Accurate location of Ni and W active sites in hierarchical zeolite catalyst for the conversion of cellulose to alcohols

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-02-05 Epub Date: 2024-11-29 DOI:10.1016/j.apcata.2024.120052
Wanying Liang , Guangyue Xu , Yao Fu
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Abstract

The process of converting cellulose into short-chain alcohols is a critical component of biomass valorization. In this study, we utilized an anion-cation co-directed hydrothermal method and wet impregnation to synthesize a hierarchical MFI zeolite with isolated Ni and W sites. We employed linear correlation analysis to evaluate the influence of pore size, site accessibility, and acidity on product selectivity. Balancing hydrogenation and acidic sites on the catalyst enhanced retro-aldol condensation and hydrogenation during cellulose conversion. Surface acidic sites accelerated glucose retro-aldol condensation, while micropore acidic sites aided in ethylene glycol hydrogenolysis. The close proximity of Ni and W facilitated high selectivity and yield of ethanol through bimetallic synergy. This research presented a novel strategy for preparing hierarchical zeolites with isolated metal sites and provides clarity on the cooperative roles of active sites in Ni-W bimetallic catalysts for cellulose conversion.
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纤维素制醇分级沸石催化剂中Ni和W活性位点的精确定位
纤维素转化成短链醇的过程是生物质增值的关键组成部分。在这项研究中,我们利用阴离子-阳离子共定向水热法和湿浸渍法合成了一种具有分离Ni和W位点的多层MFI沸石。我们采用线性相关分析来评价孔径、位点可及性和酸度对产物选择性的影响。平衡催化剂上的加氢和酸性位点增强了纤维素转化过程中的反醛醇缩合和加氢。表面酸性位点加速葡萄糖反醛醇缩合,而微孔酸性位点有助于乙二醇氢解。镍和钨的紧密结合使乙醇通过双金属协同作用具有较高的选择性和产率。本研究提出了一种制备具有隔离金属位点的分级沸石的新策略,并为纤维素转化Ni-W双金属催化剂中活性位点的协同作用提供了清晰的思路。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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