{"title":"在 Cu-C24N24 单原子催化剂上进行 H2O2 电合成的第一性原理研究","authors":"","doi":"10.1016/j.mcat.2024.114520","DOIUrl":null,"url":null,"abstract":"<div><p>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is an important chemical. The direct synthesis of H<sub>2</sub>O<sub>2</sub> has been identified as an environmentally friendly process through the two-electron oxygen reduction reaction (2e<sup>-</sup> ORR) under acidic conditions. Nevertheless, the reliance of this technique on expensive electrocatalysts derived from precious metals significantly impedes its practicality for large-scale industrial application. In our study, based on density functional theory calculations, we prove that Cu-modified C<sub>24</sub>N<sub>24</sub> (Cu-C<sub>24</sub>N<sub>24</sub>) single-atom catalyst (SAC) is an efficient electrocatalyst based on non-noble metals for 2e<sup>-</sup> ORR. The results show that Cu-C<sub>24</sub>N<sub>24</sub>, Pd-C<sub>24</sub>N<sub>24</sub>, Pt-C<sub>24</sub>N<sub>24</sub>, and Rh-C<sub>24</sub>N<sub>24</sub> possess good stability. In addition, the Cu-C<sub>24</sub>N<sub>24</sub> SAC exhibits an ideal OOH* binding energy of 4.26 eV, leading to a notably optimal catalytic activity for 2e<sup>-</sup> ORR. What is more, the Cu-C<sub>24</sub>N<sub>24</sub> SAC shows a preference for aiding in H<sub>2</sub>O<sub>2</sub> production over the rival 4e<sup>-</sup> ORR with an overpotential of merely 0.04 V. Given these desirable properties, the Cu-C<sub>24</sub>N<sub>24</sub> SAC emerges as a promising option for facilitating 2e<sup>-</sup> ORR.</p></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":null,"pages":null},"PeriodicalIF":3.9000,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"First-Principles investigation of H2O2 electrosynthesis on Cu-C24N24 single-atom catalyst\",\"authors\":\"\",\"doi\":\"10.1016/j.mcat.2024.114520\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is an important chemical. The direct synthesis of H<sub>2</sub>O<sub>2</sub> has been identified as an environmentally friendly process through the two-electron oxygen reduction reaction (2e<sup>-</sup> ORR) under acidic conditions. Nevertheless, the reliance of this technique on expensive electrocatalysts derived from precious metals significantly impedes its practicality for large-scale industrial application. In our study, based on density functional theory calculations, we prove that Cu-modified C<sub>24</sub>N<sub>24</sub> (Cu-C<sub>24</sub>N<sub>24</sub>) single-atom catalyst (SAC) is an efficient electrocatalyst based on non-noble metals for 2e<sup>-</sup> ORR. The results show that Cu-C<sub>24</sub>N<sub>24</sub>, Pd-C<sub>24</sub>N<sub>24</sub>, Pt-C<sub>24</sub>N<sub>24</sub>, and Rh-C<sub>24</sub>N<sub>24</sub> possess good stability. In addition, the Cu-C<sub>24</sub>N<sub>24</sub> SAC exhibits an ideal OOH* binding energy of 4.26 eV, leading to a notably optimal catalytic activity for 2e<sup>-</sup> ORR. What is more, the Cu-C<sub>24</sub>N<sub>24</sub> SAC shows a preference for aiding in H<sub>2</sub>O<sub>2</sub> production over the rival 4e<sup>-</sup> ORR with an overpotential of merely 0.04 V. Given these desirable properties, the Cu-C<sub>24</sub>N<sub>24</sub> SAC emerges as a promising option for facilitating 2e<sup>-</sup> ORR.</p></div>\",\"PeriodicalId\":393,\"journal\":{\"name\":\"Molecular Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2024-09-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Molecular Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468823124007028\",\"RegionNum\":2,\"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":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823124007028","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
First-Principles investigation of H2O2 electrosynthesis on Cu-C24N24 single-atom catalyst
Hydrogen peroxide (H2O2) is an important chemical. The direct synthesis of H2O2 has been identified as an environmentally friendly process through the two-electron oxygen reduction reaction (2e- ORR) under acidic conditions. Nevertheless, the reliance of this technique on expensive electrocatalysts derived from precious metals significantly impedes its practicality for large-scale industrial application. In our study, based on density functional theory calculations, we prove that Cu-modified C24N24 (Cu-C24N24) single-atom catalyst (SAC) is an efficient electrocatalyst based on non-noble metals for 2e- ORR. The results show that Cu-C24N24, Pd-C24N24, Pt-C24N24, and Rh-C24N24 possess good stability. In addition, the Cu-C24N24 SAC exhibits an ideal OOH* binding energy of 4.26 eV, leading to a notably optimal catalytic activity for 2e- ORR. What is more, the Cu-C24N24 SAC shows a preference for aiding in H2O2 production over the rival 4e- ORR with an overpotential of merely 0.04 V. Given these desirable properties, the Cu-C24N24 SAC emerges as a promising option for facilitating 2e- ORR.
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods