Yiming Chen , Chuan Wang , Yi Liu , Qianwen Zhang , Ling Zhou , Yi Zhang
{"title":"The Pd/ZrO2 catalyst inversely loaded with various metal oxides for methanol synthesis from carbon dioxide","authors":"Yiming Chen , Chuan Wang , Yi Liu , Qianwen Zhang , Ling Zhou , Yi Zhang","doi":"10.1016/j.jcat.2024.115527","DOIUrl":null,"url":null,"abstract":"<div><p>The selectivity and stability of catalysts for methanol synthesis from CO<sub>2</sub> still remain to be enhanced. In this work, we synthesized a series of Pd/ZrO<sub>2</sub> catalysts inversely loaded with various metal oxide promoters (ZnO, In<sub>2</sub>O<sub>3</sub>, and CeO<sub>2</sub>), those would partially cover Pd metal surface and form some new metal-promoter interface, to explore the nature in the performance of CO<sub>2</sub> hydrogenation to methanol. The catalyst synthesized by this approach could limit the growth of Pd particles during the reduction and form new metal–metal oxide interfaces with different functions of CO<sub>2</sub> hydrogenation, improving the reaction performance of Pd-ZrO<sub>2</sub> catalysts. As a result, the ZnO-Pd/ZrO<sub>2</sub> catalyst exhibited the highest CO<sub>2</sub> conversion (12.0 %), methanol selectivity (95.6 %), and STY of methanol (472 g<sub>MeOH</sub>kg<sub>cat</sub><sup>-1</sup>h<sup>−1</sup>), with excellent stability. The results of HRTEM, H<sub>2</sub>-TPR, XPS, and XAFS showed that the ZnO-Pd/ZrO<sub>2</sub> catalyst had the typical Pd-ZnO interface with Pd<sup>2+</sup> species after the H<sub>2</sub> reduction, which could enhance the adsorption and activation of CO<sub>2</sub>. In addition, the <em>in situ</em> DRIFTS and NAP-XPS results implied that the Pd-ZnO interface significantly improved the formation of formate (HCOO*) and methoxy (H<sub>3</sub>CO*) species, which were considered to be the key intermediates of methanol generation, and thus greatly enhanced the selectivity of methanol.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-05-01","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/S0021951724002409","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The selectivity and stability of catalysts for methanol synthesis from CO2 still remain to be enhanced. In this work, we synthesized a series of Pd/ZrO2 catalysts inversely loaded with various metal oxide promoters (ZnO, In2O3, and CeO2), those would partially cover Pd metal surface and form some new metal-promoter interface, to explore the nature in the performance of CO2 hydrogenation to methanol. The catalyst synthesized by this approach could limit the growth of Pd particles during the reduction and form new metal–metal oxide interfaces with different functions of CO2 hydrogenation, improving the reaction performance of Pd-ZrO2 catalysts. As a result, the ZnO-Pd/ZrO2 catalyst exhibited the highest CO2 conversion (12.0 %), methanol selectivity (95.6 %), and STY of methanol (472 gMeOHkgcat-1h−1), with excellent stability. The results of HRTEM, H2-TPR, XPS, and XAFS showed that the ZnO-Pd/ZrO2 catalyst had the typical Pd-ZnO interface with Pd2+ species after the H2 reduction, which could enhance the adsorption and activation of CO2. In addition, the in situ DRIFTS and NAP-XPS results implied that the Pd-ZnO interface significantly improved the formation of formate (HCOO*) and methoxy (H3CO*) species, which were considered to be the key intermediates of methanol generation, and thus greatly enhanced the selectivity of methanol.
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.