Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion

IF 15.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-02-27 DOI:10.1021/jacs.4c1738010.1021/jacs.4c17380

Xin Li, Guangtong Hai, Daniel H. C. Wan, Yiwen Liao, Zhangyi Yao, Fenglin Zhao, Lingzhi Huang, Jinsong Zhou, Gang Li, Gao-Feng Chen*, Feng Ryan Wang*, Michael K. H. Leung* and Haihui Wang*,

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Abstract

Current nitrate production involves a two-step thermochemical process that is energy-intensive and generates substantial CO₂ emissions. Sustainable NO₃^– production via the nitrogen electrooxidation reaction powered by renewable electricity is highly desirable, but the Faradaic efficiency (FE) at high production rates is unsatisfactory due to competition from the oxygen evolution reaction (OER). In this study, we propose reengineering the catalyst’s microstructure-to-macroenvironment interface by particularly utilizing the previously considered unfavored oxygen from the OER. We demonstrate that the re-engineered interface facilitates a record-breaking FE of 35.52% under 8 atm air, with an impressive increase in FE (41.56%) observed during a continuous electrochemical process lasting for 60 h due to the in situ formation of the O₂-rich macro-interface environment. The revelation is anticipated to furnish groundbreaking perspectives for the reaction systems design in electrochemical nitrate production and other electrocatalytic fields.

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有利于原本不利的氧以增强氮到硝酸盐的电转化

目前的硝酸盐生产涉及两步热化学过程，这是一个能源密集型过程，并产生大量的二氧化碳排放。通过可再生电力驱动的氮电氧化反应可持续生产NO3 -是非常理想的，但由于来自析氧反应（OER）的竞争，高生产率下的法拉第效率（FE）是不令人满意的。在这项研究中，我们建议重新设计催化剂的微观结构-宏观环境界面，特别是利用以前认为来自OER的不利氧。研究表明，在8 atm空气中，重新设计的界面促进了创纪录的35.52%的FE，在持续60 h的连续电化学过程中，由于原位形成了富含o2的宏观界面环境，FE显著增加（41.56%）。这一发现有望为电化学硝酸盐生产和其他电催化领域的反应系统设计提供突破性的视角。

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.