氢在Pt/WO3上的溢出促进了氢同位素的低温催化交换

IF 8.3 2区 工程技术 Q1 CHEMISTRY, PHYSICAL
Weiyi Liu , Chenxiao Liu , Jia Ren , Yongsheng Xu , Guilin Liu , Feng Xin
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引用次数: 0

摘要

氢同位素的催化交换是消除核废水中重氢同位素的关键。然而,高铂(Pt)负载和不满意的低温本征活性阻碍了催化剂的商业可行性。在此,我们开发了一种负载Pt (Pt/WO3)的氧化钨催化剂,通过氢溢出充分利用Pt活性位点上的活化氢(H)原子。在接近室温的条件下,所制备的催化剂的周转频率达到了前所未有的水平。结合前位和原位表征,我们证明了Pt和WO3之间的氢溢出通过自发地将活化的H原子迁移到WO3,形成羟基并释放Pt位点来促进反应。这些羟基直接参与交换反应,间接调节Pt位点的电子结构,显著促进了低Pt负载下的催化活性。本研究为氢同位素低温催化交换提供了一种新的载体辅助反应机制。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Hydrogen spillover on Pt/WO3 promoted low-temperature catalytic exchange of hydrogen isotopes

Hydrogen spillover on Pt/WO3 promoted low-temperature catalytic exchange of hydrogen isotopes
The catalytic exchange of hydrogen isotopes is crucial for eliminating heavy hydrogen isotopes in nuclear wastewater. However, high platinum (Pt) loading and unsatisfied intrinsic activity at low temperatures hinder the commercial viability of catalysts. Herein, we develop a tungsten oxide loading Pt (Pt/WO3) catalyst to sufficiently utilize activated hydrogen (H) atoms over Pt active sites through hydrogen spillover. The turnover frequency of the as-prepared catalyst reaches an unprecedented level at near room temperature. Combining ex- and in-situ characterizations, we demonstrate that hydrogen spillover between Pt and WO3 promotes the reaction by spontaneously migrating activated H atoms to WO3, forming hydroxyl groups, and releasing Pt sites. These hydroxyl groups directly participate in the exchange reaction and indirectly regulate the electronic structure of Pt sites, significantly facilitating catalytic activity at low Pt loading. This work provides a novel support-assisted reaction mechanism for low-temperature catalytic exchange of hydrogen isotopes.
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来源期刊
International Journal of Hydrogen Energy
International Journal of Hydrogen Energy 工程技术-环境科学
CiteScore
13.50
自引率
25.00%
发文量
3502
审稿时长
60 days
期刊介绍: The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc. The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.
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