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Nano Research

Article Title

Advanced Ni-Nx-C single-site catalysts for CO2 electroreduction to CO based on hierarchical carbon nanocages and S-doping

Authors

Yiqun Chen, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Yuejian Yao, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Yujian Xia, Soochow University-Western University Centre for Synchrotron Radiation Research, Institute of Functional Nano and Soft Material (FUNSOM), Soochow University, Suzhou 215123, China
Kun Mao, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Gongao Tang, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Qiang Wu, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Lijun Yang, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Xizhang Wang, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Xuhui Sun, Soochow University-Western University Centre for Synchrotron Radiation Research, Institute of Functional Nano and Soft Material (FUNSOM), Soochow University, Suzhou 215123, China
Zheng Hu, Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China

Keywords

CO2 electroreduction, single-site catalysts, nickel-nitrogen-carbon, S-doping, hierarchical carbon nanocages

Abstract

Metal-nitrogen-carbon materials are promising catalysts for CO2 electroreduction to CO. Herein, by taking the unique hierarchical carbon nanocages as the support, an advanced nickel-nitrogen-carbon single-site catalyst is conveniently prepared by pyrolyzing the mixture of NiCl2 and phenanthroline, which exhibits a Faradaic efficiency plateau of > 87% in a wide potential window of −0.6 – −1.0 V. Further S-doping by adding KSCN into the precursor much enhances the CO specific current density by 68%, up to 37.5 A·g−1 at −0.8 V, along with an improved CO Faradaic efficiency plateau of > 90%. Such an enhancement can be ascribed to the facilitated CO pathway and suppressed hydrogen evolution from thermodynamic viewpoint as well as the increased electroactive surface area and improved charge transfer fromkinetic viewpoint due to the S-doping. This study demonstrates a simple and effective approach to advanced electrocatalysts by synergetic modification of the porous carbon-based support and electronic structure of the active sites.

Graphical Abstract

Publisher

Tsinghua University Press

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