{"title":"调节钯的氧化态以提高 5-羟甲基糠醛的选择性氢化作用","authors":"","doi":"10.1016/j.cjche.2024.05.006","DOIUrl":null,"url":null,"abstract":"<div><p>The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd<sup>0</sup>/Pd<sup>2+</sup> and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C<sub>3</sub>N<sub>4</sub>–300 catalyst with a Pd<sup>0</sup>/Pd<sup>2+</sup> ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd<sup>0</sup> and Pd<sup>2+</sup> in Pd/g–C<sub>3</sub>N<sub>4</sub>–300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.</p></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":3.7000,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural\",\"authors\":\"\",\"doi\":\"10.1016/j.cjche.2024.05.006\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd<sup>0</sup>/Pd<sup>2+</sup> and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C<sub>3</sub>N<sub>4</sub>–300 catalyst with a Pd<sup>0</sup>/Pd<sup>2+</sup> ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd<sup>0</sup> and Pd<sup>2+</sup> in Pd/g–C<sub>3</sub>N<sub>4</sub>–300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.</p></div>\",\"PeriodicalId\":9966,\"journal\":{\"name\":\"Chinese Journal of Chemical Engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.7000,\"publicationDate\":\"2024-08-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S100495412400171X\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S100495412400171X","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd0/Pd2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C3N4–300 catalyst with a Pd0/Pd2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd0 and Pd2+ in Pd/g–C3N4–300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
期刊介绍:
The Chinese Journal of Chemical Engineering (Monthly, started in 1982) is the official journal of the Chemical Industry and Engineering Society of China and published by the Chemical Industry Press Co. Ltd. The aim of the journal is to develop the international exchange of scientific and technical information in the field of chemical engineering. It publishes original research papers that cover the major advancements and achievements in chemical engineering in China as well as some articles from overseas contributors.
The topics of journal include chemical engineering, chemical technology, biochemical engineering, energy and environmental engineering and other relevant fields. Papers are published on the basis of their relevance to theoretical research, practical application or potential uses in the industry as Research Papers, Communications, Reviews and Perspectives. Prominent domestic and overseas chemical experts and scholars have been invited to form an International Advisory Board and the Editorial Committee. It enjoys recognition among Chinese academia and industry as a reliable source of information of what is going on in chemical engineering research, both domestic and abroad.