{"title":"揭示催化剂的非微观拓扑表面态,实现二氧化碳的有效光化学转化","authors":"Kangwang Wang, Longfu Li, Peifeng Yu, Nannan Tang, Lingyong Zeng, Kuan Li, Chao Zhang, Rui Chen, Zaichen Xiang, Huichao Wang, Yongqing Cai, Kai Yan, Huixia Luo","doi":"arxiv-2408.11373","DOIUrl":null,"url":null,"abstract":"Topological semimetals with protected surface states mark a new paradigm of\nresearch beyond the early landmarks of band-structure engineering, allowing\nfabrication of efficient catalyst to harness the rich metallic surface states\nto activate specific chemical processes. Herein, we demonstrate a facile\nsolid-phase method for in-situ doping of Ir at the Os sites in the Os3Sn7, an\nalloy with topological states, which significantly improves the photocatalytic\nperformance for the reduction of CO2 to CO and CH4. Experimental evidence\ncombined with theoretical calculations reveal that the nontrivial topological\nsurface states greatly accelerate charge-separation/electron-enrichment and\nadsorption/activation of CO2 molecules, rendering highly efficient reaction\nchannels to stimulate the formation of *COOH and *CO, as well CHO*. This work\nshows the promise of achieving high photocatalytic performances with\nsynthesizing topological catalysts and provides hints on the design of novel\ntopological catalysts with superior photoactivity towards the CO2 reduction\nreaction.","PeriodicalId":501211,"journal":{"name":"arXiv - PHYS - Other Condensed Matter","volume":"22 1","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Revealing the nontrivial topological surface states of catalysts for effective photochemical carbon dioxide conversion\",\"authors\":\"Kangwang Wang, Longfu Li, Peifeng Yu, Nannan Tang, Lingyong Zeng, Kuan Li, Chao Zhang, Rui Chen, Zaichen Xiang, Huichao Wang, Yongqing Cai, Kai Yan, Huixia Luo\",\"doi\":\"arxiv-2408.11373\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Topological semimetals with protected surface states mark a new paradigm of\\nresearch beyond the early landmarks of band-structure engineering, allowing\\nfabrication of efficient catalyst to harness the rich metallic surface states\\nto activate specific chemical processes. Herein, we demonstrate a facile\\nsolid-phase method for in-situ doping of Ir at the Os sites in the Os3Sn7, an\\nalloy with topological states, which significantly improves the photocatalytic\\nperformance for the reduction of CO2 to CO and CH4. Experimental evidence\\ncombined with theoretical calculations reveal that the nontrivial topological\\nsurface states greatly accelerate charge-separation/electron-enrichment and\\nadsorption/activation of CO2 molecules, rendering highly efficient reaction\\nchannels to stimulate the formation of *COOH and *CO, as well CHO*. This work\\nshows the promise of achieving high photocatalytic performances with\\nsynthesizing topological catalysts and provides hints on the design of novel\\ntopological catalysts with superior photoactivity towards the CO2 reduction\\nreaction.\",\"PeriodicalId\":501211,\"journal\":{\"name\":\"arXiv - PHYS - Other Condensed Matter\",\"volume\":\"22 1\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-08-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"arXiv - PHYS - Other Condensed Matter\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/arxiv-2408.11373\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"arXiv - PHYS - Other Condensed Matter","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/arxiv-2408.11373","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
摘要
具有受保护表面态的拓扑半金属标志着一个超越早期带状结构工程研究的新范例,它允许制造高效催化剂,利用丰富的金属表面态激活特定的化学过程。在本文中,我们展示了一种在 Os3Sn7 合金的 Os 位点原位掺杂 Ir 的固相简便方法,该方法具有拓扑态,可显著提高将 CO2 还原成 CO 和 CH4 的光催化性能。实验证据与理论计算相结合表明,非对称的拓扑表面态大大加快了电荷分离/电子富集和二氧化碳分子的吸附/活化,从而提供了高效的反应通道,促进*COOH和*CO以及CHO*的形成。该研究表明,合成拓扑催化剂有望实现高光催化性能,并为设计具有优异光活性的新型拓扑催化剂提供了线索,从而实现二氧化碳还原反应。
Revealing the nontrivial topological surface states of catalysts for effective photochemical carbon dioxide conversion
Topological semimetals with protected surface states mark a new paradigm of
research beyond the early landmarks of band-structure engineering, allowing
fabrication of efficient catalyst to harness the rich metallic surface states
to activate specific chemical processes. Herein, we demonstrate a facile
solid-phase method for in-situ doping of Ir at the Os sites in the Os3Sn7, an
alloy with topological states, which significantly improves the photocatalytic
performance for the reduction of CO2 to CO and CH4. Experimental evidence
combined with theoretical calculations reveal that the nontrivial topological
surface states greatly accelerate charge-separation/electron-enrichment and
adsorption/activation of CO2 molecules, rendering highly efficient reaction
channels to stimulate the formation of *COOH and *CO, as well CHO*. This work
shows the promise of achieving high photocatalytic performances with
synthesizing topological catalysts and provides hints on the design of novel
topological catalysts with superior photoactivity towards the CO2 reduction
reaction.