Liao Wanru, Wang Jun, Ni Ganghai, Liu Kang, Liu Changxu, Chen Shanyong, Wang Qiyou, Chen Yingkang, Luo Tao, Wang Xiqing, Wang Yanqiu, Li Wenzhang, Chan Ting-Shan, Ma Chao, Li Hongmei, Liang Ying, Liu Weizhen, Fu Junwei, Xi Beidou, Liu Min
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083, PR China.
Centre for Metamaterial Research & Innovation, Department of Engineering, University of Exeter, Exeter, EX4 4QF, UK.
Nat Commun. 2024 Feb 10;15(1):1264. doi: 10.1038/s41467-024-45534-2.
Nitrate (NO) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO reduction reaction (NORR) emerges as an attractive route for enabling NO removal and sustainable ammonia (NH) synthesis. However, it suffers from insufficient proton (H) supply in high pH conditions, restricting NO-to-NH activity. Herein, we propose a halogen-mediated H feeding strategy to enhance the alkaline NORR performance. Our platform achieves near-100% NH Faradaic efficiency (pH = 14) with a current density of 2 A cm and enables an over 99% NO-to-NH conversion efficiency. We also convert NO to high-purity NHCl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d-band center of Pd atoms to construct local H-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO-to-NH conversion.
硝酸盐（NO）污染对水质和全球氮循环构成重大威胁。碱性电催化NO还原反应（NORR）作为一种有吸引力的途径，可实现NO去除和可持续氨（NH₃）合成。然而，在高pH条件下，它存在质子（H⁺）供应不足的问题，限制了NO转化为NH₃的活性。在此，我们提出一种卤素介导的H⁺供给策略来提高碱性NORR性能。我们的平台在电流密度为2 A cm⁻²时实现了近100%的NH₃法拉第效率（pH = 14），并实现了超过99%的NO转化为NH₃的效率。我们还以接近单位效率将NO转化为高纯度NH₄Cl，这表明了一种将污染物转化为有价值氨产品的实用方法。理论模拟和原位实验表明，Cl配位使Pd原子的d带中心发生移动，通过激发悬空的O - H水解离和快速的H脱附，构建局部富H环境，用于NO中间体加氢，最终实现有效的NO到NH₃转化。
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