{"title":"用于串联转化合成气为乙醇的双金属氧化物界面的原子紧密装配","authors":"Shang Li, Li Feng, Hengwei Wang, Yue Lin, Zhihu Sun, Lulu Xu, Yuxing Xu, Xinyu Liu, Wei-Xue Li, Shiqiang Wei, Jin-Xun Liu, Junling Lu","doi":"10.1038/s41565-024-01824-w","DOIUrl":null,"url":null,"abstract":"<p>Selective conversion of syngas to value-added higher alcohols (containing two or more carbon atoms), particularly to a specific alcohol, is of great interest but remains challenging. Here we show that atomically intimate assembly of FeO<sub><i>x</i></sub>-Rh-ZrO<sub>2</sub> dual interfaces by selectively architecting highly dispersed FeO<sub><i>x</i></sub> on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol. The ethanol selectivity in oxygenates reached ~90% at CO conversion up to 51%, along with a markedly high space-time yield of ethanol of 668.2 mg g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>. In situ spectroscopic characterization and theoretical calculations reveal that Rh-ZrO<sub>2</sub> interface promotes dissociative CO activation into CH<sub><i>x</i></sub> through a formate pathway, while the adjacent Rh-FeO<sub><i>x</i></sub> interface accelerates subsequent C–C coupling via nondissociative CO insertion. Consequently, these dual interfaces in atomic-scale proximity with complementary functionalities synergistically boost the exclusive formation of ethanol with exceptional productivity in a tandem manner.</p>","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"80 1","pages":""},"PeriodicalIF":38.1000,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Atomically intimate assembly of dual metal–oxide interfaces for tandem conversion of syngas to ethanol\",\"authors\":\"Shang Li, Li Feng, Hengwei Wang, Yue Lin, Zhihu Sun, Lulu Xu, Yuxing Xu, Xinyu Liu, Wei-Xue Li, Shiqiang Wei, Jin-Xun Liu, Junling Lu\",\"doi\":\"10.1038/s41565-024-01824-w\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Selective conversion of syngas to value-added higher alcohols (containing two or more carbon atoms), particularly to a specific alcohol, is of great interest but remains challenging. Here we show that atomically intimate assembly of FeO<sub><i>x</i></sub>-Rh-ZrO<sub>2</sub> dual interfaces by selectively architecting highly dispersed FeO<sub><i>x</i></sub> on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol. The ethanol selectivity in oxygenates reached ~90% at CO conversion up to 51%, along with a markedly high space-time yield of ethanol of 668.2 mg g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>. In situ spectroscopic characterization and theoretical calculations reveal that Rh-ZrO<sub>2</sub> interface promotes dissociative CO activation into CH<sub><i>x</i></sub> through a formate pathway, while the adjacent Rh-FeO<sub><i>x</i></sub> interface accelerates subsequent C–C coupling via nondissociative CO insertion. Consequently, these dual interfaces in atomic-scale proximity with complementary functionalities synergistically boost the exclusive formation of ethanol with exceptional productivity in a tandem manner.</p>\",\"PeriodicalId\":18915,\"journal\":{\"name\":\"Nature nanotechnology\",\"volume\":\"80 1\",\"pages\":\"\"},\"PeriodicalIF\":38.1000,\"publicationDate\":\"2024-11-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature nanotechnology\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1038/s41565-024-01824-w\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature nanotechnology","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1038/s41565-024-01824-w","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Atomically intimate assembly of dual metal–oxide interfaces for tandem conversion of syngas to ethanol
Selective conversion of syngas to value-added higher alcohols (containing two or more carbon atoms), particularly to a specific alcohol, is of great interest but remains challenging. Here we show that atomically intimate assembly of FeOx-Rh-ZrO2 dual interfaces by selectively architecting highly dispersed FeOx on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol. The ethanol selectivity in oxygenates reached ~90% at CO conversion up to 51%, along with a markedly high space-time yield of ethanol of 668.2 mg gcat−1 h−1. In situ spectroscopic characterization and theoretical calculations reveal that Rh-ZrO2 interface promotes dissociative CO activation into CHx through a formate pathway, while the adjacent Rh-FeOx interface accelerates subsequent C–C coupling via nondissociative CO insertion. Consequently, these dual interfaces in atomic-scale proximity with complementary functionalities synergistically boost the exclusive formation of ethanol with exceptional productivity in a tandem manner.
期刊介绍：
Nature Nanotechnology is a prestigious journal that publishes high-quality papers in various areas of nanoscience and nanotechnology. The journal focuses on the design, characterization, and production of structures, devices, and systems that manipulate and control materials at atomic, molecular, and macromolecular scales. It encompasses both bottom-up and top-down approaches, as well as their combinations.
Furthermore, Nature Nanotechnology fosters the exchange of ideas among researchers from diverse disciplines such as chemistry, physics, material science, biomedical research, engineering, and more. It promotes collaboration at the forefront of this multidisciplinary field. The journal covers a wide range of topics, from fundamental research in physics, chemistry, and biology, including computational work and simulations, to the development of innovative devices and technologies for various industrial sectors such as information technology, medicine, manufacturing, high-performance materials, energy, and environmental technologies. It includes coverage of organic, inorganic, and hybrid materials.
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