Zhendong Yu, Zihao Qin, Hongyuan Liu, Shaoyu Yuan, Renjie Huang, Binglin Chen, Zheng Li, Lu Lin, Carol Sze Ki Lin, Xianhai Zeng
{"title":"Ni-TT-Nb2O5 对生物质衍生呋喃化合物中 C-OH 键的选择性吸附和氢解作用","authors":"Zhendong Yu, Zihao Qin, Hongyuan Liu, Shaoyu Yuan, Renjie Huang, Binglin Chen, Zheng Li, Lu Lin, Carol Sze Ki Lin, Xianhai Zeng","doi":"10.1016/j.jcat.2024.115844","DOIUrl":null,"url":null,"abstract":"The selective hydrogenolysis of C-OH in renewable furanic compounds to corresponding high-value products has been attractive yet challenging, and the mechanism remains vague. Herein, a non-noble catalyst (Ni-TT-Nb<sub>2</sub>O<sub>5</sub>) was prepared to address this challenge. Batch and continuous reaction results show that Ni-TT-Nb<sub>2</sub>O<sub>5</sub> can selectively hydrodeoxygenate 5-hdyroxymethylfurfural to 5-methylfurfural with a very high selectivity of 99 %. Moreover, Ni-TT-Nb<sub>2</sub>O<sub>5</sub> can also selectively hydrodeoxygenate various furanic, benzenoid and aliphatic alcohols, achieving up to > 95 % selectivity. In-situ FTIR and DFT calculations showed that compared with other Ni-supported (supports = Al<sub>2</sub>O<sub>3</sub>, CeO<sub>2</sub>, SiO<sub>2</sub>, ZrO<sub>2</sub>) catalysts, HMF was adsorbed on Ni-TT-Nb<sub>2</sub>O<sub>5</sub> surface <em>via</em> parallel mode exclusively, and the C-OH bond was easier to be activated. This work therefore explained the mechanism of selective hydrogenolysis of C-OH in HMF over Ni-TT-Nb<sub>2</sub>O<sub>5</sub>, and offered an advanced approach for the upgrading of C-OH-containing furanic compounds as well as benzenoid and aliphatic alcohols.","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"16 1","pages":""},"PeriodicalIF":6.5000,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective adsorption and hydrogenolysis of C-OH bond in biomass derived furanic compounds over Ni-TT-Nb2O5\",\"authors\":\"Zhendong Yu, Zihao Qin, Hongyuan Liu, Shaoyu Yuan, Renjie Huang, Binglin Chen, Zheng Li, Lu Lin, Carol Sze Ki Lin, Xianhai Zeng\",\"doi\":\"10.1016/j.jcat.2024.115844\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The selective hydrogenolysis of C-OH in renewable furanic compounds to corresponding high-value products has been attractive yet challenging, and the mechanism remains vague. Herein, a non-noble catalyst (Ni-TT-Nb<sub>2</sub>O<sub>5</sub>) was prepared to address this challenge. Batch and continuous reaction results show that Ni-TT-Nb<sub>2</sub>O<sub>5</sub> can selectively hydrodeoxygenate 5-hdyroxymethylfurfural to 5-methylfurfural with a very high selectivity of 99 %. Moreover, Ni-TT-Nb<sub>2</sub>O<sub>5</sub> can also selectively hydrodeoxygenate various furanic, benzenoid and aliphatic alcohols, achieving up to > 95 % selectivity. In-situ FTIR and DFT calculations showed that compared with other Ni-supported (supports = Al<sub>2</sub>O<sub>3</sub>, CeO<sub>2</sub>, SiO<sub>2</sub>, ZrO<sub>2</sub>) catalysts, HMF was adsorbed on Ni-TT-Nb<sub>2</sub>O<sub>5</sub> surface <em>via</em> parallel mode exclusively, and the C-OH bond was easier to be activated. This work therefore explained the mechanism of selective hydrogenolysis of C-OH in HMF over Ni-TT-Nb<sub>2</sub>O<sub>5</sub>, and offered an advanced approach for the upgrading of C-OH-containing furanic compounds as well as benzenoid and aliphatic alcohols.\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"16 1\",\"pages\":\"\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-11-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jcat.2024.115844\",\"RegionNum\":1,\"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":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.jcat.2024.115844","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Selective adsorption and hydrogenolysis of C-OH bond in biomass derived furanic compounds over Ni-TT-Nb2O5
The selective hydrogenolysis of C-OH in renewable furanic compounds to corresponding high-value products has been attractive yet challenging, and the mechanism remains vague. Herein, a non-noble catalyst (Ni-TT-Nb2O5) was prepared to address this challenge. Batch and continuous reaction results show that Ni-TT-Nb2O5 can selectively hydrodeoxygenate 5-hdyroxymethylfurfural to 5-methylfurfural with a very high selectivity of 99 %. Moreover, Ni-TT-Nb2O5 can also selectively hydrodeoxygenate various furanic, benzenoid and aliphatic alcohols, achieving up to > 95 % selectivity. In-situ FTIR and DFT calculations showed that compared with other Ni-supported (supports = Al2O3, CeO2, SiO2, ZrO2) catalysts, HMF was adsorbed on Ni-TT-Nb2O5 surface via parallel mode exclusively, and the C-OH bond was easier to be activated. This work therefore explained the mechanism of selective hydrogenolysis of C-OH in HMF over Ni-TT-Nb2O5, and offered an advanced approach for the upgrading of C-OH-containing furanic compounds as well as benzenoid and aliphatic alcohols.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.