Xinyu Yang , Long Lin , Xiangyu Guo , Shengli Zhang
{"title":"基于导电 1T-HfTe2 的具有阴离子中心的单原子氧电催化催化剂","authors":"Xinyu Yang , Long Lin , Xiangyu Guo , Shengli Zhang","doi":"10.1016/j.jcat.2024.115548","DOIUrl":null,"url":null,"abstract":"<div><p>Advancing efficient catalysts for oxygen reduction reaction (ORR) or oxygen evolution reaction (OER) is imperative for commercializing emerging energy devices. Using density functional theory (DFT) calculations, we propose doping different transition metal (TM) atoms to regulate the electronic structures of the two-dimensional 1T-HfTe<sub>2</sub> monolayer to achieve bifunctional catalysis for the ORR/OER. Due to the small electronegativity of the Hf atom, we found the doped TM atoms can generally form anion centers by accepting abundant charges from the Hf interlayer. At the same time, the highly conductive 1T-HfTe<sub>2</sub> contributes to the charge transfer between the active center and the reaction intermediates, rendering the designed SACs the tunable activity for the reactions. By comparing the theoretical overpotentials of ORR and OER on 15 single-atom catalysts (SACs), Pt-doped system exhibits excellent catalytic activity for both ORR and OER, outperforming the traditional Pt(1<!--> <!-->1<!--> <!-->1) and RuO<sub>2</sub>(1<!--> <!-->1<!--> <!-->0) catalysts. Based on the charge transfer mechanism, we clarified that the doped TM atoms act as a ‘bridge’ to transfer the electrons from the substrate to the reaction intermediates, thereby effectively contributing to the improvement of catalytic activity. In summary, our study shows that, by doping appropriate TM atoms, the intrinsic inert HfTe<sub>2</sub> can be activated toward efficient ORR/OER. This could provide some guidance for the design of new two-dimensional ORR/OER bifunctional catalyst materials.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0021951724002616/pdfft?md5=6a9e24bd10734cff9aaf3c7704889d90&pid=1-s2.0-S0021951724002616-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Single atom catalysts with anion center toward oxygen electrocatalysis based on the conductive 1T-HfTe2\",\"authors\":\"Xinyu Yang , Long Lin , Xiangyu Guo , Shengli Zhang\",\"doi\":\"10.1016/j.jcat.2024.115548\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Advancing efficient catalysts for oxygen reduction reaction (ORR) or oxygen evolution reaction (OER) is imperative for commercializing emerging energy devices. Using density functional theory (DFT) calculations, we propose doping different transition metal (TM) atoms to regulate the electronic structures of the two-dimensional 1T-HfTe<sub>2</sub> monolayer to achieve bifunctional catalysis for the ORR/OER. Due to the small electronegativity of the Hf atom, we found the doped TM atoms can generally form anion centers by accepting abundant charges from the Hf interlayer. At the same time, the highly conductive 1T-HfTe<sub>2</sub> contributes to the charge transfer between the active center and the reaction intermediates, rendering the designed SACs the tunable activity for the reactions. By comparing the theoretical overpotentials of ORR and OER on 15 single-atom catalysts (SACs), Pt-doped system exhibits excellent catalytic activity for both ORR and OER, outperforming the traditional Pt(1<!--> <!-->1<!--> <!-->1) and RuO<sub>2</sub>(1<!--> <!-->1<!--> <!-->0) catalysts. Based on the charge transfer mechanism, we clarified that the doped TM atoms act as a ‘bridge’ to transfer the electrons from the substrate to the reaction intermediates, thereby effectively contributing to the improvement of catalytic activity. In summary, our study shows that, by doping appropriate TM atoms, the intrinsic inert HfTe<sub>2</sub> can be activated toward efficient ORR/OER. This could provide some guidance for the design of new two-dimensional ORR/OER bifunctional catalyst materials.</p></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-05-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0021951724002616/pdfft?md5=6a9e24bd10734cff9aaf3c7704889d90&pid=1-s2.0-S0021951724002616-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951724002616\",\"RegionNum\":1,\"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":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951724002616","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Single atom catalysts with anion center toward oxygen electrocatalysis based on the conductive 1T-HfTe2
Advancing efficient catalysts for oxygen reduction reaction (ORR) or oxygen evolution reaction (OER) is imperative for commercializing emerging energy devices. Using density functional theory (DFT) calculations, we propose doping different transition metal (TM) atoms to regulate the electronic structures of the two-dimensional 1T-HfTe2 monolayer to achieve bifunctional catalysis for the ORR/OER. Due to the small electronegativity of the Hf atom, we found the doped TM atoms can generally form anion centers by accepting abundant charges from the Hf interlayer. At the same time, the highly conductive 1T-HfTe2 contributes to the charge transfer between the active center and the reaction intermediates, rendering the designed SACs the tunable activity for the reactions. By comparing the theoretical overpotentials of ORR and OER on 15 single-atom catalysts (SACs), Pt-doped system exhibits excellent catalytic activity for both ORR and OER, outperforming the traditional Pt(1 1 1) and RuO2(1 1 0) catalysts. Based on the charge transfer mechanism, we clarified that the doped TM atoms act as a ‘bridge’ to transfer the electrons from the substrate to the reaction intermediates, thereby effectively contributing to the improvement of catalytic activity. In summary, our study shows that, by doping appropriate TM atoms, the intrinsic inert HfTe2 can be activated toward efficient ORR/OER. This could provide some guidance for the design of new two-dimensional ORR/OER bifunctional catalyst materials.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.