Improving NiNX and pyridinic N active sites with space-confined pyrolysis for effective CO2 electroreduction

Zhaozhao Zhu; Zhao Li; Junjie Wang; Rong Li; Haiyuan Chen; Yulan Li; Jun Song Chen; Rui Wu; Zidong Wei

eScience (Jul 2022)

Improving NiNX and pyridinic N active sites with space-confined pyrolysis for effective CO2 electroreduction

Zhaozhao Zhu,
Zhao Li,
Junjie Wang,
Rong Li,
Haiyuan Chen,
Yulan Li,
Jun Song Chen,
Rui Wu,
Zidong Wei

Affiliations

Zhaozhao Zhu: School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China; College of Chemistry and Chemical Engineering, China West Normal University, Nanchong, 637000, China
Zhao Li: School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China
Junjie Wang: School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China
Rong Li: College of Chemistry and Chemical Engineering, China West Normal University, Nanchong, 637000, China
Haiyuan Chen: School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China
Yulan Li: School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China
Jun Song Chen: School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China
Rui Wu: School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China; Corresponding authors.
Zidong Wei: School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 400044, China; Corresponding authors.

Journal volume & issue: Vol. 2, no. 4
pp. 445 – 452

Abstract

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Even though various nickel–nitrogen–carbon (Ni-N-C) combinations are prospective low-cost catalysts for the CO2 electroreduction reaction (CO2RR), which is one avenue for attaining carbon neutrality, the detailed role of different N species has hardly been investigated. Here, we report a hollow porous N-doped carbon nanofiber with NiNX-pyridinic N active species (denoted as h-Ni-N-C) developed using a facile electrospinning and SiO2 space-confined pyrolysis strategy. The NiNX-pyridinic N species are facilely generated during the pyrolysis process, giving rise to enhanced activity and selectivity for the CO2RR. The optimized h-Ni-N-C exhibits a high CO Faradaic efficiency of 91.3% and a large current density of −15.1 mA cm−2 at −0.75 V versus reversible hydrogen electrode in an H-cell. Density functional theory (DFT) results show that NiN4-pyridinic N species demonstrate a lower free energy for the catalyst's rate-determining step than isolated NiN4 and pyridinic N species, without affecting the desorption of CO∗ intermediate.

Published in eScience

ISSN: 2667-1417 (Online)
Publisher: KeAi Communications Co. Ltd.
Country of publisher: China
LCC subjects: Technology: Mechanical engineering and machinery; Technology: Electrical engineering. Electronics. Nuclear engineering: Electronics
Website: https://www.keaipublishing.com/en/journals/escience/

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