Nasir Shezad , Muddasar Safdar , Harvey Arellano-García , Cheuk-Wai Tai , Shaojiang Chen , Dong-Kyun Seo , Shujie You , Alberto Vomiero , Farid Akhtar
{"title":"破译APTES在调整NiO纳米层在13X沸石上的金属支撑相互作用中对CO2甲烷化的作用","authors":"Nasir Shezad , Muddasar Safdar , Harvey Arellano-García , Cheuk-Wai Tai , Shaojiang Chen , Dong-Kyun Seo , Shujie You , Alberto Vomiero , Farid Akhtar","doi":"10.1016/j.ccst.2025.100424","DOIUrl":null,"url":null,"abstract":"<div><div>The development of robust nickel catalysts on porous substrates offers great potential for converting carbon dioxide (CO<sub>2</sub>) into methane, thereby helping to address the global warming and sustainability challenges. This study investigates the dispersion and stability of Ni nanolayers by grafting bifunctional groups over the hierarchical zeolite 13X (h13X) support using (3-aminopropyl)triethoxysilane (APTES). The Ni nanolayers, with a thickness of 1.5–7 nm, were deposited around the edges of h13X and analyzed using STEM imaging. A clear shift in the binding energies was observed by XPS analysis, substantiating the enhanced metal-support interaction (MSI) between NiO and h13X. The influence of reaction temperature on APTES incorporation into h13X was revealed by H<sub>2</sub>-TPR and CO<sub>2</sub>-TPD, with notable variations in the reducibility and surface basicity profiles of the catalysts. The optimized catalyst exhibited CO<sub>2</sub> conversion of 61 % with CH<sub>4</sub> selectivity of 97 % under GHSV of 60,000 mlg<sub>Cat</sub><sup>-1</sup>h<sup>-1</sup> at 400 °C and 1 bar and demonstrated robust stability over a period of 150 h without discernible degradation. The enhanced performance could be attributed to the strengthened MSI and reduced size of Ni nanolayers over h13X. These findings highlight the development of robust heterogeneous catalysts by changing the surface chemistry of support material for various catalytic applications.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"15 ","pages":"Article 100424"},"PeriodicalIF":0.0000,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Deciphering the role of APTES in tuning the metal support interaction of NiO nanolayers over hierarchical zeolite 13X for CO2 methanation\",\"authors\":\"Nasir Shezad , Muddasar Safdar , Harvey Arellano-García , Cheuk-Wai Tai , Shaojiang Chen , Dong-Kyun Seo , Shujie You , Alberto Vomiero , Farid Akhtar\",\"doi\":\"10.1016/j.ccst.2025.100424\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The development of robust nickel catalysts on porous substrates offers great potential for converting carbon dioxide (CO<sub>2</sub>) into methane, thereby helping to address the global warming and sustainability challenges. This study investigates the dispersion and stability of Ni nanolayers by grafting bifunctional groups over the hierarchical zeolite 13X (h13X) support using (3-aminopropyl)triethoxysilane (APTES). The Ni nanolayers, with a thickness of 1.5–7 nm, were deposited around the edges of h13X and analyzed using STEM imaging. A clear shift in the binding energies was observed by XPS analysis, substantiating the enhanced metal-support interaction (MSI) between NiO and h13X. The influence of reaction temperature on APTES incorporation into h13X was revealed by H<sub>2</sub>-TPR and CO<sub>2</sub>-TPD, with notable variations in the reducibility and surface basicity profiles of the catalysts. The optimized catalyst exhibited CO<sub>2</sub> conversion of 61 % with CH<sub>4</sub> selectivity of 97 % under GHSV of 60,000 mlg<sub>Cat</sub><sup>-1</sup>h<sup>-1</sup> at 400 °C and 1 bar and demonstrated robust stability over a period of 150 h without discernible degradation. The enhanced performance could be attributed to the strengthened MSI and reduced size of Ni nanolayers over h13X. These findings highlight the development of robust heterogeneous catalysts by changing the surface chemistry of support material for various catalytic applications.</div></div>\",\"PeriodicalId\":9387,\"journal\":{\"name\":\"Carbon Capture Science & Technology\",\"volume\":\"15 \",\"pages\":\"Article 100424\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-04-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Carbon Capture Science & Technology\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2772656825000636\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Capture Science & Technology","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2772656825000636","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Deciphering the role of APTES in tuning the metal support interaction of NiO nanolayers over hierarchical zeolite 13X for CO2 methanation
The development of robust nickel catalysts on porous substrates offers great potential for converting carbon dioxide (CO2) into methane, thereby helping to address the global warming and sustainability challenges. This study investigates the dispersion and stability of Ni nanolayers by grafting bifunctional groups over the hierarchical zeolite 13X (h13X) support using (3-aminopropyl)triethoxysilane (APTES). The Ni nanolayers, with a thickness of 1.5–7 nm, were deposited around the edges of h13X and analyzed using STEM imaging. A clear shift in the binding energies was observed by XPS analysis, substantiating the enhanced metal-support interaction (MSI) between NiO and h13X. The influence of reaction temperature on APTES incorporation into h13X was revealed by H2-TPR and CO2-TPD, with notable variations in the reducibility and surface basicity profiles of the catalysts. The optimized catalyst exhibited CO2 conversion of 61 % with CH4 selectivity of 97 % under GHSV of 60,000 mlgCat-1h-1 at 400 °C and 1 bar and demonstrated robust stability over a period of 150 h without discernible degradation. The enhanced performance could be attributed to the strengthened MSI and reduced size of Ni nanolayers over h13X. These findings highlight the development of robust heterogeneous catalysts by changing the surface chemistry of support material for various catalytic applications.