Zhou Limin, Chen Xueqiu, Zhu Shaojun, You Kun, Wang Zheng-Jun, Fan Ru, Li Jun, Yuan Yifei, Wang Xin, Wang Jichang, Chen Yihuang, Jin Huile, Wang Shun, Lv Jing-Jing
Zhejiang Province Key Lab of Leather Engineering, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang, 325000, China.
Zhejiang Engineering Research Center for Electrochemical Energy Materials and Devices, Institute of New Materials and Industrial Technologies, Wenzhou, Zhejiang, 325035, China.
Angew Chem Int Ed Engl. 2024 Apr 24;63(18):e202401924. doi: 10.1002/anie.202401924. Epub 2024 Mar 1.
Nitrate electroreduction reaction (eNO RR) to ammonia (NH) provides a promising strategy for nitrogen utilization, while achieving high selectivity and durability at an industrial scale has remained challenging. Herein, we demonstrated that the performance of eNO RR could be significantly boosted by introducing two-dimensional Cu plates as electrocatalysts and eliminating the general carrier gas to construct a steady fluid field. The developed eNO RR setup provided superior NH Faradaic efficiency (FE) of 99 %, exceptional long-term electrolysis for 120 h at 200 mA cm, and a record-high yield rate of 3.14 mmol cm h. Furthermore, the proposed strategy was successfully extended to the Zn-nitrate battery system, providing a power density of 12.09 mW cm and NH FE of 85.4 %, outperforming the state-of-the-art eNO RR catalysts. Coupled with the COMSOL multiphysics simulations and in situ infrared spectroscopy, the main contributor for the high-efficiency NH production could be the steady fluid field to timely rejuvenate the electrocatalyst surface during the electrocatalysis.
硝酸盐电还原反应(eNO RR)制氨(NH₃)为氮利用提供了一种很有前景的策略,然而在工业规模上实现高选择性和耐久性仍然具有挑战性。在此,我们证明通过引入二维铜板作为电催化剂并去除一般载气以构建稳定的流体场,可以显著提高eNO RR的性能。所开发的eNO RR装置提供了99%的卓越NH₃法拉第效率(FE),在200 mA cm⁻²下进行了120小时的超长时电解,以及创纪录的3.14 mmol cm⁻² h⁻¹的高产率。此外,所提出的策略成功扩展到了锌 - 硝酸盐电池系统,提供了12.09 mW cm⁻²的功率密度和85.4%的NH₃ FE,优于目前最先进的eNO RR催化剂。结合COMSOL多物理场模拟和原位红外光谱,高效NH₃生成的主要贡献因素可能是稳定的流体场,它在电催化过程中能及时使电催化剂表面恢复活力。