Maya Shopska, Krassimir Tenchev, Georgi Kadinov, Hristo Kolev, Martin Fabian, Katerina Aleksieva
{"title":"CO 加氢过程中 (10%Co + 0.5%Pd)/TiO2 催化剂表面吸附和反应位点的异质性","authors":"Maya Shopska, Krassimir Tenchev, Georgi Kadinov, Hristo Kolev, Martin Fabian, Katerina Aleksieva","doi":"10.1007/s11144-024-02644-8","DOIUrl":null,"url":null,"abstract":"<div><p>Adsorption and reaction site heterogeneity of titania-supported (10%Co + 0.5%Pd) catalysts in CO hydrogenation was studied by chemisorption, temperature-programmed desorption, and diffuse reflectance infrared Fourier transform spectroscopy techniques. Precursor material was treated in various media as reductive, inert, or oxidative. Cobalt metal sites and TiO<sub>2</sub> support heterogeneity were proved. Upon H<sub>2</sub> chemisorption, a pre-reduced sample exposed mostly homogeneous metal surface. Surface heterogeneity toward CO chemisorption depended on preliminary treatment. A catalyst prepared in inert medium revealed moderate activity dynamics of adsorption and reaction sites. Weak to medium strength sites toward hydrogen adsorption were relatively strong in terms of CO adsorption. Carbonate-(like) species occupied medium and strong sites on the support. Sites of weak strength for CO adsorption were active in hydrogenation but very strong in terms of CH<sub>x</sub> intermediates adsorption.</p><h3>Graphical abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":750,"journal":{"name":"Reaction Kinetics, Mechanisms and Catalysis","volume":"137 4","pages":"2147 - 2171"},"PeriodicalIF":1.7000,"publicationDate":"2024-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Heterogeneity of adsorption and reaction sites on the surface of (10%Co + 0.5%Pd)/TiO2 catalysts during CO hydrogenation\",\"authors\":\"Maya Shopska, Krassimir Tenchev, Georgi Kadinov, Hristo Kolev, Martin Fabian, Katerina Aleksieva\",\"doi\":\"10.1007/s11144-024-02644-8\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Adsorption and reaction site heterogeneity of titania-supported (10%Co + 0.5%Pd) catalysts in CO hydrogenation was studied by chemisorption, temperature-programmed desorption, and diffuse reflectance infrared Fourier transform spectroscopy techniques. Precursor material was treated in various media as reductive, inert, or oxidative. Cobalt metal sites and TiO<sub>2</sub> support heterogeneity were proved. Upon H<sub>2</sub> chemisorption, a pre-reduced sample exposed mostly homogeneous metal surface. Surface heterogeneity toward CO chemisorption depended on preliminary treatment. A catalyst prepared in inert medium revealed moderate activity dynamics of adsorption and reaction sites. Weak to medium strength sites toward hydrogen adsorption were relatively strong in terms of CO adsorption. Carbonate-(like) species occupied medium and strong sites on the support. Sites of weak strength for CO adsorption were active in hydrogenation but very strong in terms of CH<sub>x</sub> intermediates adsorption.</p><h3>Graphical abstract</h3>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":750,\"journal\":{\"name\":\"Reaction Kinetics, Mechanisms and Catalysis\",\"volume\":\"137 4\",\"pages\":\"2147 - 2171\"},\"PeriodicalIF\":1.7000,\"publicationDate\":\"2024-05-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Reaction Kinetics, Mechanisms and Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11144-024-02644-8\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Reaction Kinetics, Mechanisms and Catalysis","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s11144-024-02644-8","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
通过化学吸附、温度编程解吸和漫反射红外傅立叶变换光谱技术,研究了二氧化钛支撑(10%Co + 0.5%Pd)催化剂在 CO 加氢过程中的吸附和反应位点异质性。前驱体材料在不同介质中进行了还原、惰性或氧化处理。证明了钴金属位点和二氧化钛支持物的异质性。在对 H2 进行化学吸附时,预还原样品的金属表面大多是均匀的。CO 化学吸附的表面异质性取决于初步处理。在惰性介质中制备的催化剂显示出吸附和反应位点的中等活性动态。对氢的吸附强度为弱至中等,而对 CO 的吸附强度则相对较强。碳酸盐(类)物种占据了支持物上的中强位点。二氧化碳吸附强度较弱的位点在氢化反应中很活跃,但对 CHx 中间产物的吸附却很强。
Heterogeneity of adsorption and reaction sites on the surface of (10%Co + 0.5%Pd)/TiO2 catalysts during CO hydrogenation
Adsorption and reaction site heterogeneity of titania-supported (10%Co + 0.5%Pd) catalysts in CO hydrogenation was studied by chemisorption, temperature-programmed desorption, and diffuse reflectance infrared Fourier transform spectroscopy techniques. Precursor material was treated in various media as reductive, inert, or oxidative. Cobalt metal sites and TiO2 support heterogeneity were proved. Upon H2 chemisorption, a pre-reduced sample exposed mostly homogeneous metal surface. Surface heterogeneity toward CO chemisorption depended on preliminary treatment. A catalyst prepared in inert medium revealed moderate activity dynamics of adsorption and reaction sites. Weak to medium strength sites toward hydrogen adsorption were relatively strong in terms of CO adsorption. Carbonate-(like) species occupied medium and strong sites on the support. Sites of weak strength for CO adsorption were active in hydrogenation but very strong in terms of CHx intermediates adsorption.
期刊介绍:
Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields:
-kinetics of homogeneous reactions in gas, liquid and solid phase;
-Homogeneous catalysis;
-Heterogeneous catalysis;
-Adsorption in heterogeneous catalysis;
-Transport processes related to reaction kinetics and catalysis;
-Preparation and study of catalysts;
-Reactors and apparatus.
Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.