{"title":"介孔二氧化硅包裹核壳 NiRh@NiO 纳米催化剂用于性能增强型乙醇蒸汽转化","authors":"Qiangqiang Xue, Zhengwen Li, Binhang Yan, Shafqat Ullah, Yujun Wang, Guangsheng Luo","doi":"10.1016/j.jcat.2024.115536","DOIUrl":null,"url":null,"abstract":"<div><p>A novel mesoporous SiO<sub>2</sub> encapsulated core-shell NiRh@NiO nanostructure was constructed to enhance the activity and stability of ethanol steam reforming (ESR). At 550 °C and ethanol-WHSV = 21 h<sup>−1</sup>, the specific activity and conversion loss (17 h) of NiRh@NiO@m-SiO<sub>2</sub> were 0.42 mol<sub>ethanol</sub>/(g<sub>cat.</sub>·h) and 10.9 %. The alloying of NiRh core, dominated NiO in shell, and abundant mesopore of SiO<sub>2</sub> were confirmed by systematic characterization techniques. The in situ DRIFTS results indicated that alloying Ni and Rh boosted ethoxide dehydrogenation to acetaldehyde and acetate demethanation to carbonate. ReaxFF molecular dynamics (MD) simulations suggested that NiO shell was conducive to water activation, which, in turn, promoted the conversion of CH<sub>x</sub>O<sub>y</sub> species. The SiO<sub>2</sub> encapsulation derived confinement effect inhibited both metal core sintering and leaching caused by the filamentous carbon. The abundant mesopores of SiO<sub>2</sub> ensured the facile in-diffusion of water and out-diffusion of carbonaceous products, suppressing carbon deposition within the SiO<sub>2</sub> encapsulation and the destruction of core-shell structure.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mesoporous silica encapsulated core-shell NiRh@NiO nanocatalyst for performance-enhanced ethanol steam reforming\",\"authors\":\"Qiangqiang Xue, Zhengwen Li, Binhang Yan, Shafqat Ullah, Yujun Wang, Guangsheng Luo\",\"doi\":\"10.1016/j.jcat.2024.115536\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A novel mesoporous SiO<sub>2</sub> encapsulated core-shell NiRh@NiO nanostructure was constructed to enhance the activity and stability of ethanol steam reforming (ESR). At 550 °C and ethanol-WHSV = 21 h<sup>−1</sup>, the specific activity and conversion loss (17 h) of NiRh@NiO@m-SiO<sub>2</sub> were 0.42 mol<sub>ethanol</sub>/(g<sub>cat.</sub>·h) and 10.9 %. The alloying of NiRh core, dominated NiO in shell, and abundant mesopore of SiO<sub>2</sub> were confirmed by systematic characterization techniques. The in situ DRIFTS results indicated that alloying Ni and Rh boosted ethoxide dehydrogenation to acetaldehyde and acetate demethanation to carbonate. ReaxFF molecular dynamics (MD) simulations suggested that NiO shell was conducive to water activation, which, in turn, promoted the conversion of CH<sub>x</sub>O<sub>y</sub> species. The SiO<sub>2</sub> encapsulation derived confinement effect inhibited both metal core sintering and leaching caused by the filamentous carbon. The abundant mesopores of SiO<sub>2</sub> ensured the facile in-diffusion of water and out-diffusion of carbonaceous products, suppressing carbon deposition within the SiO<sub>2</sub> encapsulation and the destruction of core-shell structure.</p></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-05-06\",\"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/S0021951724002495\",\"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/S0021951724002495","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
A novel mesoporous SiO2 encapsulated core-shell NiRh@NiO nanostructure was constructed to enhance the activity and stability of ethanol steam reforming (ESR). At 550 °C and ethanol-WHSV = 21 h−1, the specific activity and conversion loss (17 h) of NiRh@NiO@m-SiO2 were 0.42 molethanol/(gcat.·h) and 10.9 %. The alloying of NiRh core, dominated NiO in shell, and abundant mesopore of SiO2 were confirmed by systematic characterization techniques. The in situ DRIFTS results indicated that alloying Ni and Rh boosted ethoxide dehydrogenation to acetaldehyde and acetate demethanation to carbonate. ReaxFF molecular dynamics (MD) simulations suggested that NiO shell was conducive to water activation, which, in turn, promoted the conversion of CHxOy species. The SiO2 encapsulation derived confinement effect inhibited both metal core sintering and leaching caused by the filamentous carbon. The abundant mesopores of SiO2 ensured the facile in-diffusion of water and out-diffusion of carbonaceous products, suppressing carbon deposition within the SiO2 encapsulation and the destruction of core-shell structure.
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.