NbC Nanoparticles Decorated Carbon Nanofibers as Highly Active and Robust Heterostructural Electrocatalysts for Ammonia Synthesis

Zhihao Zhang; Aihui Niu; Yaxin Lv; Haoran Guo; Jun Song Chen; Qian Liu; Kai Dong; Xuping Sun; Tingshuai Li

doi:10.1002/anie.202406441

NbC Nanoparticles Decorated Carbon Nanofibers as Highly Active and Robust Heterostructural Electrocatalysts for Ammonia Synthesis

Angew Chem Int Ed Engl. 2024 May 14:e202406441. doi: 10.1002/anie.202406441. Online ahead of print.

Authors

Zhihao Zhang¹, Aihui Niu², Yaxin Lv³, Haoran Guo⁴, Jun Song Chen², Qian Liu⁵, Kai Dong⁶, Xuping Sun⁷, Tingshuai Li⁸

Affiliations

¹ University of Electronic Science and Technology of China, School of Materials and Energy, Chengdu, CHINA.
² University of Electronic Science and Technology of China, School of Materials and Energy, No.2006, Xiyuan Ave, West Hi-Tech Zone, Chengdu, Sichuan, P.R.China, 611731, Chengdu, CHINA.
³ University of Electronic Science and Technology of China, School of Materials and Energy, Xiyuan road 2006, CHINA.
⁴ Xiangtan University, Department of Chemistry, Yuhu District, Xiangtan, Hunan, China, 411105, Xiangtan, CHINA.
⁵ Chengdu University, Institute for Advanced Study, No. 2025, Chengluo Avenue, Chengdu City, Sichuan Province, China, 611731, Chengdu, CHINA.
⁶ Shandong Normal University, College of Chemistry, No.88 East Wenhua Road, Lixia District, Ji'nan, Shandong, China, Jinan, CHINA.
⁷ Shandong Normal University, Department of Chemistry, No.2006, Xiyuan Ave, West Hi-Tech Zone, Chengdu, Sichuan, China, Chengdu, CHINA.
⁸ University of Electronic Science and Technology of China, School of Materials and Energy, Xiyuan road 2006, 611731, Chengdu, CHINA.

PMID: 38742483
DOI: 10.1002/anie.202406441

Abstract

Transition-metal carbides with metallic properties have been extensively used as electrocatalysts due to their excellent conductivity and unique electronic structures. Herein, NbC nanoparticles decorated carbon nanofibers (NbC@CNFs) are proposed as an efficient and robust catalyst for electrochemical synthesis of ammonia from nitrate/nitrite reduction, which achieves a high Faradaic efficiency (FE) of 94.4% and a large ammonia yield of 30.9 mg h-1 mg-1cat.. In situ electrochemical tests reveal the nitrite reduction at the catalyst surface follows the *NO pathway and theoretical calculations reveal the formation of NbC@CNFs heterostructure significantly broadens density of states nearby the Fermi energy. Finite element simulations unveil that the current and electric field converge on the NbC nanoparticles along the fiber, suggesting the dispersed carbides are highly active for nitrite reduction.

Keywords: DFT calculation; Finite element simulation; carbide; nitrate reduction.