·H effectively enhance electrocatalytic nitrogen fixation

Yuyao Sun; Yaodong Yu; Wenxia Xu; Di Wu; Yingying Wei; Jianping Lai; Lei Wang

doi:10.1016/j.jcis.2023.02.056

·H effectively enhance electrocatalytic nitrogen fixation

J Colloid Interface Sci. 2023 Jun 15:640:619-625. doi: 10.1016/j.jcis.2023.02.056. Epub 2023 Mar 2.

Authors

Yuyao Sun¹, Yaodong Yu¹, Wenxia Xu¹, Di Wu¹, Yingying Wei¹, Jianping Lai², Lei Wang³

Affiliations

¹ Key Laboratory of Eco-chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China.
² Key Laboratory of Eco-chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China. Electronic address: jplai@qust.edu.cn.
³ Key Laboratory of Eco-chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China; Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection, College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China. Electronic address: inorchemwl@126.com.

PMID: 36889059
DOI: 10.1016/j.jcis.2023.02.056

Abstract

Nowadays, most reported ammonia (NH₃) yields and Faradaic efficiency (FE) of electrocatalysts are very low in the field of electrocatalytic nitrogen reduction reactions (NRR). Here, we are reported ·H for the first time in the field of electrocatalytic NRR, which are generated by sulfite (SO₃^2-) and H₂O in electrolyte solutions upon exposure to UV light. The high NH₃ yields can achieve 100.7 μg h^-1 mg_cat^-1, while stability can achieve 64 h and the FE can achieve 27.1% at -0.3 V (vs. RHE) with UV irradiation. In situ Fourier transform infrared spectroscopy (FTIR), electron spin resonance (ESR), density functional theory (DFT) and ¹H nuclear magnetic resonance (NMR) tests showed that the ∙H effectively lowered the reaction energy barrier at each step of the NRR process and inhibits the occurrence of competitive hydrogen evolution reaction (HER). This explores the path and provides ideas for the field of electrocatalysis involving water.

Keywords: Electrolyte solutions; NRR; Transition metal oxide; UV irradiation; ·H.