Yifan Wei , Jingyi Liu , Hanbo Li , Xian Zhang , Ying Zhang , Jiangong Yang , Mingpei Wang , Zhen Liu , Zifeng Yan
{"title":"CuZnAl包埋硅铝酸盐催化剂促进二氧化碳加氢制二甲醚","authors":"Yifan Wei , Jingyi Liu , Hanbo Li , Xian Zhang , Ying Zhang , Jiangong Yang , Mingpei Wang , Zhen Liu , Zifeng Yan","doi":"10.1016/j.apcata.2025.120286","DOIUrl":null,"url":null,"abstract":"<div><div>The resource utilization of CO<sub>2</sub> serves as a feasible method for emission reduction and the establishment of an artificial carbon cycle. This study primarily focuses on the direct synthesis of dimethyl ether (DME) from the hydrogenation of CO<sub>2</sub>. We have prepared bifunctional catalysts with metal oxides embedded in amorphous silicon-aluminum by an improved Stöber method. By precisely adjusting the Si/Al molar ratio and the CTAB/Si molar ratio in the synthesis precursor solution, structural characteristics and acid properties of the catalyst could be effectively regulated. The results indicated that compared to Cu/ZnO/Al<sub>2</sub>O<sub>3</sub>, the catalyst significantly enhanced the selectivity of DME and methanol (MeOH), reduced the selectivity of CO with a moderate conversion rate of CO<sub>2</sub>. The highest DME selectivity of 37.94 % was achieved at an Si/Al ratio of 8, with the total selectivity for methanol and DME reaching 52.96 %. The addition of cetyltrimethylammonium bromide (CTAB) increased the proportion of Brønsted acid sites and medium-strong acid sites, thereby enhancing methanol dehydration and suppressing the reverse water-gas shift reaction. The optimal selectivity for DME of 43 % was obtained over catalyst prepared with a CTAB/Si molar ratio of 0.1. This study provides a new strategy for the structural design of bifunctional catalysts for CO<sub>2</sub> hydrogenation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"700 ","pages":"Article 120286"},"PeriodicalIF":4.7000,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"CuZnAl embedded silicoaluminate catalyst promotion for the hydrogenation of carbon dioxide to dimethyl ether\",\"authors\":\"Yifan Wei , Jingyi Liu , Hanbo Li , Xian Zhang , Ying Zhang , Jiangong Yang , Mingpei Wang , Zhen Liu , Zifeng Yan\",\"doi\":\"10.1016/j.apcata.2025.120286\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The resource utilization of CO<sub>2</sub> serves as a feasible method for emission reduction and the establishment of an artificial carbon cycle. This study primarily focuses on the direct synthesis of dimethyl ether (DME) from the hydrogenation of CO<sub>2</sub>. We have prepared bifunctional catalysts with metal oxides embedded in amorphous silicon-aluminum by an improved Stöber method. By precisely adjusting the Si/Al molar ratio and the CTAB/Si molar ratio in the synthesis precursor solution, structural characteristics and acid properties of the catalyst could be effectively regulated. The results indicated that compared to Cu/ZnO/Al<sub>2</sub>O<sub>3</sub>, the catalyst significantly enhanced the selectivity of DME and methanol (MeOH), reduced the selectivity of CO with a moderate conversion rate of CO<sub>2</sub>. The highest DME selectivity of 37.94 % was achieved at an Si/Al ratio of 8, with the total selectivity for methanol and DME reaching 52.96 %. The addition of cetyltrimethylammonium bromide (CTAB) increased the proportion of Brønsted acid sites and medium-strong acid sites, thereby enhancing methanol dehydration and suppressing the reverse water-gas shift reaction. The optimal selectivity for DME of 43 % was obtained over catalyst prepared with a CTAB/Si molar ratio of 0.1. This study provides a new strategy for the structural design of bifunctional catalysts for CO<sub>2</sub> hydrogenation.</div></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"700 \",\"pages\":\"Article 120286\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2025-04-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X25001875\",\"RegionNum\":2,\"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":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X25001875","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
CuZnAl embedded silicoaluminate catalyst promotion for the hydrogenation of carbon dioxide to dimethyl ether
The resource utilization of CO2 serves as a feasible method for emission reduction and the establishment of an artificial carbon cycle. This study primarily focuses on the direct synthesis of dimethyl ether (DME) from the hydrogenation of CO2. We have prepared bifunctional catalysts with metal oxides embedded in amorphous silicon-aluminum by an improved Stöber method. By precisely adjusting the Si/Al molar ratio and the CTAB/Si molar ratio in the synthesis precursor solution, structural characteristics and acid properties of the catalyst could be effectively regulated. The results indicated that compared to Cu/ZnO/Al2O3, the catalyst significantly enhanced the selectivity of DME and methanol (MeOH), reduced the selectivity of CO with a moderate conversion rate of CO2. The highest DME selectivity of 37.94 % was achieved at an Si/Al ratio of 8, with the total selectivity for methanol and DME reaching 52.96 %. The addition of cetyltrimethylammonium bromide (CTAB) increased the proportion of Brønsted acid sites and medium-strong acid sites, thereby enhancing methanol dehydration and suppressing the reverse water-gas shift reaction. The optimal selectivity for DME of 43 % was obtained over catalyst prepared with a CTAB/Si molar ratio of 0.1. This study provides a new strategy for the structural design of bifunctional catalysts for CO2 hydrogenation.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.