Efficient Photocatalytic Propane Direct Dehydrogenation to Propylene Over PtO2 Clusters

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Advanced Materials Pub Date : 2025-01-19 DOI:10.1002/adma.202411648
Chi Duan, Jinjia Liu, Zhenhua Li, Run Shi, Jiaqi Zhao, Geoffrey I. N. Waterhouse, Xiao-Dong Wen, Li-Ping Zhang, Li-Zhu Wu, Tierui Zhang
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Abstract

The direct dehydrogenation of alkanes to olefins under mild conditions is challenging due to the inert nature of alkyl C─H bonds. Herein, an efficient photocatalytic system is developed for propane direct dehydrogenation (PDH) to propylene, consisting of ≈1.30 nm sized PtO2 clusters immobilized on a layered double hydroxide -derived ZnO/Al2O3 support (LD-Ptn). Under UV excitation (365 nm), photogenerated holes in ZnO migrate to Pt sites at PtO2/ZnO interfaces, thereby activating and dissociating C─H bonds in propane. A propylene production rate of almost 1 mmol g−1 h−1 and a nearly 100% selectivity are achieved for the compositionally optimized LD-Ptn photocatalyst. Control experiments and density functional theory calculations further verify that the excellent photocatalytic PDH performance of LD-Ptn stems from synergism between ZnO semiconductor and the loaded Pt species. This work identifies a promising new route for direct production of olefins from alkanes.

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光催化丙烷在PtO2簇上直接脱氢制丙烯
由于烷基C─H键的惰性性质,在温和条件下将烷烃直接脱氢为烯烃是具有挑战性的。本文开发了一种丙烷直接脱氢制丙烯的高效光催化体系,该体系由约1.30 nm大小的PtO2团簇固定在层状双氢氧化物衍生的ZnO/Al2O3载体(LD‐Ptn)上组成。在紫外激发(365 nm)下,ZnO中的光生空穴迁移到PtO2/ZnO界面上的Pt位点,从而激活和解离丙烷中的C─H键。优化后的LD - Ptn光催化剂丙烯的产率接近1 mmol g−1 h−1,选择性接近100%。控制实验和密度泛函理论计算进一步验证了LD - Ptn优异的光催化PDH性能源于ZnO半导体与负载Pt物质之间的协同作用。这项工作确定了一条有前途的由烷烃直接生产烯烃的新路线。
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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