Plasma-Driven Dual-Membrane System for Intensified Hydrogen Production with Integrated Ammonia Recovery

作者：Shengyan Meng, Yuxin Chen, Zhaolun Cui, Yang Gu, Hongyan Xiao, Yi Liu, Yi Liu, Shijie Yang, Junze Li, Kunpeng Yu, Chen Wang, Wenjing Hu, Hongbo Xie, Xiaoxia Gao, Wei Shao, Gaohong He, Jun Cai, Zhi Liu, Hui Li, Yanhui Yi, Yi Liu, Yi Liu · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c15789 · 被引用次数：2 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Catalysts for Methane Reforming、Hydrogen Storage and Materials

Ammonia (NH 3 ) is a principal carbon-free hydrogen (H 2 ) carrier, yet its decomposition via conventional thermocatalysis is restricted by kinetically demanding high temperatures. Integrating the reaction with in situ product removal to achieve high decomposition efficiency under mild conditions presents a formidable challenge. Here, we report a plasma-enhanced dual-membrane ammonia decomposition system (PEDMADS) that synergistically couples dielectric barrier discharge (DBD), a highly dispersed atomic layer deposition (ALD)-synthesized Ru/SiO 2 catalyst, and an integrated ultrathin Pd membrane (1.8 μm) to enable a high H 2 space-time yield of 1567 mmol g –1 h –1 at 400 °C. Furthermore, a downstream cascade of high-performance Silicalite-1 (S-1) membranes achieved energy-efficient NH 3 recovery, exhibiting unprecedented NH 3 /H 2 and NH 3 /N 2 separation factors of 686 and 7076 under ambient conditions. Molecular dynamics simulations revealed this selectivity arose from a preferential adsorption-driven molecular sieving mechanism. The five-stage cascade reduced the effluent NH 3 concentration from 24.1% to below 4%, achieving 87% removal efficiency. Techno-economic analysis indicated a levelized cost of 0.92 $/kg H 2 with a 95.9% carbon footprint reduction compared to the conventional thermal process, thus offering a compelling blueprint for a sustainable ammonia–hydrogen economy.