Room-Temperature Catalyst-Free Ammonia Decomposition for Hydrogen Production on Water Microdroplets

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Kejian Li, Bingxing Zhang, Deming Xia, Zhengwei Ye, Yuyang Pan, Joseph S. Francisco, Zetian Mi
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引用次数: 0

Abstract

Ammonia has been considered a viable carbon-free hydrogen carrier, yet its decomposition to hydrogen mainly relies on noble-metal-based catalysts and high temperatures. Here, through leveraging extraordinary physicochemical properties at the gas–liquid interface of water microdroplets, we present a catalyst-free and scalable approach for hydrogen production from ammonia under ambient conditions. A maximum hydrogen evolution rate of 226.8 μmol/h was observed, which outperformed most conventional catalytic methods at room temperature. Comprehensive experimental investigations and theoretical calculations revealed the underlying ammonia splitting mechanisms: hydroxyl radical and hydrogen radical, generated at the gas–liquid interface of microdroplets, synergistically triggered the interfacial ammonia decomposition following a thermodynamically favorable redox pathway, and the reaction rates can be enhanced by the high electric fields and reactants concentration accumulation at the gas–liquid interface. This work provides a new paradigm for green hydrogen production, advancing microdroplet chemistry and a sustainable hydrogen society.
微水滴室温无催化剂氨分解制氢研究
氨一直被认为是一种可行的无碳氢载体,但其分解为氢主要依赖于贵金属催化剂和高温。在这里,通过利用水微滴气液界面非凡的物理化学性质,我们提出了一种在环境条件下由氨制氢的无催化剂和可扩展的方法。在室温下,最大析氢速率为226.8 μmol/h,优于大多数传统的催化方法。综合实验研究和理论计算揭示了氨分裂的潜在机制:微滴气液界面产生的羟基自由基和氢自由基协同引发界面氨分解,遵循热力学有利的氧化还原途径,高电场和反应物浓度在气液界面积聚可提高反应速率。这项工作为绿色制氢、推进微滴化学和可持续氢社会提供了新的范例。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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