{"title":"提高脱层 ITQ-6 沸石支撑的镍基催化剂在二氧化碳甲烷化中的催化活性","authors":"R.B. Machado-Silva, J.F. Da Costa-Serra, A. Chica","doi":"10.1016/j.jcat.2024.115609","DOIUrl":null,"url":null,"abstract":"<div><p>Ni-based catalysts supported on delaminated ITQ-6 zeolite with different Si/Al ratios, 30 and ∞, were tested in the methanation of CO<sub>2</sub> and CO. ITQ-6 supports exhibited high surface areas (> 590 m<sup>2</sup>/g), and the catalysts based on them presented elevated CO<sub>2</sub> and CO conversion values, turnover frequencies (TOF), and CH<sub>4</sub> selectivity (> 90 %). Comparing the ITQ-6 catalyst and its precursor ferrierite (FER)-based catalyst, H<sub>2</sub>-chemisorption results confirmed higher metallic dispersion for the former, which resulted in improved H<sub>2</sub> uptake and efficient interaction of reaction intermediates via the associative pathway. Combined kinetic studies indicated that their higher available metallic surface contributed to lower apparent activation energies towards CH<sub>4</sub> formation, accounting for the higher selectivity values. A 15 wt% Ni-based catalyst supported on ITQ-6 zeolite (Si/Al = 30) exhibited catalytic results (X<sub>CO2</sub> = 79 % y S<sub>CH4</sub> = 98 %) comparable or even superior to some of the best zeolite-based catalysts reported so far.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0021951724003221/pdfft?md5=c6ce5261012d81e2ef7f5ad693767328&pid=1-s2.0-S0021951724003221-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Enhancement of catalytic activity in CO2 methanation in Ni-based catalysts supported on delaminated ITQ-6 zeolite\",\"authors\":\"R.B. Machado-Silva, J.F. Da Costa-Serra, A. Chica\",\"doi\":\"10.1016/j.jcat.2024.115609\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Ni-based catalysts supported on delaminated ITQ-6 zeolite with different Si/Al ratios, 30 and ∞, were tested in the methanation of CO<sub>2</sub> and CO. ITQ-6 supports exhibited high surface areas (> 590 m<sup>2</sup>/g), and the catalysts based on them presented elevated CO<sub>2</sub> and CO conversion values, turnover frequencies (TOF), and CH<sub>4</sub> selectivity (> 90 %). Comparing the ITQ-6 catalyst and its precursor ferrierite (FER)-based catalyst, H<sub>2</sub>-chemisorption results confirmed higher metallic dispersion for the former, which resulted in improved H<sub>2</sub> uptake and efficient interaction of reaction intermediates via the associative pathway. Combined kinetic studies indicated that their higher available metallic surface contributed to lower apparent activation energies towards CH<sub>4</sub> formation, accounting for the higher selectivity values. A 15 wt% Ni-based catalyst supported on ITQ-6 zeolite (Si/Al = 30) exhibited catalytic results (X<sub>CO2</sub> = 79 % y S<sub>CH4</sub> = 98 %) comparable or even superior to some of the best zeolite-based catalysts reported so far.</p></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-06-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0021951724003221/pdfft?md5=c6ce5261012d81e2ef7f5ad693767328&pid=1-s2.0-S0021951724003221-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951724003221\",\"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/S0021951724003221","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
摘要
在二氧化碳和一氧化碳的甲烷化过程中，测试了在不同硅/铝比（30 和 ∞）的脱层 ITQ-6 沸石上支撑的镍基催化剂。ITQ-6 支持物显示出较高的表面积（590 m2/g），以其为基础的催化剂显示出较高的 CO2 和 CO 转化值、转化率（TOF）和 CH4 选择性（90%）。将 ITQ-6 催化剂与其前驱体铁氧体（FER）基催化剂进行比较，H2-化学吸附结果表明前者的金属分散度更高，从而提高了 H2 的吸收率，并使反应中间产物通过缔合途径有效地相互作用。综合动力学研究表明，前者更高的可用金属表面有助于降低 CH4 生成的表观活化能，从而获得更高的选择性。在 ITQ-6 沸石（Si/Al = 30）上支撑的 15 wt% Ni 基催化剂的催化效果（XCO2 = 79 % y SCH4 = 98 %）可媲美甚至优于迄今报道的一些最佳沸石基催化剂。
Enhancement of catalytic activity in CO2 methanation in Ni-based catalysts supported on delaminated ITQ-6 zeolite
Ni-based catalysts supported on delaminated ITQ-6 zeolite with different Si/Al ratios, 30 and ∞, were tested in the methanation of CO2 and CO. ITQ-6 supports exhibited high surface areas (> 590 m2/g), and the catalysts based on them presented elevated CO2 and CO conversion values, turnover frequencies (TOF), and CH4 selectivity (> 90 %). Comparing the ITQ-6 catalyst and its precursor ferrierite (FER)-based catalyst, H2-chemisorption results confirmed higher metallic dispersion for the former, which resulted in improved H2 uptake and efficient interaction of reaction intermediates via the associative pathway. Combined kinetic studies indicated that their higher available metallic surface contributed to lower apparent activation energies towards CH4 formation, accounting for the higher selectivity values. A 15 wt% Ni-based catalyst supported on ITQ-6 zeolite (Si/Al = 30) exhibited catalytic results (XCO2 = 79 % y SCH4 = 98 %) comparable or even superior to some of the best zeolite-based catalysts reported so far.
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.
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