{"title":"铝负载铜镍催化剂对糠醛和5-羟甲基糠醛加氢的协同作用研究","authors":"Sanjay Srivastava, G.C. Jadeja, Jigisha Parikh","doi":"10.1016/j.molcata.2016.11.023","DOIUrl":null,"url":null,"abstract":"<div><p>The structure of alumina-supported copper-nickel catalysts prepared by impregnation method was studied by using a combination of various characterization techniques including XRD, N<sub>2</sub>-sorption, TEM, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD, XANES/EXAFS and CHNS methods. A series of characterizations revealed that dispersion of copper increases with an increase in nickel loading on ɣ-Al<sub>2</sub>O<sub>3</sub> due to strong interaction between nickel and copper oxide particles. This also led to the formation of mixed copper-nickel oxides in calcined catalysts at the highest loading of nickel and copper (i.e. Cu/Ni<!--> <!-->=<!--> <!-->1). In catalytic activity, both the monometallic Cu/ɣ-Al<sub>2</sub>O<sub>3</sub> and Ni/ɣ-Al<sub>2</sub>O<sub>3</sub> showed lower activity and selectivity towards hydrogenation of both Furfural and 5-Hydroxymethylfurfural to 2-methylfuran (2-MF) and 2, 5-dimethylfuran (DMF), respectively. However, with increase in nickel loading, the activity and the selectivity of Cu/ɣ-Al<sub>2</sub>O<sub>3</sub> drastically increased for both the cases and Cu-Ni/ɣ-Al<sub>2</sub>O<sub>3</sub> (Cu/Ni<!--> <!-->=<!--> <!-->1) showed the highest catalytic activity. Furthermore, combination of Cu/Ni ratios and temperature plays a significant role in the product distribution, as in the case of furfural hydrogenation, at a lower temperature, furfuryl alcohol (FOL) appears as the main product while at a higher temperature, 2-methylfuran (2-MF) is found to be the dominant product over Cu-Ni/ɣ-Al<sub>2</sub>O<sub>3</sub> (Cu/Ni<!--> <!-->=<!--> <!-->1) catalysts. Similarly, 2,5-bishydroxymethylfuran (BHF) is found to be the major product at a lower temperature and 2,5-dimethylfuran (DMF) is selectively produced at a higher temperature in the HMF hydrogenation. Furthermore, reaction pathways are discussed for both the reactions.</p></div>","PeriodicalId":370,"journal":{"name":"Journal of Molecular Catalysis A: Chemical","volume":"426 ","pages":"Pages 244-256"},"PeriodicalIF":5.0620,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.molcata.2016.11.023","citationCount":"109","resultStr":"{\"title\":\"Synergism studies on alumina-supported copper-nickel catalysts towards furfural and 5-hydroxymethylfurfural hydrogenation\",\"authors\":\"Sanjay Srivastava, G.C. Jadeja, Jigisha Parikh\",\"doi\":\"10.1016/j.molcata.2016.11.023\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The structure of alumina-supported copper-nickel catalysts prepared by impregnation method was studied by using a combination of various characterization techniques including XRD, N<sub>2</sub>-sorption, TEM, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD, XANES/EXAFS and CHNS methods. A series of characterizations revealed that dispersion of copper increases with an increase in nickel loading on ɣ-Al<sub>2</sub>O<sub>3</sub> due to strong interaction between nickel and copper oxide particles. This also led to the formation of mixed copper-nickel oxides in calcined catalysts at the highest loading of nickel and copper (i.e. Cu/Ni<!--> <!-->=<!--> <!-->1). In catalytic activity, both the monometallic Cu/ɣ-Al<sub>2</sub>O<sub>3</sub> and Ni/ɣ-Al<sub>2</sub>O<sub>3</sub> showed lower activity and selectivity towards hydrogenation of both Furfural and 5-Hydroxymethylfurfural to 2-methylfuran (2-MF) and 2, 5-dimethylfuran (DMF), respectively. However, with increase in nickel loading, the activity and the selectivity of Cu/ɣ-Al<sub>2</sub>O<sub>3</sub> drastically increased for both the cases and Cu-Ni/ɣ-Al<sub>2</sub>O<sub>3</sub> (Cu/Ni<!--> <!-->=<!--> <!-->1) showed the highest catalytic activity. Furthermore, combination of Cu/Ni ratios and temperature plays a significant role in the product distribution, as in the case of furfural hydrogenation, at a lower temperature, furfuryl alcohol (FOL) appears as the main product while at a higher temperature, 2-methylfuran (2-MF) is found to be the dominant product over Cu-Ni/ɣ-Al<sub>2</sub>O<sub>3</sub> (Cu/Ni<!--> <!-->=<!--> <!-->1) catalysts. Similarly, 2,5-bishydroxymethylfuran (BHF) is found to be the major product at a lower temperature and 2,5-dimethylfuran (DMF) is selectively produced at a higher temperature in the HMF hydrogenation. Furthermore, reaction pathways are discussed for both the reactions.</p></div>\",\"PeriodicalId\":370,\"journal\":{\"name\":\"Journal of Molecular Catalysis A: Chemical\",\"volume\":\"426 \",\"pages\":\"Pages 244-256\"},\"PeriodicalIF\":5.0620,\"publicationDate\":\"2017-01-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/j.molcata.2016.11.023\",\"citationCount\":\"109\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Molecular Catalysis A: Chemical\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S138111691630499X\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Molecular Catalysis A: Chemical","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S138111691630499X","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Synergism studies on alumina-supported copper-nickel catalysts towards furfural and 5-hydroxymethylfurfural hydrogenation
The structure of alumina-supported copper-nickel catalysts prepared by impregnation method was studied by using a combination of various characterization techniques including XRD, N2-sorption, TEM, H2-TPR, NH3-TPD, XANES/EXAFS and CHNS methods. A series of characterizations revealed that dispersion of copper increases with an increase in nickel loading on ɣ-Al2O3 due to strong interaction between nickel and copper oxide particles. This also led to the formation of mixed copper-nickel oxides in calcined catalysts at the highest loading of nickel and copper (i.e. Cu/Ni = 1). In catalytic activity, both the monometallic Cu/ɣ-Al2O3 and Ni/ɣ-Al2O3 showed lower activity and selectivity towards hydrogenation of both Furfural and 5-Hydroxymethylfurfural to 2-methylfuran (2-MF) and 2, 5-dimethylfuran (DMF), respectively. However, with increase in nickel loading, the activity and the selectivity of Cu/ɣ-Al2O3 drastically increased for both the cases and Cu-Ni/ɣ-Al2O3 (Cu/Ni = 1) showed the highest catalytic activity. Furthermore, combination of Cu/Ni ratios and temperature plays a significant role in the product distribution, as in the case of furfural hydrogenation, at a lower temperature, furfuryl alcohol (FOL) appears as the main product while at a higher temperature, 2-methylfuran (2-MF) is found to be the dominant product over Cu-Ni/ɣ-Al2O3 (Cu/Ni = 1) catalysts. Similarly, 2,5-bishydroxymethylfuran (BHF) is found to be the major product at a lower temperature and 2,5-dimethylfuran (DMF) is selectively produced at a higher temperature in the HMF hydrogenation. Furthermore, reaction pathways are discussed for both the reactions.
期刊介绍:
The Journal of Molecular Catalysis A: Chemical publishes original, rigorous, and scholarly full papers that examine the molecular and atomic aspects of catalytic activation and reaction mechanisms in homogeneous catalysis, heterogeneous catalysis (including supported organometallic catalysis), and computational catalysis.