通过光诱导加速氧气迁移率实现甲烷的高效干法重整。

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Journal of Colloid and Interface Science Pub Date : 2024-07-25 DOI:10.1016/j.jcis.2024.07.194
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引用次数: 0

摘要

甲烷干重整(DRM)可以消耗温室气体(CH4 和 CO2)来生产有价值的费托合成气(CO 和 H2)。然而,传统的热驱动 DRM 需要消耗大量能源,并面临催化剂烧结和碳沉积等问题,导致催化活性不足。本研究设计了一种高效的光热协同 TiO2/CeO2/Ru 催化剂。在光照条件下,H2 和 CO 的产率分别达到 496.3 mmol g-1 h-1 和 522.4 mmol g-1 h-1。此外,经过 100 小时的循环稳定性测试,该催化剂表现出卓越的稳定性。原位 X 射线光电子能谱(IS-XPS)和密度泛函理论(DFT)计算表明,TiO2/CeO2/Ru 形成的异质结界面有利于捕获光生电子并抑制光子和空穴的重组率,从而提高光催化性能。此外,光诱导的金属-金属电荷转移(MMCT)加速了氧迁移,不仅提高了催化活性,还抑制了催化剂表面碳沉积的形成,从而提高了循环稳定性。这项研究探索了光热协同 DRM 的机理,为高效利用太阳能提供了一条新途径。
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Efficient dry reforming of methane realized by photoinduced acceleration of oxygen migration rate

Methane dry reforming (DRM) can consume greenhouse gases (CH4 and CO2) to produce valuable Fischer-Tropsch syngas (CO and H2). However, conventional thermally driven DRM consume large amounts of energy and face problems such as catalyst sintering and carbon deposition leading to insufficient catalytic activity. In this study, a photothermal synergistic TiO2/CeO2/Ru catalyst with high efficiency was designed. Under the light condition, the yields of H2 and CO reached 496.3 mmol g−1 h−1 and 522.4 mmol g−1 h−1, respectively. In addition, the catalyst demonstrated excellent stability after 100 h cyclic stability test. In-situ X-ray photoelectron spectroscopy (IS-XPS) and density functional theory (DFT) calculations revealed that the heterojunction interface formed by TiO2/CeO2/Ru is favourable for capturing photogenerated electrons and suppressing the recombination rate of photons and holes, thus improving the photocatalytic performance. Furthermore, light-induced metal-to-metal charge transfer (MMCT) accelerated oxygen migration, which not only improved the catalytic activity, but also suppressed the formation of carbon deposits on the catalyst surface, thereby enhancing the cycling stability. This study explores the mechanism of photothermally synergistic DRM, which provides a new pathway for the efficient use of solar energy.

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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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