{"title":"具有金属碳化物/金属氮负载相互作用的高性能钼基多组分催化剂的原位构建","authors":"Xiaolong Li, Jundi Wan, Manni Sun, Yahui Zhang, Zhiyan Yang, Xiru Wang, Junli Zhu, Yongning Ma, Zhuoya Zhao, Yuhao Yang","doi":"10.1021/acs.iecr.5c00319","DOIUrl":null,"url":null,"abstract":"The development of nonprecious metal supported catalysts is crucial for advancing the chemical industry. In this study, we successfully synthesized molybdenum-based three-component catalysts (Mo-BMC) by in situ loading β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N onto the reducible MoO<sub>2-x</sub> through the thermal decomposition method of metal complexes. Notably, XPS revealed a significant electronic transfer from β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N to MoO<sub>2–<i>x</i></sub> in Mo-BMC, reflecting the presence of strong metal carbide/metal nitride-support interactions. Using the reverse water gas shift reaction (RWGS) as a model, the Mo-BMC demonstrated outstanding catalytic performance, achieving a CO<sub>2</sub> conversion of 43.07% and over 99.7% CO selectivity at 500 °C, outperforming 5% Pt/MoO<sub>2–<i>x</i></sub> with a CO<sub>2</sub> conversion (12.61%) 3.42 times higher. Mechanistic studies reveal that in the Mo-BMC, the reducible MoO<sub>2–<i>x</i></sub> primarily facilitates CO<sub>2</sub> activation, while the Pt-like β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N effectively activate H<sub>2</sub>. The RWGS reaction proceeds via the formate mechanism. By replacing active metals in traditional metal-supported catalysts with β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N, Mo-BMC not only retains high activity but also significantly reduces costs and improves sintering resistance. This study provides a new approach for the development of novel high-performance catalysts, effectively advancing the industrial application of low-cost, high-activity, and highly stable catalysts.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"112 1","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"In Situ Construction of High-Performance Molybdenum-Based Multicomponent Catalysts with Metal Carbide/Metal Nitride-Support Interactions\",\"authors\":\"Xiaolong Li, Jundi Wan, Manni Sun, Yahui Zhang, Zhiyan Yang, Xiru Wang, Junli Zhu, Yongning Ma, Zhuoya Zhao, Yuhao Yang\",\"doi\":\"10.1021/acs.iecr.5c00319\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The development of nonprecious metal supported catalysts is crucial for advancing the chemical industry. In this study, we successfully synthesized molybdenum-based three-component catalysts (Mo-BMC) by in situ loading β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N onto the reducible MoO<sub>2-x</sub> through the thermal decomposition method of metal complexes. Notably, XPS revealed a significant electronic transfer from β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N to MoO<sub>2–<i>x</i></sub> in Mo-BMC, reflecting the presence of strong metal carbide/metal nitride-support interactions. Using the reverse water gas shift reaction (RWGS) as a model, the Mo-BMC demonstrated outstanding catalytic performance, achieving a CO<sub>2</sub> conversion of 43.07% and over 99.7% CO selectivity at 500 °C, outperforming 5% Pt/MoO<sub>2–<i>x</i></sub> with a CO<sub>2</sub> conversion (12.61%) 3.42 times higher. Mechanistic studies reveal that in the Mo-BMC, the reducible MoO<sub>2–<i>x</i></sub> primarily facilitates CO<sub>2</sub> activation, while the Pt-like β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N effectively activate H<sub>2</sub>. The RWGS reaction proceeds via the formate mechanism. By replacing active metals in traditional metal-supported catalysts with β-Mo<sub>2</sub>C and γ-Mo<sub>2</sub>N, Mo-BMC not only retains high activity but also significantly reduces costs and improves sintering resistance. This study provides a new approach for the development of novel high-performance catalysts, effectively advancing the industrial application of low-cost, high-activity, and highly stable catalysts.\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"112 1\",\"pages\":\"\"},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2025-05-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial & Engineering Chemistry Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.iecr.5c00319\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial & Engineering Chemistry Research","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1021/acs.iecr.5c00319","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
In Situ Construction of High-Performance Molybdenum-Based Multicomponent Catalysts with Metal Carbide/Metal Nitride-Support Interactions
The development of nonprecious metal supported catalysts is crucial for advancing the chemical industry. In this study, we successfully synthesized molybdenum-based three-component catalysts (Mo-BMC) by in situ loading β-Mo2C and γ-Mo2N onto the reducible MoO2-x through the thermal decomposition method of metal complexes. Notably, XPS revealed a significant electronic transfer from β-Mo2C and γ-Mo2N to MoO2–x in Mo-BMC, reflecting the presence of strong metal carbide/metal nitride-support interactions. Using the reverse water gas shift reaction (RWGS) as a model, the Mo-BMC demonstrated outstanding catalytic performance, achieving a CO2 conversion of 43.07% and over 99.7% CO selectivity at 500 °C, outperforming 5% Pt/MoO2–x with a CO2 conversion (12.61%) 3.42 times higher. Mechanistic studies reveal that in the Mo-BMC, the reducible MoO2–x primarily facilitates CO2 activation, while the Pt-like β-Mo2C and γ-Mo2N effectively activate H2. The RWGS reaction proceeds via the formate mechanism. By replacing active metals in traditional metal-supported catalysts with β-Mo2C and γ-Mo2N, Mo-BMC not only retains high activity but also significantly reduces costs and improves sintering resistance. This study provides a new approach for the development of novel high-performance catalysts, effectively advancing the industrial application of low-cost, high-activity, and highly stable catalysts.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.