Guo Xuecheng, Wang Zhongliao, Gao Yuan, Zhang Chao, Zhang Shuai, Sang Shuaikang, Ma Jun, Sun Shuhui, Murzin Dmitry Yu, Low Jingxiang, Shao Tao, Xiong Yujie
School of Chemistry and Materials Science, and Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, China.
Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Huaibei Normal University, Huaibei, Anhui, 235000, China.
Angew Chem Int Ed Engl. 2024 Oct 1;63(40):e202410517. doi: 10.1002/anie.202410517. Epub 2024 Aug 13.
Electrochemical nitrogen oxide ions reduction reaction (NO RR) shows great opportunity for ammonia production under ambient conditions. Yet, performing NO RR in strong acidic conditions remains challenging due to the corrosion effect on the catalyst and competing hydrogen evolution reactions. Here, we demonstrate a stable LaSrNiFeO perovskite oxide for the NO RR at pH 0, achieving a Faradaic efficiency for ammonia of approaching 100 % at a current density of 2 A cm in a H-type cell. At industrially relevant current density, the NO RR system shows stable cell voltage and Faradaic efficiency for >350 h in membrane electrode assembly (MEA) at pH 0. By integrating the catalyst in a stacked MEA with a series connection, we have successfully obtained a record-breaking 2.578 g h NH production rate at 20 A. This catalyst's unique acid-operability streamlines downstream ammonia utilization for direct ammonium salt production and upstream integration with NO sources. Techno-economic and lifecycle assessments reveal substantial economic advantages for this ammonia production strategy, even when coupled with a plasma-based NO production system, presenting a sustainable complement to the conventional Haber-Bosch process.
电化学氮氧化物离子还原反应（NO RR）在环境条件下展现出了巨大的制氨潜力。然而，在强酸性条件下进行NO RR仍具有挑战性，这是由于对催化剂的腐蚀作用以及竞争性析氢反应。在此，我们展示了一种用于在pH值为0时进行NO RR的稳定的LaSrNiFeO钙钛矿氧化物，在H型电解槽中，在2 A cm的电流密度下，实现了接近100%的氨法拉第效率。在工业相关电流密度下，该NO RR系统在pH值为0的膜电极组件（MEA）中，在>350 h的时间内显示出稳定的电池电压和法拉第效率。通过将催化剂集成到串联连接的堆叠式MEA中，我们成功地在20 A时获得了创纪录的2.578 g h NH产率。这种催化剂独特的耐酸性简化了下游氨用于直接生产铵盐以及上游与NO源整合的利用过程。技术经济和生命周期评估表明，即使与基于等离子体的NO生产系统相结合，这种制氨策略也具有显著的经济优势，为传统哈伯-博施法提供了可持续的补充。
