{"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":"10.1016/j.apcatb.2024.124428","DOIUrl":null,"url":null,"abstract":"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 OsSn, an alloy with topological states, which significantly improves the photocatalytic performance for the reduction of CO to CO and CH. Experimental evidence combined with theoretical calculations reveal that the nontrivial topological surface states greatly accelerate charge-separation/electron-enrichment and adsorption/activation of CO 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 CO reduction reaction.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"44 1","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2024-07-20","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\":\"10.1016/j.apcatb.2024.124428\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"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 OsSn, an alloy with topological states, which significantly improves the photocatalytic performance for the reduction of CO to CO and CH. Experimental evidence combined with theoretical calculations reveal that the nontrivial topological surface states greatly accelerate charge-separation/electron-enrichment and adsorption/activation of CO 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 CO reduction reaction.\",\"PeriodicalId\":516528,\"journal\":{\"name\":\"Applied Catalysis B: Environment and Energy\",\"volume\":\"44 1\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-07-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis B: Environment and Energy\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1016/j.apcatb.2024.124428\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis B: Environment and Energy","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1016/j.apcatb.2024.124428","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超越带状结构工程早期里程碑的一种新的研究范式,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。在此,我们展示了一种在具有拓扑态的合金 OsSn 的 Os 位点原位掺杂 Ir 的简便固相方法,该方法显著提高了将 CO 还原成 CO 和 CH 的光催化性能。实验证据与理论计算相结合,揭示了非难拓扑表面态极大地加速了电荷分离/电子富集和 CO 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。这项工作表明,合成拓扑催化剂有望实现较高的光催化性能,并为设计具有优异光活性的新型拓扑催化剂提供了线索。
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 OsSn, an alloy with topological states, which significantly improves the photocatalytic performance for the reduction of CO to CO and CH. Experimental evidence combined with theoretical calculations reveal that the nontrivial topological surface states greatly accelerate charge-separation/electron-enrichment and adsorption/activation of CO 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 CO reduction reaction.