Crystal defects Boost cellulose conversion to C2 alcohols over Pd/WO3 catalysts

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Catalysis Pub Date : 2024-11-26 DOI:10.1016/j.jcat.2024.115860

Wei Jia, Wengang Liu, Yuandong Cui, Hang Song, Chengfeng Zhou, Wei Jiang, Haoxi Ben, Xiaoli Yang, De Chen

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Abstract

Converting cellulose into C₂ alcohols presents a sustainable alternative to fossil fuels, contributing to the development of eco-friendly and economically viable biofuels and chemicals. Tungsten oxide (WO₃) is a key solid acid catalyst for this process, yet limited research explores its diverse morphologies and unique catalytic effects. This study investigates diverse WO₃ morphologies (nanosheets, nanoflowers, nanoblocks, and tetrahedral octahedra) in combination with Pd for converting cellulose to C₂ alcohols. Optimized conditions with Pd/o-WO₃ catalyst resulted in the highest C₂ alcohols (ethylene glycol and ethanol, 80.9 %), notably yielding 64.8 % ethylene glycol. Extensive characterizations and DFT calculations reveal the smaller element occupancy rates and a longer W-O bond length led to a large number of crystal defects over Pd/o-WO₃. It facilitated the formation of W⁵⁺–OH sites and Pd-O(H)-W interactions, further synergistically enhancing hydrogenation ability and acidity. Designed experiments to elucidate cellulose conversion pathways, including hydrolysis, retro-aldol condensation, and hydrogenation. This study emphasizes the unique impact of WO₃ morphologies and underscores the importance of supporting crystal defects for catalytic performance in eco-friendly biofuel and chemical production.

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晶体缺陷促进纤维素在 Pd/WO3 催化剂上转化为 C2 醇

将纤维素转化为 C2 醇是化石燃料的可持续替代品，有助于开发生态友好、经济可行的生物燃料和化学品。氧化钨（WO3）是这一工艺的关键固体酸催化剂，但对其不同形态和独特催化效果的研究却很有限。本研究调查了 WO3 的不同形态（纳米片、纳米花、纳米块和四面体八面体）与钯的结合，用于将纤维素转化为 C2 醇。在 Pd/o-WO3 催化剂的优化条件下，C2 醇（乙二醇和乙醇，80.9%）的产量最高，尤其是乙二醇的产量高达 64.8%。广泛的表征和 DFT 计算显示，较小的元素占有率和较长的 W-O 键长度导致 Pd/o-WO3 上出现大量晶体缺陷。这促进了 W5+-OH 位点和 Pd-O(H)-W 相互作用的形成，进一步协同增强了氢化能力和酸性。设计实验以阐明纤维素的转化途径，包括水解、逆醛缩合和氢化。这项研究强调了 WO3 形态的独特影响，并强调了支持性晶体缺陷对环保型生物燃料和化学品生产催化性能的重要性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.