Controlling the Reaction Pathways of Mixed NOxHy Reactants in Plasma-Electrochemical Ammonia Synthesis

作者：Xiaoli Ge, Chengyi Zhang, Mayuresh Janpandit, Shwetha Prakash, Pratahdeep Gogoi, Daoyang Zhang, Timothy R. Cook, Geoffrey I. N. Waterhouse, Longwei Yin, Ziyun Wang, Yuguang Li · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.4c12858 · 被引用次数：32 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Catalytic Processes in Materials Science、Plasma Applications and Diagnostics

Electrochemical activation of dinitrogen (N 2 ) is notoriously challenging, typically yielding very low ammonia (NH 3 ) production rates. In this study, we present a continuous flow plasma-electrochemical reactor system for the direct conversion of nitrogen from air into ammonia. In our system, nitrogen molecules are first converted into a mixture of NO x species in the plasma reactor, which are then fed into an electrochemical reactor. To selectively convert the generated NO x species into NH 3, we employed a graph theory approach combined with first-principles calculations to comprehensively enumerate all possible pathways from N 2 -to-NH 3, pinpointing key intermediates (NH 2 * and NO*). A series of bimetallic catalysts was then designed to target the optimal adsorption and conversion of the limiting intermediate in the NO x -to-NH 3 pathway. Using an optimized CuPd foam catalyst, we demonstrated an ammonia production rate of 81.2 mg h –1 cm –2 with stability over 1000 h at an applied current of 2 A.