{"title":"Neighbouring metal and Lewis acid sites: Synergistic cooperators for the selective hydrogenation of C = O in anthraquinone","authors":"Chunyan Zhang , Xiao Liang , Mengdi Li, Qingmao Yang, Chun Shen","doi":"10.1016/j.ces.2024.120455","DOIUrl":null,"url":null,"abstract":"<div><p>Selective hydrogenation of 2-ethylanthraquinone to 2-ethylanthrahydroquinone is a critical step to produce hydrogen peroxide in industry, and the development of non-noble catalysts with both high selectivity for C = O hydrogenation and superior activity is highly desirable but challenging. Herein, we developed a Ni@Si(5<!--> <!-->5<!--> <!-->0) catalyst for this reaction, affording 90.7 % conversion and 99.2 % selectivity after reaction at 50 °C for 6 h. The initial reaction rate reached 363.0 μmol·g<sup>–1</sup><sub>Ni</sub>·min<sup>−1</sup>, which is about two-fold higher than those of the previously-reported Ni-based catalysts. Kinetic studies, catalysts characterizations and the adsorption experiment revealed that the catalytic performance of Ni@Si(<em>T</em>) catalysts critically depends on the synergy between the metal site (Ni<sup>0</sup>) and Lewis acid site (positively charged Ni): Ni<sup>0</sup> accounts for the dissociation of hydrogen, and Lewis acid site is responsible for the adsorptive activation of C = O group. This catalyst design strategy and insights into active sites may provide beneficial guidance for high-performance catalyst design.</p></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":null,"pages":null},"PeriodicalIF":4.1000,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Science","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0009250924007553","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Selective hydrogenation of 2-ethylanthraquinone to 2-ethylanthrahydroquinone is a critical step to produce hydrogen peroxide in industry, and the development of non-noble catalysts with both high selectivity for C = O hydrogenation and superior activity is highly desirable but challenging. Herein, we developed a Ni@Si(5 5 0) catalyst for this reaction, affording 90.7 % conversion and 99.2 % selectivity after reaction at 50 °C for 6 h. The initial reaction rate reached 363.0 μmol·g–1Ni·min−1, which is about two-fold higher than those of the previously-reported Ni-based catalysts. Kinetic studies, catalysts characterizations and the adsorption experiment revealed that the catalytic performance of Ni@Si(T) catalysts critically depends on the synergy between the metal site (Ni0) and Lewis acid site (positively charged Ni): Ni0 accounts for the dissociation of hydrogen, and Lewis acid site is responsible for the adsorptive activation of C = O group. This catalyst design strategy and insights into active sites may provide beneficial guidance for high-performance catalyst design.
期刊介绍:
Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline.
Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.