Highly Boosted Reaction Kinetics in Carbon Dioxide Electroreduction by Surface-Introduced Electronegative Dopants

Zheng W, Wang Y, Shuai L, Wang X, He F, Lei C, Li Z, Yang B, Lei L, Yuan C, Qiu M, Hou Y, Feng X (2021)

Publication Type: Journal article

Publication year: 2021

Journal

Advanced Functional Materials Wiley-VCH Verlag

Book Volume: 31

Article Number: 2008146

Journal Issue: 15

DOI: 10.1002/adfm.202008146

Abstract

Effectively improving the selectivity while reducing the overpotential over the electroreduction of CO2 (CO2ER) has been challenging. Herein, electronegative N atoms and coordinatively unsaturated Ni-N3 moieties co-anchored carbon nanofiber (Ni-N3-NCNFs) catalyst via an integrated electrospinning and carbonization strategy are reported. The catalyst exhibits a maximum CO Faradaic efficiency (F.E.) of 96.6%, an onset potential of −0.3 V, and a low Tafel slope of 71 mV dec−1 along with high stability over 100 h. Aberration corrected scanning transmission electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy identify the atomically dispersed Ni-N3 sites with Ni atom bonded by three pyridinic N atoms. The existence of abundant electronegative N dopants adjoin the Ni-N3 centers in Ni-N3-NCNFs. Theoretical calculations reveal that both, the undercoordinated Ni-N3 centers and their first neighboring C atoms modified by extra N dopants, display the positive effect on boosting CO2 adsorption and water dissociation processes, thus accelerating the CO2ER kinetics process. Furthermore, a designed Zn-CO2 battery with the cathode of Ni-N3-NCNFs delivers a maximum power density of 1.05 mW cm−2 and CO F.E. of 96% during the discharge process, thus providing a promising approach to electric energy output and chemical conversion.

Involved external institutions

Zhejiang University CN China (CN) Chinese Academy of Sciences (CAS) / 中国科学院 CN China (CN) Central China Normal University (CCNU) / Huazhong Normal University / 华中师范大学 CN China (CN) Zhejiang University of Technology (ZJUT) / 浙江工业大学 CN China (CN) Case Western Reserve University US United States (USA) (US) Technische Universität Dresden DE Germany (DE)

How to cite

APA:

Zheng, W., Wang, Y., Shuai, L., Wang, X., He, F., Lei, C.,... Feng, X. (2021). Highly Boosted Reaction Kinetics in Carbon Dioxide Electroreduction by Surface-Introduced Electronegative Dopants. Advanced Functional Materials, 31(15). https://doi.org/10.1002/adfm.202008146

MLA:

Zheng, Wanzhen, et al. "Highly Boosted Reaction Kinetics in Carbon Dioxide Electroreduction by Surface-Introduced Electronegative Dopants." Advanced Functional Materials 31.15 (2021).

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