Improving NiN<sub>X</sub> and pyridinic N active sites with space-confined pyrolysis for effective CO<sub>2</sub> electroreduction

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

doi:10.1016/j.esci.2022.05.002

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Article Navigation > eScience > 2022 > 2(4): 445-452

Zhu Zhaozhao, Li Zhao, Wang Junjie, Li Rong, Chen Haiyuan, Li Yulan, Chen Jun Song, Wu Rui, Wei Zidong. Improving NiNX and pyridinic N active sites with space-confined pyrolysis for effective CO2 electroreduction[J]. eScience, 2022, 2(4): 445-452. doi: 10.1016/j.esci.2022.05.002

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Zhu Zhaozhao, Li Zhao, Wang Junjie, Li Rong, Chen Haiyuan, Li Yulan, Chen Jun Song, Wu Rui, Wei Zidong. Improving NiN_X and pyridinic N active sites with space-confined pyrolysis for effective CO₂ electroreduction[J]. eScience, 2022, 2(4): 445-452. doi: 10.1016/j.esci.2022.05.002

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

doi: 10.1016/j.esci.2022.05.002

Zhu Zhaozhao^{a, c, 1},
Li Zhao^{a, 1},
Wang Junjie^a,
Li Rong^c,
Chen Haiyuan^a,
Li Yulan^a,
Chen Jun Song^a,
Wu Rui^{a
,
,},
Wei Zidong^{b
,
,}

a.
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China
b.
School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 400044, China
c.
College of Chemistry and Chemical Engineering, China West Normal University, Nanchong, 637000, China

More Information

Corresponding author: E-mail address: ruiwu0904@uestc.edu.cn (R. Wu); E-mail address: zdwei@cqu.edu.cn (Z. Wei)
Received Date: 2022-02-08
Revised Date: 2022-04-17
Accepted Date: 2022-05-11

Available Online: 2022-05-27

Abstract

Abstract

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 NiN_X-pyridinic N active species (denoted as h-Ni-N-C) developed using a facile electrospinning and SiO₂ space-confined pyrolysis strategy. The NiN_X-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.
- CO₂ electroreduction,
- NiN_X-pyridinic N,
- Porous carbon nanofiber,
- SiO₂ confinement

● DFT calculations reveal that NiN₄ and pyridinic N active species facilitate the adsorption and desorption of intermediates.
● A porous hollow N-doped carbon nanofiber with NiNX-pyridinic N active species (h-N-N-C) catalyst was prepared through a simple electrospinning and SiO₂ space-confined pyrolysis strategy.
● The h-Ni-N-C catalyst exhibits a high FE_CO of 91.3% and a large j_CO of −15.1 mA cm⁻² toward CO production.
¹ These authors contributed equally to this work.

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