V-N Co-doped Mesoporous Carbon Nanomaterials as Catalysts for Artificial N2 Reduction

doi:10.11944/j.issn.1000-0518.2020.00.200037

Chinese Journal of Applied Chemistry ›› 2020, Vol. 37 ›› Issue (8): 930-938.DOI: 10.11944/j.issn.1000-0518.2020.00.200037

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V-N Co-doped Mesoporous Carbon Nanomaterials as Catalysts for Artificial N₂ Reduction

LI Lin^a, REN Huimin^a, WEI Bohui^b, LI Jun^b, WANG Jie^b, LI Hui^b, YAO Chenzhong^b,c*

^aSchool of Chemistry and Materials Science,Shanxi Normal University,Linfen,Shanxi 041004,China;
^bDepartment of Applied Chemistry,Yuncheng University,Yuncheng,Shanxi 044000,China;
^cKey Laboratory of Education Ministry for Coal Science and Technology, Taiyuan University of Technology,Taiyuan 030024,China

Received:2020-02-12 Published:2020-08-01 Online:2020-08-07
Contact: YAO Chenzhong, professor; Tel:0359-2513059; E-mail:yaochzh1999@126.com; Research interests:electrochemical catalysis and energy storage
Supported by:
National Natural Science Foundation of China(No.U1810110, No.21576230, No.51808485), China Scholarship Fund, the Natural Science Foundation of Shanxi(No.201903D121105, No.201701D211004, No.201701D221045), the Chemical Key Subject Construction Project of Yuncheng University, the Foundation from Beijing Key Laboratory of Plastics Health and Safety Quality Evaluation Technology(No.BS201709), and the Foundation from the Key Laboratory of Coal Science and Technology from Taiyuan University of Technology(No.MKX201904)

Abstract

Abstract: Compared with the Haber-Bosch process, electrochemical nitrogen fixation can directly convert N₂ to NH₃ under mild environmental conditions, which is the building block of fertilizer for agricultural production. However, the screening of nitrogen reduction electrocatalyst with high activity and high stability is the most important. Here, vanadium doped ZIF-8 was synthesized by the sol-gel method, and used as the precursor to prepare mesoporous carbon electrochemical N₂ reduction reaction (NRR) catalysts at high temperature. The catalysts were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy, etc. The catalyst shows a highly disordered three-dimensional carbon structure. The presence of appropriate amount of V⁵⁺, nitrogen carbide and pyridine nitrogen in the catalyst can promote NRR significantly. In the 0.1 mol/L KOH electrolyte solution, with V doped amount of 1/8 and the applied potential of -0.4 V, the catalyst has the best NRR performance at the calcination temperature of 1100 ℃. The ammonia production rate can reach 7.092 mol/(cm²·h) and the Faraday efficiency (FE%) is 23.88%. Meanwhile, its current density has a slight fluctuation at -0.4 V for 18 h electrochemical reaction, further suggesting that V-N co-doped carbon based mesoporous nanomaterials has high durability.

Key words: mesoporous carbon, V, N co-doping, N₂ reduction reaction, electrolysis

LI Lin, REN Huimin, WEI Bohui, LI Jun, WANG Jie, LI Hui, YAO Chenzhong. V-N Co-doped Mesoporous Carbon Nanomaterials as Catalysts for Artificial N₂ Reduction[J]. Chinese Journal of Applied Chemistry, 2020, 37(8): 930-938.

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V-N Co-doped Mesoporous Carbon Nanomaterials as Catalysts for Artificial N₂ Reduction

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