Long Tao, Zhaoxi Cai, Chenglei Xiao, Yayun Pang, Jinpeng Liang, Prof. Jinliang Song
{"title":"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","authors":"Long Tao, Zhaoxi Cai, Chenglei Xiao, Yayun Pang, Jinpeng Liang, Prof. Jinliang Song","doi":"10.1002/cctc.202500961","DOIUrl":null,"url":null,"abstract":"<p>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 ZnCl<sub>2</sub> 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 ZnN<sub>x</sub> 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 ZnN<sub>x</sub> 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.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 19","pages":""},"PeriodicalIF":3.9000,"publicationDate":"2025-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Single-Atom Zn Catalyst with ZnNx Active Sites Efficiently Promoted Meerwein–Ponndorf–Verley Reduction of Biomass-Derived Carbonyl Compounds\",\"authors\":\"Long Tao, Zhaoxi Cai, Chenglei Xiao, Yayun Pang, Jinpeng Liang, Prof. Jinliang Song\",\"doi\":\"10.1002/cctc.202500961\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>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 ZnCl<sub>2</sub> 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 ZnN<sub>x</sub> 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 ZnN<sub>x</sub> 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.</p>\",\"PeriodicalId\":141,\"journal\":{\"name\":\"ChemCatChem\",\"volume\":\"17 19\",\"pages\":\"\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-08-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ChemCatChem\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cctc.202500961\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemCatChem","FirstCategoryId":"92","ListUrlMain":"https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cctc.202500961","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
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.
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.