{"title":"构建具有多种氧化态和金属态的匹配亚纳米钴簇,实现高效丙烷脱氢","authors":"Weihua Deng, Dedong He, Dingkai Chen, Zijun Huang, Jiguang Deng, Yongming Luo","doi":"10.1038/s43246-024-00656-4","DOIUrl":null,"url":null,"abstract":"Modulating unique microenvironment including both oxidation and metallic states on sub-nanocluster metal catalysts remains challenging, since designing heterogeneous catalysis within controllable oxidation state is necessary for achieving optimum performance. Here we construct stable sub-nano-Co clusters, which shows different microenvironment with the reported sub-nanocluster catalysts and reported Co-based catalysts. The coexistence of both ionic bonds of Co-O and metallic bonds of Co-Co shows features of multiple oxidation and metallic states, which changes the electronic orbital configuration of the individual Co atom in clusters. The specific microenvironment within low oxidation state and high electron density promotes combination of empty and filled host orbitals to yield high electron transfer between metal and propane, which exhibits higher reactivity than the reported Co-based and other non-noble metals catalysts. The desired reactivity offers the possibility for the exploitation of highly efficient non-noble metal catalysts for propane dehydrogenation in industrial applications. Designing heterogeneous catalysts with modulated microenvironments is important for optimum performance. Here, cobalt sub-nanoclusters with Co-O and Co-Co bonds show multiple oxidation and metallic states for propane dehydrogenation.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5000,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00656-4.pdf","citationCount":"0","resultStr":"{\"title\":\"Constructing matched sub-nanometric cobalt clusters with multiple oxidation and metallic states for efficient propane dehydrogenation\",\"authors\":\"Weihua Deng, Dedong He, Dingkai Chen, Zijun Huang, Jiguang Deng, Yongming Luo\",\"doi\":\"10.1038/s43246-024-00656-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Modulating unique microenvironment including both oxidation and metallic states on sub-nanocluster metal catalysts remains challenging, since designing heterogeneous catalysis within controllable oxidation state is necessary for achieving optimum performance. Here we construct stable sub-nano-Co clusters, which shows different microenvironment with the reported sub-nanocluster catalysts and reported Co-based catalysts. The coexistence of both ionic bonds of Co-O and metallic bonds of Co-Co shows features of multiple oxidation and metallic states, which changes the electronic orbital configuration of the individual Co atom in clusters. The specific microenvironment within low oxidation state and high electron density promotes combination of empty and filled host orbitals to yield high electron transfer between metal and propane, which exhibits higher reactivity than the reported Co-based and other non-noble metals catalysts. The desired reactivity offers the possibility for the exploitation of highly efficient non-noble metal catalysts for propane dehydrogenation in industrial applications. Designing heterogeneous catalysts with modulated microenvironments is important for optimum performance. Here, cobalt sub-nanoclusters with Co-O and Co-Co bonds show multiple oxidation and metallic states for propane dehydrogenation.\",\"PeriodicalId\":10589,\"journal\":{\"name\":\"Communications Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.5000,\"publicationDate\":\"2024-10-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.nature.com/articles/s43246-024-00656-4.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Communications Materials\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.nature.com/articles/s43246-024-00656-4\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Communications Materials","FirstCategoryId":"1085","ListUrlMain":"https://www.nature.com/articles/s43246-024-00656-4","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
在亚纳米簇金属催化剂上调节独特的微环境(包括氧化态和金属态)仍然具有挑战性,因为要实现最佳性能,必须在可控氧化态下设计异相催化。在这里,我们构建了稳定的亚纳米钴簇,它与已报道的亚纳米簇催化剂和已报道的钴基催化剂显示出不同的微环境。Co-O 的离子键和 Co-Co 的金属键共存,显示出多重氧化态和金属态的特征,从而改变了团簇中单个 Co 原子的电子轨道构型。低氧化态和高电子密度的特定微环境促进了空的和填充的主轨道的结合,从而在金属和丙烷之间产生高电子转移,与已报道的 Co 基催化剂和其他非贵金属催化剂相比,这种催化剂具有更高的反应活性。这种理想的反应活性为在工业应用中开发用于丙烷脱氢的高效非贵金属催化剂提供了可能。设计具有可调节微环境的异相催化剂对于实现最佳性能非常重要。在这里,具有 Co-O 和 Co-Co 键的钴亚纳米团簇在丙烷脱氢过程中表现出多种氧化态和金属态。
Constructing matched sub-nanometric cobalt clusters with multiple oxidation and metallic states for efficient propane dehydrogenation
Modulating unique microenvironment including both oxidation and metallic states on sub-nanocluster metal catalysts remains challenging, since designing heterogeneous catalysis within controllable oxidation state is necessary for achieving optimum performance. Here we construct stable sub-nano-Co clusters, which shows different microenvironment with the reported sub-nanocluster catalysts and reported Co-based catalysts. The coexistence of both ionic bonds of Co-O and metallic bonds of Co-Co shows features of multiple oxidation and metallic states, which changes the electronic orbital configuration of the individual Co atom in clusters. The specific microenvironment within low oxidation state and high electron density promotes combination of empty and filled host orbitals to yield high electron transfer between metal and propane, which exhibits higher reactivity than the reported Co-based and other non-noble metals catalysts. The desired reactivity offers the possibility for the exploitation of highly efficient non-noble metal catalysts for propane dehydrogenation in industrial applications. Designing heterogeneous catalysts with modulated microenvironments is important for optimum performance. Here, cobalt sub-nanoclusters with Co-O and Co-Co bonds show multiple oxidation and metallic states for propane dehydrogenation.
期刊介绍:
Communications Materials, a selective open access journal within Nature Portfolio, is dedicated to publishing top-tier research, reviews, and commentary across all facets of materials science. The journal showcases significant advancements in specialized research areas, encompassing both fundamental and applied studies. Serving as an open access option for materials sciences, Communications Materials applies less stringent criteria for impact and significance compared to Nature-branded journals, including Nature Communications.