{"title":"稳定配体对硫化铜纳米簇氧化 CO 催化特性的影响","authors":"P. S. Bandurist, D. A. Pichugina","doi":"10.1134/S0023158424601785","DOIUrl":null,"url":null,"abstract":"<p>Quantum chemical modeling of CO oxidation on the Cu<sub>12</sub>S<sub>6</sub>(PH<sub>3</sub>)<sub>8</sub> and Cu<sub>12</sub>S<sub>6</sub> clusters was performed in order to establish the general tendencies in the process on metal nanoclusters stabilized by ligands and to find out if the presence of a phosphine ligand is needed in the active site. The Langmuir–Hinshelwood mechanism was studied, which involves sequential oxidation of two CO molecules with oxygen. The calculated activation energies on Cu<sub>12</sub>S<sub>6</sub>(PH<sub>3</sub>)<sub>8</sub> are lower than on Cu<sub>12</sub>S<sub>6</sub> for all oxidation stages; therefore, the PH<sub>3</sub> ligands have a positive effect on the catalytic properties of the copper sulfide cluster in the CO oxidation. A linear correlation was found between the energy of CO adsorption on various copper sulfide clusters and the activation energy of the oxidation stage: the lowest activation energy is observed for the cluster with a CO adsorption energy of 36 kJ/mol.</p>","PeriodicalId":682,"journal":{"name":"Kinetics and Catalysis","volume":"65 4","pages":"347 - 355"},"PeriodicalIF":1.3000,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of Stabilizing Ligand on the Catalytic Properties of Copper Sulfide Nanoclusters in CO Oxidation\",\"authors\":\"P. S. Bandurist, D. A. Pichugina\",\"doi\":\"10.1134/S0023158424601785\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Quantum chemical modeling of CO oxidation on the Cu<sub>12</sub>S<sub>6</sub>(PH<sub>3</sub>)<sub>8</sub> and Cu<sub>12</sub>S<sub>6</sub> clusters was performed in order to establish the general tendencies in the process on metal nanoclusters stabilized by ligands and to find out if the presence of a phosphine ligand is needed in the active site. The Langmuir–Hinshelwood mechanism was studied, which involves sequential oxidation of two CO molecules with oxygen. The calculated activation energies on Cu<sub>12</sub>S<sub>6</sub>(PH<sub>3</sub>)<sub>8</sub> are lower than on Cu<sub>12</sub>S<sub>6</sub> for all oxidation stages; therefore, the PH<sub>3</sub> ligands have a positive effect on the catalytic properties of the copper sulfide cluster in the CO oxidation. A linear correlation was found between the energy of CO adsorption on various copper sulfide clusters and the activation energy of the oxidation stage: the lowest activation energy is observed for the cluster with a CO adsorption energy of 36 kJ/mol.</p>\",\"PeriodicalId\":682,\"journal\":{\"name\":\"Kinetics and Catalysis\",\"volume\":\"65 4\",\"pages\":\"347 - 355\"},\"PeriodicalIF\":1.3000,\"publicationDate\":\"2024-09-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Kinetics and Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1134/S0023158424601785\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Kinetics and Catalysis","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1134/S0023158424601785","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Effect of Stabilizing Ligand on the Catalytic Properties of Copper Sulfide Nanoclusters in CO Oxidation
Quantum chemical modeling of CO oxidation on the Cu12S6(PH3)8 and Cu12S6 clusters was performed in order to establish the general tendencies in the process on metal nanoclusters stabilized by ligands and to find out if the presence of a phosphine ligand is needed in the active site. The Langmuir–Hinshelwood mechanism was studied, which involves sequential oxidation of two CO molecules with oxygen. The calculated activation energies on Cu12S6(PH3)8 are lower than on Cu12S6 for all oxidation stages; therefore, the PH3 ligands have a positive effect on the catalytic properties of the copper sulfide cluster in the CO oxidation. A linear correlation was found between the energy of CO adsorption on various copper sulfide clusters and the activation energy of the oxidation stage: the lowest activation energy is observed for the cluster with a CO adsorption energy of 36 kJ/mol.
期刊介绍：
Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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