Atomically Dispersed Nickel(I) on an Alloy‐Encapsulated Nitrogen‐Doped Carbon Nanotube Array for High‐Performance Electrochemical CO 2 Reduction Reaction

Zhang, Tianyu; Han, Xu; Yang, Hongbin; Han, Aijuan; Hu, Enyuan; Li, Yaping; Yang, Xiao‐qing; Wang, Lei; Liu, Junfeng; Liu, Bin

doi:10.1002/anie.202002984

Title: Atomically Dispersed Nickel(I) on an Alloy‐Encapsulated Nitrogen‐Doped Carbon Nanotube Array for High‐Performance Electrochemical CO ₂ Reduction Reaction

Journal Article · Tue May 12 00:00:00 EDT 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202002984· OSTI ID:1637546

Zhang, Tianyu ^[1]; Han, Xu ^[2]; Yang, Hongbin ^[3]; Han, Aijuan ^[2]; Hu, Enyuan ^[4]; Li, Yaping ^[2]; Yang, Xiao‐qing ^[4]; Wang, Lei ^[5]; Liu, Junfeng ^[2];

^[3]

State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 P. R. China, School of Chemical and Biomedical Engineering Nanyang Technological University Singapore Singapore
State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 P. R. China
School of Chemical and Biomedical Engineering Nanyang Technological University Singapore Singapore
Chemistry Division Brookhaven National Laboratory Upton NY USA
College of Chemistry and Molecular Engineering Qingdao University of Science and Technology Qingdao 266042 P. R. China

Abstract Single‐atom catalysts (SACs) show great promise for electrochemical CO ₂ reduction reaction (CRR), but the low density of active sites and the poor electrical conduction and mass transport of the single‐atom electrode greatly limit their performance. Herein, we prepared a nickel single‐atom electrode consisting of isolated, high‐density and low‐valent nickel(I) sites anchored on a self‐standing N‐doped carbon nanotube array with nickel–copper alloy encapsulation on a carbon‐fiber paper. The combination of single‐atom nickel(I) sites and self‐standing array structure gives rise to an excellent electrocatalytic CO ₂ reduction performance. The introduction of copper tunes the d‐band electron configuration and enhances the adsorption of hydrogen, which impedes the hydrogen evolution reaction. The single‐nickel‐atom electrode exhibits a specific current density of −32.87 mA cm ⁻² and turnover frequency of 1962 h ⁻¹ at a mild overpotential of 620 mV for CO formation with 97 % Faradic efficiency.

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Sponsoring Organization:: USDOE

OSTI ID:: 1637546

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Vol. 59 Journal Issue: 29; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 111 works

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