Tailoring selectivity in furfural hydrogenolysis over NiCoAl catalyst through a simple rinsing process

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-11-15 DOI:10.1016/j.jcat.2024.115845

Zepeng Zhao, Wenguang Zhou, Guozhang Chang, Lungang Chen, Chenguang Wang, Yuhe Liao, Jinxing Long, Longlong Ma, Yong Liu

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Abstract

In this study, the structure–activity relationships were investigated in converting biomass-derived furfural into cyclopentanone (CPO) or tetrahydrofuran alcohol (THFA) using a rinsing method to modulate the NiCoAl catalyst. Characterization of two catalysts, NiCoAl (without rinsing) and NiCoAl-R (with rinsing), reveals differences in morphology, composition, and acidity. Rinsing induced a transition from agglomerate to layered structure in NiCoAl-R, which exhibited higher acid strength and improved Lewis to Brønsted acid ratio. NiCoAl-R contained a high percentage of metal oxides, while NiCoAl had a high percentage of metallic species on its surface. These distinctions resulted in varied performance in FFA hydrogenolysis, with NiCoAl-R favoring CPO formation and NiCoAl facilitating THFA production. In situ DRIFTS experiments reveals differing furfural sorption states, and DFT calculations highlighted the higher activity of metal oxides in ring-opening reactions. This investigation elucidates the intricate relationship between catalyst properties and performance, offering insights for tailored catalyst design in biomass conversion.

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通过简单的漂洗工艺调整镍钴铝催化剂在糠醛氢解过程中的选择性

本研究采用漂洗法调节镍钴铝催化剂，研究了将生物质衍生的糠醛转化为环戊酮（CPO）或四氢呋喃醇（THFA）的结构-活性关系。对镍钴铝（未漂洗）和镍钴铝-R（漂洗）两种催化剂的表征显示出了形态、组成和酸度方面的差异。漂洗促使镍钴铝-R 从团聚结构转变为层状结构，表现出更高的酸性强度，并改善了路易斯酸与布氏酸的比率。镍钴铝-R含有较高比例的金属氧化物，而镍钴铝表面则有较高比例的金属物种。这些区别导致了在氢解反式脂肪酸方面的不同性能，NiCoAl-R 有利于 CPO 的形成，而 NiCoAl 则有利于 THFA 的生成。原位 DRIFTS 实验揭示了不同的糠醛吸附状态，而 DFT 计算则强调了金属氧化物在开环反应中更高的活性。这项研究阐明了催化剂特性与性能之间错综复杂的关系，为生物质转化过程中催化剂的定制设计提供了启示。

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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.