{"title":"Investigating the role of zeolite supports in Ni-based catalysts for CO2-methanation using in situ/operando XAS–GC-MS","authors":"Waranya Obrom , Worapol Yingyuen , Tatchapol Nanmong , Krittanun Deekamwong , Pimrapus Tawachkultanadilok , Jatuporn Wittayakun , Sanchai Prayoonpokarach , Yingyot Poo-arporn , Karin Föttinger , Jean-Paul Desaulniers , Sirinuch Loiha","doi":"10.1016/j.micromeso.2025.113548","DOIUrl":null,"url":null,"abstract":"<div><div>Nickel (Ni) is regarded as the most effective non-noble metal catalyst for CO<sub>2</sub> methanation. Its performance is strongly influenced by support material and Ni reducibility. This study investigates the impact of zeolite types (ANA, LTA, and ZSM-5) on the reducibility and catalytic performance of 5 wt% Ni catalysts, compared with SiO<sub>2</sub>. Reducibility, measured via in situ X-ray absorption spectroscopy (XAS) from 100 to 450 °C, followed the order: 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/LTA > 5Ni/SiO<sub>2</sub>. Catalytic testing in a fixed-bed flow reactor revealed the highest CO<sub>2</sub> conversion at 400 °C, following the order: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/SiO<sub>2</sub>. Zeolite-supported catalysts achieved significantly higher CH<sub>4</sub> selectivity compared to 5Ni/SiO<sub>2</sub>, with the trend: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA ≫ 5Ni/SiO<sub>2</sub>. Comprehensive characterization using X-ray diffraction, N<sub>2</sub> adsorption-desorption, and X-ray photoelectron spectroscopy was conducted to analyze catalyst properties. The CO<sub>2</sub> methanation mechanism was deduced using data from in situ XAS-MS. These findings demonstrate that zeolite-supported Ni catalysts, particularly 5Ni/LTA, exhibit superior reducibility and catalytic performance, advancing the development of efficient materials for CO<sub>2</sub> conversion.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"390 ","pages":"Article 113548"},"PeriodicalIF":4.7000,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Microporous and Mesoporous Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1387181125000629","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
Abstract
Nickel (Ni) is regarded as the most effective non-noble metal catalyst for CO2 methanation. Its performance is strongly influenced by support material and Ni reducibility. This study investigates the impact of zeolite types (ANA, LTA, and ZSM-5) on the reducibility and catalytic performance of 5 wt% Ni catalysts, compared with SiO2. Reducibility, measured via in situ X-ray absorption spectroscopy (XAS) from 100 to 450 °C, followed the order: 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/LTA > 5Ni/SiO2. Catalytic testing in a fixed-bed flow reactor revealed the highest CO2 conversion at 400 °C, following the order: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/SiO2. Zeolite-supported catalysts achieved significantly higher CH4 selectivity compared to 5Ni/SiO2, with the trend: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA ≫ 5Ni/SiO2. Comprehensive characterization using X-ray diffraction, N2 adsorption-desorption, and X-ray photoelectron spectroscopy was conducted to analyze catalyst properties. The CO2 methanation mechanism was deduced using data from in situ XAS-MS. These findings demonstrate that zeolite-supported Ni catalysts, particularly 5Ni/LTA, exhibit superior reducibility and catalytic performance, advancing the development of efficient materials for CO2 conversion.
镍（Ni）被认为是CO2甲烷化最有效的非贵金属催化剂。其性能受载体材料和Ni还原性的影响较大。本研究考察了沸石类型（ANA、LTA和ZSM-5）对5 wt% Ni催化剂的还原性和催化性能的影响，并与SiO2进行了比较。通过原位x射线吸收光谱（XAS）在100至450°C范围内测量还原性，顺序为：5Ni/ZSM-5 >；5 ni /安娜比;5 ni / LTA祝辞5 ni /二氧化矽。固定床流动反应器的催化测试表明，在400°C时CO2转化率最高，顺序为：5Ni/LTA >；5 ni / ZSM-5祝辞5 ni /安娜比;5 ni /二氧化矽。与5Ni/SiO2相比，沸石负载型催化剂的CH4选择性显著提高，趋势为：5Ni/LTA >；5 ni / ZSM-5祝辞5Ni/ANA∶5Ni/SiO2。采用x射线衍射、N2吸附-解吸、x射线光电子能谱等方法对催化剂进行了综合表征。利用原位XAS-MS数据推导了CO2甲烷化机理。这些发现表明，沸石负载的Ni催化剂，特别是5Ni/LTA，具有优异的还原性和催化性能，促进了高效CO2转化材料的发展。
期刊介绍：
Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal.
Topics which are particularly of interest include:
All aspects of natural microporous and mesoporous solids
The synthesis of crystalline or amorphous porous materials
The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic
The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions
All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials
Adsorption (and other separation techniques) using microporous or mesoporous adsorbents
Catalysis by microporous and mesoporous materials
Host/guest interactions
Theoretical chemistry and modelling of host/guest interactions
All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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