Jiali Lu , Yongyong Shi , Xiong He , Qiao Zhou , Ziwei Li , Fei Liu , Min Li
{"title":"深入了解钼在二氧化碳甲烷转化过程中促进 CHx* 氧化的作用","authors":"Jiali Lu , Yongyong Shi , Xiong He , Qiao Zhou , Ziwei Li , Fei Liu , Min Li","doi":"10.1016/j.renene.2024.120915","DOIUrl":null,"url":null,"abstract":"<div><p>CH<sub>x</sub>* oxidation is one of the most vital routes to alleviate the carbon deposition problem of CO<sub>2</sub> reforming of methane (DRM) reaction. Whereas, little experimental evidence has been observed on NiMo catalysts where the CH<sub>x</sub>* oxidation was dominant over its dissociation reaction. Herein, to experimentally unveil the CH<sub>x</sub>* oxidation route of NiMo catalysts, we design three catalysts with different particle sizes and structures. Among them, Mo/Niphy@SiO<sub>2</sub> core shell catalyst demonstrated the dominant CH<sub>x</sub>* oxidation route over its dissociation based on <em>in-situ</em> diffuse reflectance infrared Fourier transform spectroscopy experiments. This was attributed to the confinement effect of SiO<sub>2</sub> and the formation of Ni–Mo alloy, inhibiting the CH<sub>x</sub>* dissociation reaction. It exhibited relatively stable CH<sub>4</sub> and CO<sub>2</sub> conversions (77 % and 75 % respectively) within 180 h. By contrast, on Mo/Niphy catalyst which has a big Ni size, CH<sub>x</sub>* was mainly dissociated to C* and oxidized to CO which further underwent a disproportion reaction to produce CO<sub>2</sub> and C*, leading to the severe carbon deposition and unstable DRM performance. The strategy to unveil the dominant role of CH<sub>x</sub>* oxidation via design catalysts with different sizes and structures sheds light on the study of reaction mechanism of other reactions.</p></div>","PeriodicalId":419,"journal":{"name":"Renewable Energy","volume":null,"pages":null},"PeriodicalIF":9.0000,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Insights into the role of Mo in boosting CHx* oxidation for CO2 methane reforming\",\"authors\":\"Jiali Lu , Yongyong Shi , Xiong He , Qiao Zhou , Ziwei Li , Fei Liu , Min Li\",\"doi\":\"10.1016/j.renene.2024.120915\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>CH<sub>x</sub>* oxidation is one of the most vital routes to alleviate the carbon deposition problem of CO<sub>2</sub> reforming of methane (DRM) reaction. Whereas, little experimental evidence has been observed on NiMo catalysts where the CH<sub>x</sub>* oxidation was dominant over its dissociation reaction. Herein, to experimentally unveil the CH<sub>x</sub>* oxidation route of NiMo catalysts, we design three catalysts with different particle sizes and structures. Among them, Mo/Niphy@SiO<sub>2</sub> core shell catalyst demonstrated the dominant CH<sub>x</sub>* oxidation route over its dissociation based on <em>in-situ</em> diffuse reflectance infrared Fourier transform spectroscopy experiments. This was attributed to the confinement effect of SiO<sub>2</sub> and the formation of Ni–Mo alloy, inhibiting the CH<sub>x</sub>* dissociation reaction. It exhibited relatively stable CH<sub>4</sub> and CO<sub>2</sub> conversions (77 % and 75 % respectively) within 180 h. By contrast, on Mo/Niphy catalyst which has a big Ni size, CH<sub>x</sub>* was mainly dissociated to C* and oxidized to CO which further underwent a disproportion reaction to produce CO<sub>2</sub> and C*, leading to the severe carbon deposition and unstable DRM performance. The strategy to unveil the dominant role of CH<sub>x</sub>* oxidation via design catalysts with different sizes and structures sheds light on the study of reaction mechanism of other reactions.</p></div>\",\"PeriodicalId\":419,\"journal\":{\"name\":\"Renewable Energy\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.0000,\"publicationDate\":\"2024-07-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Renewable Energy\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0960148124009832\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Renewable Energy","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0960148124009832","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Insights into the role of Mo in boosting CHx* oxidation for CO2 methane reforming
CHx* oxidation is one of the most vital routes to alleviate the carbon deposition problem of CO2 reforming of methane (DRM) reaction. Whereas, little experimental evidence has been observed on NiMo catalysts where the CHx* oxidation was dominant over its dissociation reaction. Herein, to experimentally unveil the CHx* oxidation route of NiMo catalysts, we design three catalysts with different particle sizes and structures. Among them, Mo/Niphy@SiO2 core shell catalyst demonstrated the dominant CHx* oxidation route over its dissociation based on in-situ diffuse reflectance infrared Fourier transform spectroscopy experiments. This was attributed to the confinement effect of SiO2 and the formation of Ni–Mo alloy, inhibiting the CHx* dissociation reaction. It exhibited relatively stable CH4 and CO2 conversions (77 % and 75 % respectively) within 180 h. By contrast, on Mo/Niphy catalyst which has a big Ni size, CHx* was mainly dissociated to C* and oxidized to CO which further underwent a disproportion reaction to produce CO2 and C*, leading to the severe carbon deposition and unstable DRM performance. The strategy to unveil the dominant role of CHx* oxidation via design catalysts with different sizes and structures sheds light on the study of reaction mechanism of other reactions.
期刊介绍:
Renewable Energy journal is dedicated to advancing knowledge and disseminating insights on various topics and technologies within renewable energy systems and components. Our mission is to support researchers, engineers, economists, manufacturers, NGOs, associations, and societies in staying updated on new developments in their respective fields and applying alternative energy solutions to current practices.
As an international, multidisciplinary journal in renewable energy engineering and research, we strive to be a premier peer-reviewed platform and a trusted source of original research and reviews in the field of renewable energy. Join us in our endeavor to drive innovation and progress in sustainable energy solutions.