Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yuchi Wan, Maojun Pei, Yixiang Tang, Yao Liu, Wei Yan, Jiujun Zhang, Ruitao Lv
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Abstract

Nitrate electroreduction is promising for achieving effluent waste-water treatment and ammonia production with respect to the global nitrogen balance. However, due to the impeded hydrogenation process, high overpotentials need to be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy is developed to optimize the interfacial H2O behavior for accelerating the hydrogenation conversion of nitrate to ammonia at ultralow overpotentials. The well-designed Ru─Ni(OH)2 electrocatalyst shows a remarkable energy efficiency of 44.6% at +0.1 V versus RHE and a nearly 100% Faradaic efficiency for NH3 synthesis at 0 V versus RHE. In situ characterizations and theoretical calculations indicate that Ni(OH)2 can regulate the interfacial H2O structure with a promoted H2O dissociation process and contribute to the spontaneous hydrogen spillover process for boosting NO3 electroreduction to NH3 at Ru sites. Furthermore, the assembled rechargeable Zn-NO3/ethanol battery system exhibits an outstanding long-term cycling stability during the charge–discharge tests with the production of high-value-added ammonium acetate, showing great potential for simultaneously achieving nitrate removal, energy conversion, and chemical synthesis. This work can not only provide a guidance for interfacial H2O regulation in extensive hydrogenation reactions but also inspire the design of a novel hybrid flow battery with multiple functions.

超低过电位下硝酸盐电还原制氨的界面水调节
硝酸盐电还原有望实现废水处理和氨生产,相对于全球氮平衡。然而,由于加氢过程受阻,硝酸盐电还原过程中需要克服高过电位,造成大量的能量消耗。本文提出了一种氢氧化物调节策略,以优化界面水行为,从而在超低过电位下加速硝酸盐加氢转化为氨。设计良好的Ru─Ni(OH)2电催化剂在+0.1 V时的能量效率为44.6%,在0 V时的NH3合成法拉第效率接近100%。原位表征和理论计算表明,Ni(OH)2可以通过促进H2O解离过程调节界面水结构,促进Ru位点NO3−电还原为NH3的自发氢溢出过程。此外,组装的可充电Zn - NO3−/乙醇电池系统在生产高附加值乙酸铵的充放电测试中表现出出色的长期循环稳定性,显示出同时实现硝酸盐去除、能量转换和化学合成的巨大潜力。这项工作不仅可以为广泛加氢反应的界面水调节提供指导,而且可以启发新型多功能混合液流电池的设计。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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