Chongya Yang , Weijue Wang , Hongying Zhuo , Zheng Shen , Tianyu Zhang , Xiaofeng Yang , Yanqiang Huang
{"title":"基于 Ru 的纳米催化剂的相工程,提高 CO2 甲烷化活性","authors":"Chongya Yang , Weijue Wang , Hongying Zhuo , Zheng Shen , Tianyu Zhang , Xiaofeng Yang , Yanqiang Huang","doi":"10.1016/S1872-2067(24)60055-0","DOIUrl":null,"url":null,"abstract":"<div><p>The catalytic behavior of metal nanocatalysts is intrinsically contingent on the diversity of their exposed surfaces, which can be substantially regulated through the phase engineering of metal nanoparticles. In this study, it is demonstrated that the face-centered cubic (fcc) phase Ru with a close-packed (111) surface presents superior catalytic activity towards CO<sub>2</sub> methanation. This behavior is attributed to its enhanced capability toward CO<sub>2</sub> chemisorption derived from its inherently high surface reactivity. Complete exposure of such surfaces was successfully achieved experimentally by the synthesis of icosahedral Ru metal nanoparticles, which exhibited remarkable performance for CO<sub>2</sub> methanation with 5–8 times higher activity than its conventional hexagonal close-packed (hcp) counterpart when supported on inert supports. However, for the joined fcc-Ru nanoparticles in the fresh catalyst, an fcc- to hcp-phase transformation was observed at a relatively high temperature with the <em>in situ</em> characterizations, which resulted in metal agglomeration and led to catalyst deactivation. However, the CO<sub>2</sub> conversion was still much higher than that of the hcp-phase Ru nanocatalysts, as the monodispersed particles could maintain their fcc phase. Our results demonstrate that phase engineering of Ru nanocatalysts is an effective strategy for a catalyst design with improved catalytic performance. However, the phase transformation could represent a latent instability of the catalysts, which should be considered for the further development of robust catalysts.</p></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":15.7000,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Phase engineering of Ru-based nanocatalysts for enhanced activity toward CO2 methanation\",\"authors\":\"Chongya Yang , Weijue Wang , Hongying Zhuo , Zheng Shen , Tianyu Zhang , Xiaofeng Yang , Yanqiang Huang\",\"doi\":\"10.1016/S1872-2067(24)60055-0\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The catalytic behavior of metal nanocatalysts is intrinsically contingent on the diversity of their exposed surfaces, which can be substantially regulated through the phase engineering of metal nanoparticles. In this study, it is demonstrated that the face-centered cubic (fcc) phase Ru with a close-packed (111) surface presents superior catalytic activity towards CO<sub>2</sub> methanation. This behavior is attributed to its enhanced capability toward CO<sub>2</sub> chemisorption derived from its inherently high surface reactivity. Complete exposure of such surfaces was successfully achieved experimentally by the synthesis of icosahedral Ru metal nanoparticles, which exhibited remarkable performance for CO<sub>2</sub> methanation with 5–8 times higher activity than its conventional hexagonal close-packed (hcp) counterpart when supported on inert supports. However, for the joined fcc-Ru nanoparticles in the fresh catalyst, an fcc- to hcp-phase transformation was observed at a relatively high temperature with the <em>in situ</em> characterizations, which resulted in metal agglomeration and led to catalyst deactivation. However, the CO<sub>2</sub> conversion was still much higher than that of the hcp-phase Ru nanocatalysts, as the monodispersed particles could maintain their fcc phase. Our results demonstrate that phase engineering of Ru nanocatalysts is an effective strategy for a catalyst design with improved catalytic performance. However, the phase transformation could represent a latent instability of the catalysts, which should be considered for the further development of robust catalysts.</p></div>\",\"PeriodicalId\":9832,\"journal\":{\"name\":\"Chinese Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2024-06-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872206724600550\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724600550","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Phase engineering of Ru-based nanocatalysts for enhanced activity toward CO2 methanation
The catalytic behavior of metal nanocatalysts is intrinsically contingent on the diversity of their exposed surfaces, which can be substantially regulated through the phase engineering of metal nanoparticles. In this study, it is demonstrated that the face-centered cubic (fcc) phase Ru with a close-packed (111) surface presents superior catalytic activity towards CO2 methanation. This behavior is attributed to its enhanced capability toward CO2 chemisorption derived from its inherently high surface reactivity. Complete exposure of such surfaces was successfully achieved experimentally by the synthesis of icosahedral Ru metal nanoparticles, which exhibited remarkable performance for CO2 methanation with 5–8 times higher activity than its conventional hexagonal close-packed (hcp) counterpart when supported on inert supports. However, for the joined fcc-Ru nanoparticles in the fresh catalyst, an fcc- to hcp-phase transformation was observed at a relatively high temperature with the in situ characterizations, which resulted in metal agglomeration and led to catalyst deactivation. However, the CO2 conversion was still much higher than that of the hcp-phase Ru nanocatalysts, as the monodispersed particles could maintain their fcc phase. Our results demonstrate that phase engineering of Ru nanocatalysts is an effective strategy for a catalyst design with improved catalytic performance. However, the phase transformation could represent a latent instability of the catalysts, which should be considered for the further development of robust catalysts.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.