具有ZnNx活性位的单原子Zn催化剂有效促进生物质衍生羰基化合物的Meerwein-Ponndorf-Verley还原

IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL
ChemCatChem Pub Date : 2025-08-06 DOI:10.1002/cctc.202500961
Long Tao, Zhaoxi Cai, Chenglei Xiao, Yayun Pang, Jinpeng Liang, Prof. Jinliang Song
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引用次数: 0

摘要

Meerwein-Ponndorf-Verley (MPV)还原是一种很有前途的选择性转化生物质衍生羰基化合物的方法。成本效益和高效的多相催化剂的MPV还原仍然是非常需要的。本研究通过将ZnCl2与聚乙烯醇吡咯烷酮形成的锌基配位聚合物进行热解,制备了n掺杂碳负载的锌基催化材料(表示为Zn@C-T, T为热解温度)。非常有趣的是,在900°C (Zn@C-900)下制备的材料对各种生物质衍生羰基化合物的MPV还原表现出优异的催化活性,生成相应的醇,源自Zn@C-900中形成的ZnNx位点。特别是,在常用的Zr基催化剂中,Zn的用量仅为0.6 mol%,远低于Zr的用量,证实了Zn@C-900在大规模应用中的巨大潜力。系统研究表明,Zn@C-900优异的催化活性主要是由于Zn(作为Lewis酸位)和N(作为Lewis碱位)在ZnNx位点上的协同作用,可以同时激活羰基化合物中的羰基和异丙醇中的羟基,从而显著促进羰基化合物的MPV还原。这项工作为MPV还原生物质衍生羰基化合物提供了一种经济高效的锌基催化剂。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Single-Atom Zn Catalyst with ZnNx Active Sites Efficiently Promoted Meerwein–Ponndorf–Verley Reduction of Biomass-Derived Carbonyl Compounds

Single-Atom Zn Catalyst with ZnNx Active Sites Efficiently Promoted Meerwein–Ponndorf–Verley Reduction of Biomass-Derived Carbonyl Compounds

Meerwein–Ponndorf–Verley (MPV) reduction is a highly promising strategy to selectively convert biomass-derived carbonyl compounds. Cost-effective and efficient heterogeneous catalysts for MPV reduction are still highly desired. In this study, N-doped carbon-supported Zn-based catalytic materials (denoted as Zn@C-T, in which T was the pyrolysis temperature) was fabricated by the pyrolysis of Zn-based coordination polymer formed from ZnCl2 and polyvinyl pyrrolidone. Very interestingly, the material prepared at 900 °C (Zn@C-900) showed excellent catalytic activity on MPV reduction of various biomass-derived carbonyl compounds to generate the corresponding alcohols, originating from the formed ZnNx sites in Zn@C-900. Especially, the usage of Zn was only 0.6 mol%, which was much lower than the usage of Zr in the popular Zr-based catalysts, confirming the great potential of the Zn@C-900 in large-scale applications. Systematic investigations revealed that the excellent catalytic activity of Zn@C-900 was predominantly enabled by the synergistic effect of Zn (as Lewis acid sites) and N (as Lewis base sites) in the ZnNx sites, which could simultaneously activate the carbonyl group in carbonyl compounds and the hydroxyl group in isopropanol, thereby significantly promoting the MPV reduction of carbonyl compounds. This work provided a cost-effective and efficient Zn-based catalyst for MPV reduction of biomass-derived carbonyl compounds.

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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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