{"title":"从合成气中合成低碳醇的 Cu 复合阴离子对 CuZnAl 插层类氢铝铁矿催化剂的影响","authors":"Shuyuan Wang, Zhe Hong, Lingling Yin, Zhihua Gao, Wei Huang","doi":"10.1016/j.apcata.2024.119822","DOIUrl":null,"url":null,"abstract":"<div><p>Elucidating the structure-performance relationship of catalysts for low-carbon alcohols synthesis from syngas is crucial for designing efficient catalysts. In this study, CuO particle size, reducibility, and the number of oxygen vacancies could be adjusted by changing intercalated Cu complex anions, thereby affecting the catalyst's performance. The characterization results indicated that the insertion of [Cu(C<sub>2</sub>O<sub>4</sub>)<sub>2</sub>]<sup>2-</sup> between ZnAl layered double hydroxide resulted in the largest CuO particles (26.5 nm), leading to an increase in the metallic copper surface area. Consequently, the highest CO conversion (13.0 %) was achieved without altering alcohol distribution. On the other hand, when [Cu(EDTA)]<sup>2-</sup> was inserted, the catalyst possessed the smallest CuO particle size (8.9 nm), more abundant oxygen vacancies, and enhanced interaction between Cu species and ZnO, which promoted carbon chain growth and resulted in a high C<sub>2+</sub>OH proportion of 75.8 %. Our study thus provides a new perspective on catalyst structures for the syngas production of low-carbon alcohols.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7000,"publicationDate":"2024-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Impact of Cu complex anions on CuZnAl intercalated hydrotalcite-like catalysts for low-carbon alcohols synthesis from syngas\",\"authors\":\"Shuyuan Wang, Zhe Hong, Lingling Yin, Zhihua Gao, Wei Huang\",\"doi\":\"10.1016/j.apcata.2024.119822\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Elucidating the structure-performance relationship of catalysts for low-carbon alcohols synthesis from syngas is crucial for designing efficient catalysts. In this study, CuO particle size, reducibility, and the number of oxygen vacancies could be adjusted by changing intercalated Cu complex anions, thereby affecting the catalyst's performance. The characterization results indicated that the insertion of [Cu(C<sub>2</sub>O<sub>4</sub>)<sub>2</sub>]<sup>2-</sup> between ZnAl layered double hydroxide resulted in the largest CuO particles (26.5 nm), leading to an increase in the metallic copper surface area. Consequently, the highest CO conversion (13.0 %) was achieved without altering alcohol distribution. On the other hand, when [Cu(EDTA)]<sup>2-</sup> was inserted, the catalyst possessed the smallest CuO particle size (8.9 nm), more abundant oxygen vacancies, and enhanced interaction between Cu species and ZnO, which promoted carbon chain growth and resulted in a high C<sub>2+</sub>OH proportion of 75.8 %. Our study thus provides a new perspective on catalyst structures for the syngas production of low-carbon alcohols.</p></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-05-27\",\"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/S0926860X24002679\",\"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/S0926860X24002679","RegionNum":2,"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
阐明合成气合成低碳醇催化剂的结构性能关系对于设计高效催化剂至关重要。在本研究中,可以通过改变插层 Cu 复合阴离子来调整 CuO 的粒度、还原性和氧空位的数量,从而影响催化剂的性能。表征结果表明,在 ZnAl 层状双氢氧化物之间插入 [Cu(C2O4)2]2- 会产生最大的 CuO 颗粒(26.5 nm),从而增加金属铜的表面积。因此,在不改变醇分布的情况下,实现了最高的 CO 转化率(13.0%)。另一方面,当加入[Cu(EDTA)]2-时,催化剂具有最小的 CuO 粒径(8.9 nm)、更丰富的氧空位以及 Cu 物种与 ZnO 之间更强的相互作用,这促进了碳链的增长,并使 C2+OH 的比例高达 75.8%。因此,我们的研究为低碳醇合成气生产的催化剂结构提供了一个新的视角。
Impact of Cu complex anions on CuZnAl intercalated hydrotalcite-like catalysts for low-carbon alcohols synthesis from syngas
Elucidating the structure-performance relationship of catalysts for low-carbon alcohols synthesis from syngas is crucial for designing efficient catalysts. In this study, CuO particle size, reducibility, and the number of oxygen vacancies could be adjusted by changing intercalated Cu complex anions, thereby affecting the catalyst's performance. The characterization results indicated that the insertion of [Cu(C2O4)2]2- between ZnAl layered double hydroxide resulted in the largest CuO particles (26.5 nm), leading to an increase in the metallic copper surface area. Consequently, the highest CO conversion (13.0 %) was achieved without altering alcohol distribution. On the other hand, when [Cu(EDTA)]2- was inserted, the catalyst possessed the smallest CuO particle size (8.9 nm), more abundant oxygen vacancies, and enhanced interaction between Cu species and ZnO, which promoted carbon chain growth and resulted in a high C2+OH proportion of 75.8 %. Our study thus provides a new perspective on catalyst structures for the syngas production of low-carbon alcohols.
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.