhibits outstanding activity for electrochemical reduction of carbon dioxide to carbon monoxide, achieving a 98.9% Faradaic efficiency at -1.2 V.
引用
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页数:9
相关论文
共 34 条
[1]   Single-atom catalysis: Bridging the homo- and heterogeneous catalysis [J].
Chen, Fang ;
Jiang, Xunzhu ;
Zhang, Leilei ;
Lang, Rui ;
Qiao, Botao .
CHINESE JOURNAL OF CATALYSIS, 2018, 39 (05) :893-898
[2]   Rational Design of Single Molybdenum Atoms Anchored on N-Doped Carbon for Effective Hydrogen Evolution Reaction [J].
Chen, Wenxing ;
Pei, Jiajing ;
He, Chun-Ting ;
Wan, Jiawei ;
Ren, Hanlin ;
Zhu, Youqi ;
Wang, Yu ;
Dong, Juncai ;
Tian, Shubo ;
Cheong, Weng-Chon ;
Lu, Siqi ;
Zheng, Lirong ;
Zheng, Xusheng ;
Yan, Wensheng ;
Zhuang, Zhongbin ;
Chen, Chen ;
Peng, Qing ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (50) :16086-16090
[3]   Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications [J].
Chen, Yuanjun ;
Ji, Shufang ;
Chen, Chen ;
Peng, Qing ;
Wang, Dingsheng ;
Li, Yadong .
JOULE, 2018, 2 (07) :1242-1264
[4]   Isolated Single Iron Atoms Anchored on N-Doped Porous Carbon as an Efficient Electrocatalyst for the Oxygen Reduction Reaction [J].
Chen, Yuanjun ;
Ji, Shufang ;
Wang, Yanggang ;
Dong, Juncai ;
Chen, Wenxing ;
Li, Zhi ;
Shen, Rongan ;
Zheng, Lirong ;
Zhuang, Zhongbin ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (24) :6937-6941
[5]   In Situ Raman Spectroscopy of Copper and Copper Oxide Surfaces during Electrochemical Oxygen Evolution Reaction: Identification of CuIII Oxides as Catalytically Active Species [J].
Deng, Yilin ;
Handoko, Albertus D. ;
Du, Yonghua ;
Xi, Shibo ;
Yeo, Boon Siang .
ACS CATALYSIS, 2016, 6 (04) :2473-2481
[6]   General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities [J].
Fei, Huilong ;
Dong, Juncai ;
Feng, Yexin ;
Allen, Christopher S. ;
Wan, Chengzhang ;
Volosskiy, Boris ;
Li, Mufan ;
Zhao, Zipeng ;
Wang, Yiliu ;
Sun, Hongtao ;
An, Pengfei ;
Chen, Wenxing ;
Guo, Zhiying ;
Lee, Chain ;
Chen, Dongliang ;
Shakir, Imran ;
Liu, Mingjie ;
Hu, Tiandou ;
Li, Yadong ;
Kirkland, Angus I. ;
Duan, Xiangfeng ;
Huang, Yu .
NATURE CATALYSIS, 2018, 1 (01) :63-72
[7]   Size-Dependent Electrocatalytic Reduction of CO2 over Pd Nanoparticles [J].
Gao, Dunfeng ;
Zhou, Hu ;
Wang, Jing ;
Miao, Shu ;
Yang, Fan ;
Wang, Guoxiong ;
Wang, Jianguo ;
Bao, Xinhe .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (13) :4288-4291
[8]   Single Atom (Pd/Pt) Supported on Graphitic Carbon Nitride as an Efficient Photocatalyst for Visible-Light Reduction of Carbon Dioxide [J].
Gao, Guoping ;
Jiao, Yan ;
Waclawik, Eric R. ;
Du, Aijun .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (19) :6292-6297
[9]   Achieving a Record-High Yield Rate of 120.9 μgNH3 mgcat-1. h-1 for N2 Electrochemical Reduction over Ru Single-Atom Catalysts [J].
Geng, Zhigang ;
Liu, Yan ;
Kong, Xiangdong ;
Li, Pai ;
Li, Kan ;
Liu, Zhongyu ;
Du, Junjie ;
Shu, Miao ;
Si, Rui ;
Zeng, Jie .
ADVANCED MATERIALS, 2018, 30 (40)
[10]  
Hammer B, 2000, ADV CATAL, V45, P71