Boosting Furfural Hydrogenation Performance of Confined Co-Based Composites Derived From ZIF-67 via a Surfactant-Assisted Pyrolysis Strategy

IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL ChemCatChem Pub Date : 2024-11-21 DOI:10.1002/cctc.202401651
Mengbo Huai, Xiaomeng Li, Ying Zhang, Xiaomei Qin, Yifei Zhang, Xiaoyun Qin, Yingfan Liu, Xinxin Liang, Prof. Gao Li, Jianbo Zhao
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Abstract

Developing chromium-free and non-noble metal catalysts with high performance for furfural hydrogenation to high-value product furfural alcohol is desirable but challenging. Herein we develop and prepare nitrogen-doping carbon confining cobalt-based catalysts (Co-N-C composites) by a simple pyrolysis process of well-defined ZIF-67 MOFs modified with different surfactants (i.e., polyethylene-polypropylene glycol (F127), polyvinyl pyrrolidone (PVP), cetyltrimethylammonium bromide (CTAB) in this work). The in situ formed carbon shell from F127 surfactants inhibits Co agglomeration during pyrolysis of ZIF-67 at 800 °C, thus affording abundant active CoNx species and metallic Co clusters, which is confirmed by high-resolution transmission electron microscopy (HR-TEM) and X-ray photoelectron spectroscopy (XPS). The rich mesopore structures in [email protected] benefit mass transfer of reactants. [email protected] catalyst exhibits superior catalytic performance of a 97.2% furfural conversion with a 92.5% selectivity toward furfural alcohol and good durability during the chemoselective furfural hydrogenation, which is mainly attributed to the unique confinement of the in situ generated carbon shell. The surfactant-assisted pyrolysis strategy provides an efficient and facile way to prepare efficient non-noble metal catalysts to replace chromium-based catalysts for furfural hydrogenation to furfuryl alcohol in the future.

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通过表面活性剂辅助热解策略提高由 ZIF-67 制成的封闭共基复合材料的糠醛加氢性能
开发无铬、非贵金属、高性能的糠醛加氢制备高值产品糠醛醇催化剂是一种迫切需要但又具有挑战性的技术。本文采用简单的热解工艺,将定义明确的ZIF-67 MOFs用不同的表面活性剂(即聚乙烯-聚丙烯乙二醇(F127)、聚乙烯吡咯烷酮(PVP)、十六烷基三甲基溴化铵(CTAB))改性,开发并制备了氮掺杂碳约束钴基催化剂(Co-N-C复合材料)。高分辨率透射电镜(HR-TEM)和x射线光电子能谱(XPS)证实,F127表面活性剂原位形成的碳壳抑制了ZIF-67在800℃热解过程中的Co团聚,从而提供了丰富的活性CoNx物质和金属Co团簇。[email protected]中丰富的介孔结构有利于反应物的传质。[email protected]催化剂在糠醛化学选择性加氢过程中表现出优异的催化性能,糠醛转化率为97.2%,对糠醛醇的选择性为92.5%,并且具有良好的耐久性,这主要归功于原位生成的碳壳的独特限制。表面活性剂辅助热解策略为制备高效非贵金属催化剂替代铬基催化剂催化糠醛加氢制糠醇提供了一条高效、便捷的途径。
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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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