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Optimizing oxygen vacancies through grain boundary engineering to enhance electrocatalytic nitrogen reduction

催化作用 材料科学 法拉第效率 电解质 晶界 析氧 氮气 化学工程 氧气 空位缺陷 X射线光电子能谱 电子转移 电解 电化学 化学 电极 冶金 物理化学 微观结构 结晶学 工程类 生物化学 有机化学
作者
Xiu Zhong,Enxian Yuan,Fu Yang,Yang Liu,Hao Lü,Jun Yang,Fei Gao,Yu Zhou,Jianming Pan,Jiawei Zhu,Chao Yu,Chengzhang Zhu,Aihua Yuan,Edison Huixiang Ang
出处
期刊:Proceedings of the National Academy of Sciences of the United States of America [National Academy of Sciences]
卷期号:120 (40) 被引量:53
标识
DOI:10.1073/pnas.2306673120
摘要

Electrocatalytic nitrogen reduction is a challenging process that requires achieving high ammonia yield rate and reasonable faradaic efficiency. To address this issue, this study developed a catalyst by in situ anchoring interfacial intergrown ultrafine MoO 2 nanograins on N-doped carbon fibers. By optimizing the thermal treatment conditions, an abundant number of grain boundaries were generated between MoO 2 nanograins, which led to an increased fraction of oxygen vacancies. This, in turn, improved the transfer of electrons, resulting in the creation of highly active reactive sites and efficient nitrogen trapping. The resulting optimal catalyst, MoO 2 /C 700 , outperformed commercial MoO 2 and state-of-the-art N 2 reduction catalysts, with NH 3 yield and Faradic efficiency of 173.7 μg h −1 mg −1 cat and 27.6%, respectively, under − 0.7 V vs. RHE in 1 M KOH electrolyte. In situ X-ray photoelectron spectroscopy characterization and density functional theory calculation validated the electronic structure effect and advantage of N 2 adsorption over oxygen vacancy, revealing the dominant interplay of N 2 and oxygen vacancy and generating electronic transfer between nitrogen and Mo(IV). The study also unveiled the origin of improved activity by correlating with the interfacial effect, demonstrating the big potential for practical N 2 reduction applications as the obtained optimal catalyst exhibited appreciable catalytic stability during 60 h of continuous electrolysis. This work demonstrates the feasibility of enhancing electrocatalytic nitrogen reduction by engineering grain boundaries to promote oxygen vacancies, offering a promising avenue for efficient and sustainable ammonia production.
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