{"title":"在多功能Ni@C/WOx上协同催化纤维素高效氢解制乙二醇","authors":"Mingqiang Chen, Zhiwei Yang, Haosheng Xin*, Yishuang Wang, Defang Liang and Chang Li, ","doi":"10.1021/acssuschemeng.5c06871","DOIUrl":null,"url":null,"abstract":"<p >As a major constituent of renewable biomass, conversion of cellulose to high-value chemicals presents a promising strategy. Herein, we designed a multifunctional Ni@C/WO<sub><i>x</i></sub> catalyst for direct cellulose conversion to ethylene glycol. This catalyst exhibited excellent stability while achieving a high ethylene glycol yield (69.4%). Graphene-encapsulated metal Ni stabilized hydrogenation activity and minimized metal leaching. The interaction between Ni@C and WO<sub><i>x</i></sub> facilitated the reduction of WO<sub><i>x</i></sub> and increased the formation of W<sup>5+</sup> species. Characterization by electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), NH<sub>3</sub>-TPD, and Py-IR confirmed that W<sup>5+</sup> formation induces oxygen vacancies and acid sites on the catalyst support surface. At 30% Ni loading, strong metal–support interactions maximized the W<sup>5+</sup> concentration and oxygen vacancy, enhancing the C–C bond cleavage efficiency. Consequently, the synergistic effect between Ni@C and WO<sub><i>x</i></sub> effectively facilitates key steps in cellulose conversion to ethylene glycol: cellulose hydrolysis, glucose retro-aldol condensation, and glycolaldehyde hydrogenation. The understanding of these structure–performance relationships has provided new ideas for the green and sustainable production of high-value-added chemicals from cellulose.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 36","pages":"15201–15213"},"PeriodicalIF":7.3000,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic Catalysis for Efficient Hydrogenolysis of Cellulose to Ethylene Glycol over Multifunctional Ni@C/WOx\",\"authors\":\"Mingqiang Chen, Zhiwei Yang, Haosheng Xin*, Yishuang Wang, Defang Liang and Chang Li, \",\"doi\":\"10.1021/acssuschemeng.5c06871\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >As a major constituent of renewable biomass, conversion of cellulose to high-value chemicals presents a promising strategy. Herein, we designed a multifunctional Ni@C/WO<sub><i>x</i></sub> catalyst for direct cellulose conversion to ethylene glycol. This catalyst exhibited excellent stability while achieving a high ethylene glycol yield (69.4%). Graphene-encapsulated metal Ni stabilized hydrogenation activity and minimized metal leaching. The interaction between Ni@C and WO<sub><i>x</i></sub> facilitated the reduction of WO<sub><i>x</i></sub> and increased the formation of W<sup>5+</sup> species. Characterization by electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), NH<sub>3</sub>-TPD, and Py-IR confirmed that W<sup>5+</sup> formation induces oxygen vacancies and acid sites on the catalyst support surface. At 30% Ni loading, strong metal–support interactions maximized the W<sup>5+</sup> concentration and oxygen vacancy, enhancing the C–C bond cleavage efficiency. Consequently, the synergistic effect between Ni@C and WO<sub><i>x</i></sub> effectively facilitates key steps in cellulose conversion to ethylene glycol: cellulose hydrolysis, glucose retro-aldol condensation, and glycolaldehyde hydrogenation. The understanding of these structure–performance relationships has provided new ideas for the green and sustainable production of high-value-added chemicals from cellulose.</p>\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":\"13 36\",\"pages\":\"15201–15213\"},\"PeriodicalIF\":7.3000,\"publicationDate\":\"2025-09-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acssuschemeng.5c06871\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acssuschemeng.5c06871","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Synergistic Catalysis for Efficient Hydrogenolysis of Cellulose to Ethylene Glycol over Multifunctional Ni@C/WOx
As a major constituent of renewable biomass, conversion of cellulose to high-value chemicals presents a promising strategy. Herein, we designed a multifunctional Ni@C/WOx catalyst for direct cellulose conversion to ethylene glycol. This catalyst exhibited excellent stability while achieving a high ethylene glycol yield (69.4%). Graphene-encapsulated metal Ni stabilized hydrogenation activity and minimized metal leaching. The interaction between Ni@C and WOx facilitated the reduction of WOx and increased the formation of W5+ species. Characterization by electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), NH3-TPD, and Py-IR confirmed that W5+ formation induces oxygen vacancies and acid sites on the catalyst support surface. At 30% Ni loading, strong metal–support interactions maximized the W5+ concentration and oxygen vacancy, enhancing the C–C bond cleavage efficiency. Consequently, the synergistic effect between Ni@C and WOx effectively facilitates key steps in cellulose conversion to ethylene glycol: cellulose hydrolysis, glucose retro-aldol condensation, and glycolaldehyde hydrogenation. The understanding of these structure–performance relationships has provided new ideas for the green and sustainable production of high-value-added chemicals from cellulose.
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.