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Enhanced photothermal dehydration of methanol over W18O49/Au/SAPO-34 catalysts with broadened light absorption

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Abstract

Methanol-to-olefins (MTO) process is one of the most critical pathways to produce low carbon olefins. Typically, the reaction is driven by thermal catalysis, which inevitably needs to consume large amounts of fossil fuel. Developing a new technique to substitute for the fuel burning is urgent for MTO process to improve the industry prospects and sustainability. Herein, we report a novel W18O49/Au/SAPO-34 (W/Au/S), a multifunctional photothermal catalyst for the MTO reaction. A high methanol conversion was achieved under xenonum (Xe) lamp irradiation, yielding methyl ether (ME) and ethylene as the main products. The optimized W/Au/S catalysts showed ethylene yield as high as 250 μmol in 60 min, which was 2.5 times higher than that of Au/SAPO-34. The physiochemical characterization revealed that the SAPO-34 molecular sieves were surrounded by Au and W18O49 nanoparticles, which exhibited a strong localized surface plasmon resonance excitation around 540 nm and light absorption beyond 500 nm. The multifunctional catalysts showed a strong photothermal effect, arising from the broadened light absorption of Au and W18O49 nanoparticles, leading to a temperature as high as 250 °C on the surface of the catalysts. Mechanism study showed that the superior ethylene selectivity of W/Au/S catalysts was attributed to the moderating acidic sites of W18O49 for methanol dehydration to ethylene. This research may provide new insight for designing heterostructures to improve photo-to-chemical conversion performance and is expected to accelerate progress toward the excellent multifunctional photothermal catalysts with broad light absorption for methanol activation and C–C bond formation.

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摘要

甲醇制烯烃(MTO)工艺是生产低碳烯烃的关键技术之一。通常，该反应由热催化驱动，需要消耗大量化石燃料。因此，迫切需要开发一种替代化石燃料的MTO工艺新技术以改善行业前景和可持续性。本文制备了一种用于MTO反应的多功能光热催化剂W18O49/Au/SAPO-34 (W/Au/S)。在氙灯照射下，甲醇转化率较高，其主要产物为甲醚和乙烯。优化后的W/Au/S催化剂在60 min内的乙烯产率高达250 μmol，是Au/SAPO-34催化剂的2.5倍。对催化剂的物理化学性能表征表明，SAPO-34分子筛被Au和W18O49纳米粒子包裹，复合催化剂在540 nm附近表现出强烈的局部表面等离子体共振(LSPR)激发，同时光吸收区域扩展到红外光区。由于Au和W18O49纳米粒子的光吸收变宽，导致光照下催化剂表面温度高达250℃，催化剂表现出强烈的光热效应。机理研究表明，W/Au/S催化剂具有较好的乙烯选择性是由于W18O49表面合适的酸性位点对甲醇脱水制乙烯起到了催化作用。该研究可为设计异质结构以提高光化学转化性能提供新的思路，并有望加速开发用于甲醇活化和C–C键耦合的具有广泛光吸收的高性能光热催化剂。

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Acknowledgements

This work was financially supported by the High-level Innovative Talent Cultivation Project of Guizhou Province (No. GZSQCC2019003), the Natural Science Research Project of Guizhou Provincial Department of Education (No. QJHKY Zi[2021]257) and the Academic New Seedling Cultivation and Innovation Exploration Project of Guizhou Institute of Technology (No. GZLGXM-08).

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  1. Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming, 650093, China

    Ya-Qin Tang, Shao-Yuan Li, Kui-Xian Wei, Tao Qu, Wen-Hui Ma, Yong-Nian Dai, Kong-Zhai Li & Yi-Ke Liu

  2. School of Materials and Energy Engineering, Guizhou Institute of Technology, Guiyang, 550003, China

    Ya-Qin Tang, Meng-Xia Yan, Chang-Qian Lu, Da-Jun Luo, Xue-Liang Zhang & Yi-Ke Liu

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Tang, YQ., Yan, MX., Lu, CQ. et al. Enhanced photothermal dehydration of methanol over W18O49/Au/SAPO-34 catalysts with broadened light absorption. Rare Met. 43, 1139–1152 (2024). https://doi.org/10.1007/s12598-023-02511-w

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