{"title":"用单核氧化铌装饰铂/氧化物,提高纤维素直接转化为乙醇的活性和稳定性","authors":"","doi":"10.1039/d4gc03390f","DOIUrl":null,"url":null,"abstract":"<div><div>Chemocatalytic conversion of cellulose to ethanol provides an alternative route for biofuel production with a theoretical carbon yield of 100%; however, it faces significant challenges of high catalyst cost and poor catalyst stability. In this work, we report a new strategy to decrease the use of expensive noble metals, by decorating mononuclear NbO<sub>x</sub> on a low-Pt Pt/WO<sub>x</sub> catalyst surface. The resulting 0.1Nb/0.5Pt/WO<sub>x</sub> catalyst gave rise to an ethanol yield of 33.7% together with an ethylene glycol yield of 21.8%, and the noble metal efficiency reached 25.90 g<sub>ethanol</sub> g<sub>Pt</sub><sup>−1</sup> h<sup>−1</sup>, an increase by a factor of 2–10 compared to those in the literature. Moreover, the catalyst stability was significantly enhanced by the decoration of mononuclear NbO<sub>x</sub>, allowing for recycling at least 7 times without obvious activity decay. Characterization revealed that Pt was highly dispersed at subnanometer and single atom scales, and modification with mononuclear NbO<sub>x</sub> facilitated hydrogen spillover and created more oxygen vacancies on the WO<sub>x</sub> surface upon hydrogen reduction, thus generating a higher density of Brønsted acid sites. This effect not only favored cellulose conversion to ethylene glycol but also promoted the hydrogenolysis of ethylene glycol to ethanol.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3000,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc03390f?page=search","citationCount":"0","resultStr":"{\"title\":\"Improving both activity and stability for direct conversion of cellulose to ethanol by decorating Pt/WOx with mononuclear NbOx†\",\"authors\":\"\",\"doi\":\"10.1039/d4gc03390f\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Chemocatalytic conversion of cellulose to ethanol provides an alternative route for biofuel production with a theoretical carbon yield of 100%; however, it faces significant challenges of high catalyst cost and poor catalyst stability. In this work, we report a new strategy to decrease the use of expensive noble metals, by decorating mononuclear NbO<sub>x</sub> on a low-Pt Pt/WO<sub>x</sub> catalyst surface. The resulting 0.1Nb/0.5Pt/WO<sub>x</sub> catalyst gave rise to an ethanol yield of 33.7% together with an ethylene glycol yield of 21.8%, and the noble metal efficiency reached 25.90 g<sub>ethanol</sub> g<sub>Pt</sub><sup>−1</sup> h<sup>−1</sup>, an increase by a factor of 2–10 compared to those in the literature. Moreover, the catalyst stability was significantly enhanced by the decoration of mononuclear NbO<sub>x</sub>, allowing for recycling at least 7 times without obvious activity decay. Characterization revealed that Pt was highly dispersed at subnanometer and single atom scales, and modification with mononuclear NbO<sub>x</sub> facilitated hydrogen spillover and created more oxygen vacancies on the WO<sub>x</sub> surface upon hydrogen reduction, thus generating a higher density of Brønsted acid sites. This effect not only favored cellulose conversion to ethylene glycol but also promoted the hydrogenolysis of ethylene glycol to ethanol.</div></div>\",\"PeriodicalId\":78,\"journal\":{\"name\":\"Green Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.3000,\"publicationDate\":\"2024-09-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc03390f?page=search\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/org/science/article/pii/S1463926224007581\",\"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":"Green Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S1463926224007581","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Improving both activity and stability for direct conversion of cellulose to ethanol by decorating Pt/WOx with mononuclear NbOx†
Chemocatalytic conversion of cellulose to ethanol provides an alternative route for biofuel production with a theoretical carbon yield of 100%; however, it faces significant challenges of high catalyst cost and poor catalyst stability. In this work, we report a new strategy to decrease the use of expensive noble metals, by decorating mononuclear NbOx on a low-Pt Pt/WOx catalyst surface. The resulting 0.1Nb/0.5Pt/WOx catalyst gave rise to an ethanol yield of 33.7% together with an ethylene glycol yield of 21.8%, and the noble metal efficiency reached 25.90 gethanol gPt−1 h−1, an increase by a factor of 2–10 compared to those in the literature. Moreover, the catalyst stability was significantly enhanced by the decoration of mononuclear NbOx, allowing for recycling at least 7 times without obvious activity decay. Characterization revealed that Pt was highly dispersed at subnanometer and single atom scales, and modification with mononuclear NbOx facilitated hydrogen spillover and created more oxygen vacancies on the WOx surface upon hydrogen reduction, thus generating a higher density of Brønsted acid sites. This effect not only favored cellulose conversion to ethylene glycol but also promoted the hydrogenolysis of ethylene glycol to ethanol.
期刊介绍:
Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.