Mengyao Xu, Fei Liu, Shike Liu, Jun Ma, Mengqin Yao, Xiaodan Wang, Jianxin Cao
{"title":"Atomically dispersed Ru on flower-like In2O3 to boost CO2 hydrogenation to methanol","authors":"Mengyao Xu, Fei Liu, Shike Liu, Jun Ma, Mengqin Yao, Xiaodan Wang, Jianxin Cao","doi":"10.1016/j.jmst.2024.10.004","DOIUrl":null,"url":null,"abstract":"Metal-based catalysts are prevalent in the CO<sub>2</sub> hydrogenation to methanol owing to their remarkable catalytic activity. Herein, Ru/In<sub>2</sub>O<sub>3</sub> catalysts with different morphologies obtained by doping Ru into In<sub>2</sub>O<sub>3</sub> with irregular, rod-like, and flower-like morphologies are used for catalytic CO<sub>2</sub> hydrogenation to methanol. Results indicate that the flower-like Ru/In<sub>2</sub>O<sub>3</sub> (Ru/In<sub>2</sub>O<sub>3</sub>-F) exhibits higher catalytic performance than Ru/In<sub>2</sub>O<sub>3</sub> with other morphologies, achieving a 12.9% CO<sub>2</sub> conversion, 74.02% methanol selectivity, and 671.36 mg<sub>MeOH</sub>·h<sup>−1</sup>·g<sub>cat</sub><sup>−1</sup> methanol spatiotemporal yield. Furthermore, Ru/In<sub>2</sub>O<sub>3</sub>-F maintains its catalytic stability over 200 h at 5 MPa and 290 °C. The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In<sub>2</sub>O<sub>3</sub>. The strong interaction between atomically dispersed Ru and In<sub>2</sub>O<sub>3</sub>-F enhances the structural stability of Ru, inhibiting the agglomeration of the catalyst during the reaction process. Furthermore, density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes, facilitating the catalytic activation of H<sub>2</sub> into H intermediates. It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO<sub>2</sub> reduction. These findings provide a theoretical basis for the development of high-performance catalysts for CO<sub>2</sub> hydrogenation.","PeriodicalId":16154,"journal":{"name":"Journal of Materials Science & Technology","volume":"44 1","pages":""},"PeriodicalIF":11.2000,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Science & Technology","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.jmst.2024.10.004","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Metal-based catalysts are prevalent in the CO2 hydrogenation to methanol owing to their remarkable catalytic activity. Herein, Ru/In2O3 catalysts with different morphologies obtained by doping Ru into In2O3 with irregular, rod-like, and flower-like morphologies are used for catalytic CO2 hydrogenation to methanol. Results indicate that the flower-like Ru/In2O3 (Ru/In2O3-F) exhibits higher catalytic performance than Ru/In2O3 with other morphologies, achieving a 12.9% CO2 conversion, 74.02% methanol selectivity, and 671.36 mgMeOH·h−1·gcat−1 methanol spatiotemporal yield. Furthermore, Ru/In2O3-F maintains its catalytic stability over 200 h at 5 MPa and 290 °C. The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In2O3. The strong interaction between atomically dispersed Ru and In2O3-F enhances the structural stability of Ru, inhibiting the agglomeration of the catalyst during the reaction process. Furthermore, density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes, facilitating the catalytic activation of H2 into H intermediates. It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO2 reduction. These findings provide a theoretical basis for the development of high-performance catalysts for CO2 hydrogenation.
期刊介绍:
Journal of Materials Science & Technology strives to promote global collaboration in the field of materials science and technology. It primarily publishes original research papers, invited review articles, letters, research notes, and summaries of scientific achievements. The journal covers a wide range of materials science and technology topics, including metallic materials, inorganic nonmetallic materials, and composite materials.