Light-driven propane dehydrogenation by a single-atom catalyst under near-ambient conditions

IF 20.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nature chemistry Pub Date : 2025-03-21 DOI:10.1038/s41557-025-01766-3
Leilei Kang, Beien Zhu, Qingqing Gu, Xinyi Duan, Lei Ying, Guodong Qi, Jun Xu, Lin Li, Yang Su, Yanan Xing, Yanlong Wang, Gang Li, Rengui Li, Yi Gao, Bing Yang, Xiao Yan Liu, Aiqin Wang, Tao Zhang
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Abstract

Propane dehydrogenation is an energy-intensive industrial reaction that requires high temperatures (550–750 °C) to overcome thermodynamic barriers. Here we overcome these limits and demonstrate that near-ambient propane dehydrogenation can be achieved through photo-thermo-catalysis in a water-vapour environment. We reduce the reaction temperature to 50–80 °C using a single-atom catalyst of copper supported on TiO2 and a continuous-flow fixed-bed reactor. The mechanism differs from conventional propane dehydrogenation in that hydrogen is produced from the photocatalytic splitting of water vapour, surface-bound hydroxyl radicals extract propane hydrogen atoms to form propylene without over-oxidation, and water serves as a catalyst. This route also works for the dehydrogenation of other small alkanes. Moreover, we demonstrate sunlight-driven water-catalysed propane dehydrogenation operating at reaction temperatures as low as 10 °C. We anticipate that this work will be a starting point for integrating solar energy usage into a wide range of high-temperature industrial reactions. Propane dehydrogenation is challenging to perform under mild conditions due to the reaction’s endothermic nature. Now, near-ambient propane dehydrogenation has been shown using copper single-atom catalysts supported on titanium oxide under light illumination and a water vapour environment.

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近环境条件下单原子催化剂驱动丙烷脱氢
丙烷脱氢是一种能源密集型工业反应,需要高温(550-750°C)来克服热力学障碍。在这里,我们克服了这些限制,并证明了近环境丙烷脱氢可以通过光热催化在水蒸气环境中实现。我们使用负载在TiO2上的单原子铜催化剂和连续流固定床反应器将反应温度降低到50-80℃。其机理与传统丙烷脱氢的不同之处在于,氢气是由水蒸气的光催化分裂产生的,表面结合的羟基自由基提取丙烷氢原子形成丙烯而不过度氧化,水作为催化剂。这条路线也适用于其他小烷烃的脱氢反应。此外,我们展示了在低至10°C的反应温度下,由阳光驱动的水催化丙烷脱氢操作。我们预计这项工作将成为将太阳能利用纳入广泛的高温工业反应的起点。
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来源期刊
Nature chemistry
Nature chemistry 化学-化学综合
CiteScore
29.60
自引率
1.40%
发文量
226
审稿时长
1.7 months
期刊介绍: Nature Chemistry is a monthly journal that publishes groundbreaking and significant research in all areas of chemistry. It covers traditional subjects such as analytical, inorganic, organic, and physical chemistry, as well as a wide range of other topics including catalysis, computational and theoretical chemistry, and environmental chemistry. The journal also features interdisciplinary research at the interface of chemistry with biology, materials science, nanotechnology, and physics. Manuscripts detailing such multidisciplinary work are encouraged, as long as the central theme pertains to chemistry. Aside from primary research, Nature Chemistry publishes review articles, news and views, research highlights from other journals, commentaries, book reviews, correspondence, and analysis of the broader chemical landscape. It also addresses crucial issues related to education, funding, policy, intellectual property, and the societal impact of chemistry. Nature Chemistry is dedicated to ensuring the highest standards of original research through a fair and rigorous review process. It offers authors maximum visibility for their papers, access to a broad readership, exceptional copy editing and production standards, rapid publication, and independence from academic societies and other vested interests. Overall, Nature Chemistry aims to be the authoritative voice of the global chemical community.
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