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Research Article

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

Yiqun Chen1, Yuejian Yao1, Yujian Xia2, Kun Mao1, Gongao Tang1, Qiang Wu1( ), Lijun Yang1( ), Xizhang Wang1, Xuhui Sun2, Zheng Hu1( )
Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Soochow University-Western University Centre for Synchrotron Radiation Research, Institute of Functional Nano and Soft Material (FUNSOM), Soochow University, Suzhou 215123, China
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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.

Keywords

CO2 electroreductionsingle-site catalystsnickel-nitrogen-carbonS-dopinghierarchical carbon nanocages

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Nano Research
Volume 13 Issue 10,
October 2020
Pages 2777-2783
DOI: 10.1007/s12274-020-2928-0
Cite this article:
Chen Y, Yao Y, Xia Y, et al. Advanced Ni-Nx-C single-site catalysts for CO2 electroreduction to CO based on hierarchical carbon nanocages and S-doping. Nano Research, 2020, 13(10): 2777-2783. https://doi.org/10.1007/s12274-020-2928-0
Topics:
CarbonCarbon dioxideCharge transferChlorine compoundsElectrocatalystsElectrolytic reduction Electronic structureNickel compoundsNitrogenPorous materials

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Received: 29 April 2020
Revised: 09 June 2020
Accepted: 11 June 2020
Published: 05 October 2020
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020
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