微水滴室温无催化剂氨分解制氢研究

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

摘要

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。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Room-Temperature Catalyst-Free Ammonia Decomposition for Hydrogen Production on Water Microdroplets
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.
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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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