Xinyu Yao , Dong Liu , Junhong Fu , Jian Wang , Mengle Shen , Zuoyi Xiao , Qingda An , Jiahui Huang
{"title":"水辅助制备用于高效催化四氢呋喃-二甲醇 C-O 键氢解的 Ni/La(OH)3催化剂","authors":"Xinyu Yao , Dong Liu , Junhong Fu , Jian Wang , Mengle Shen , Zuoyi Xiao , Qingda An , Jiahui Huang","doi":"10.1016/j.jcat.2024.115790","DOIUrl":null,"url":null,"abstract":"<div><div>Due to easy dehydration of La(OH)<sub>3</sub> to LaOOH by thermal treatment, it is challenging to prepare highly efficient Ni/La(OH)<sub>3</sub> catalyst for hydrogenolysis reactions. Herein, Ni/La(OH)<sub>3</sub> (Ni/La-2) catalyst is prepared by thermal reduction of NiO/La(OH)<sub>3</sub> in hydrogen flow with vaporized water, while La(OH)<sub>3</sub> is partially dehydrated to LaOOH without water vapor affording Ni/(La(OH)<sub>3</sub> + LaOOH) (Ni/La-1). Ni/La-2 displays 93 % and 3 % yields of 1,2,6-hexanetriol (HTO) and 1,6-hexanediol (HDO) respectively towards C-O hydrogenolysis of tetrahydrofuran-dimethanol (THFDM) in batch reactor and high stability (200 h) in fixed-bed reactor, which is the best among the reported catalysts to the best of our knowledge. Ni/La-2 possesses pure La(OH)<sub>3</sub> as support, enhanced dispersion of Ni species and abundant Ni<sup>δ+</sup>-O-La interfaces in comparison to Ni/La-1, which results in the exceptional catalytic performances in C-O hydrogenolysis of THFDM. A fine control of reaction temperature and time is required to optimize the yields HTO and HDO in hydrogenolysis of THFDM over Ni/La-2. The water-assisted preparation method provides a new perspective for the preparation of La(OH)<sub>3</sub> supported metal catalysts.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115790"},"PeriodicalIF":6.5000,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Water-assisted preparation of Ni/La(OH)3 catalyst for efficient catalytic C-O bond hydrogenolysis of tetrahydrofuran-dimethanol\",\"authors\":\"Xinyu Yao , Dong Liu , Junhong Fu , Jian Wang , Mengle Shen , Zuoyi Xiao , Qingda An , Jiahui Huang\",\"doi\":\"10.1016/j.jcat.2024.115790\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Due to easy dehydration of La(OH)<sub>3</sub> to LaOOH by thermal treatment, it is challenging to prepare highly efficient Ni/La(OH)<sub>3</sub> catalyst for hydrogenolysis reactions. Herein, Ni/La(OH)<sub>3</sub> (Ni/La-2) catalyst is prepared by thermal reduction of NiO/La(OH)<sub>3</sub> in hydrogen flow with vaporized water, while La(OH)<sub>3</sub> is partially dehydrated to LaOOH without water vapor affording Ni/(La(OH)<sub>3</sub> + LaOOH) (Ni/La-1). Ni/La-2 displays 93 % and 3 % yields of 1,2,6-hexanetriol (HTO) and 1,6-hexanediol (HDO) respectively towards C-O hydrogenolysis of tetrahydrofuran-dimethanol (THFDM) in batch reactor and high stability (200 h) in fixed-bed reactor, which is the best among the reported catalysts to the best of our knowledge. Ni/La-2 possesses pure La(OH)<sub>3</sub> as support, enhanced dispersion of Ni species and abundant Ni<sup>δ+</sup>-O-La interfaces in comparison to Ni/La-1, which results in the exceptional catalytic performances in C-O hydrogenolysis of THFDM. A fine control of reaction temperature and time is required to optimize the yields HTO and HDO in hydrogenolysis of THFDM over Ni/La-2. The water-assisted preparation method provides a new perspective for the preparation of La(OH)<sub>3</sub> supported metal catalysts.</div></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"440 \",\"pages\":\"Article 115790\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-10-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951724005037\",\"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://www.sciencedirect.com/science/article/pii/S0021951724005037","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Water-assisted preparation of Ni/La(OH)3 catalyst for efficient catalytic C-O bond hydrogenolysis of tetrahydrofuran-dimethanol
Due to easy dehydration of La(OH)3 to LaOOH by thermal treatment, it is challenging to prepare highly efficient Ni/La(OH)3 catalyst for hydrogenolysis reactions. Herein, Ni/La(OH)3 (Ni/La-2) catalyst is prepared by thermal reduction of NiO/La(OH)3 in hydrogen flow with vaporized water, while La(OH)3 is partially dehydrated to LaOOH without water vapor affording Ni/(La(OH)3 + LaOOH) (Ni/La-1). Ni/La-2 displays 93 % and 3 % yields of 1,2,6-hexanetriol (HTO) and 1,6-hexanediol (HDO) respectively towards C-O hydrogenolysis of tetrahydrofuran-dimethanol (THFDM) in batch reactor and high stability (200 h) in fixed-bed reactor, which is the best among the reported catalysts to the best of our knowledge. Ni/La-2 possesses pure La(OH)3 as support, enhanced dispersion of Ni species and abundant Niδ+-O-La interfaces in comparison to Ni/La-1, which results in the exceptional catalytic performances in C-O hydrogenolysis of THFDM. A fine control of reaction temperature and time is required to optimize the yields HTO and HDO in hydrogenolysis of THFDM over Ni/La-2. The water-assisted preparation method provides a new perspective for the preparation of La(OH)3 supported metal catalysts.
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.