化工进展 ›› 2021, Vol. 40 ›› Issue (12): 6670-6687.DOI: 10.16085/j.issn.1000-6613.2020-2520

• 工业催化 • 上一篇    下一篇

电催化氮气还原合成氨反应中抑制水解析氢竞争的研究进展

张婷(), 孙晓红, 于宏兵, 董恒()   

  1. 南开大学环境科学与工程学院,天津 300350
  • 收稿日期:2020-12-17 修回日期:2021-03-08 出版日期:2021-12-05 发布日期:2021-12-21
  • 通讯作者: 董恒
  • 作者简介:张婷(1995—),女,硕士研究生,研究方向为电化学。E-mail:zhangt@nankai.edu.cn
  • 基金资助:
    国家自然科学基金(51708300)

Research progress of inhibiting hydrogen evolution in electro-catalytic ammonia synthesis

ZHANG Ting(), SUN Xiaohong, YU Hongbing, DONG Heng()   

  1. College of Environmental Science and Engineering, Nankai University, TianJin 300350, China
  • Received:2020-12-17 Revised:2021-03-08 Online:2021-12-05 Published:2021-12-21
  • Contact: DONG Heng

摘要:

传统工业合成氨Haber-Bosch工艺条件要求严苛,并且存在高能耗以及高CO2排放问题。电催化氮气还原(nitrogen reduction reaction, NRR)是一种在常温常压下利用氮气合成氨的新工艺,具有成本低、反应条件温和、环境友好等优势。但该反应所需过电位较高,水解析氢反应(hydrogen evolution reaction, HER)竞争明显,导致电流密度和选择性较低,无法达到工业应用水平。本文在介绍电催化NRR合成氨的反应机理的基础上,主要从氮气分子的吸附活化和电还原阶段反应过程出发,综述了电催化氮气还原合成氨反应中HER与NRR的竞争机制。重点梳理了通过设计催化剂和反应体系抑制HER的国内外最新研究成果,最后对电催化NRR合成氨面临的挑战和机遇进行了展望。

关键词: 电化学, 催化剂, 活化, 选择性, 氨, 氮气还原, 析氢反应

Abstract:

The Haber-Bosch process is of high energy consumption and high CO2 emissions. Electro-catalytic nitrogen reduction reaction (NRR) is a novel process which works at room temperature and atmospheric pressure with N2 input. It has the advantages of low cost, mild reaction conditions and environmental friendliness. However, due to its high overpotential, low current density and low selectivity, electrocatalytic NRR currently is still in the laboratory research stage. Particularly, the Faraday efficiency is severely limited by the hydrogen evolution reaction (HER). In this paper, we introduced the reaction mechanism of ammonia synthesis by electrocatalytic NRR. Moreover, we reviewed the competition mechanism between HER and NRR, mainly from the adsorption and activation of nitrogen and the specific reaction of electroreduction stages. This article focused on the latest research achievements in controlling HER by rational catalysts and reaction system design. Finally, we summarized the challenges in the development of electrocatalytic NRR for ammonia synthesis and gave the corresponding solutions. The potential application of electrocatalytic NRR ammonia synthesis under mild conditions is proposed.

Key words: electrochemistry, catalyst, activation, selectivity, ammonia, nitrogen reduction reaction, hydrogen evolution reaction

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