Combinatorial Computational Chemistry Approach to the High-Throughput Screening of Metal Sulfide Catalysts for CO Hydrogenation Process

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• 作者：Momoji Kubo ; Tsuguo Kubota ; Changho Jung ; Kotaro Seki ; Seiichi Takami ; Naoto Koizumi ; Kohji Omata ; Muneyoshi Yamada ; and Akira Miyamoto
• 刊名：Energy & Fuels
• 出版年：2003
• 出版时间：July 2003
• 年：2003
• 卷：17
• 期：4
• 页码：857 - 861
• 全文大小：182K
• 年卷期：v.17,no.4(July 2003)
• ISSN：1520-5029

文摘

We have already proposed that a "Combinatorial Computational Chemistry" approach is veryeffective for performing the theoretical high-throughput screening of new catalysts, and its validitywas strongly confirmed in various catalyst systems. In the present study, we applied ourcombinatorial computational chemistry approach to the design of new metal sulfide catalysts forthe CO hydrogenation process and proposed new guidance for designing the highly selectivecatalysts for methanol synthesis. We investigated H₂ and CO adsorption on a large number ofmetal and metal sulfide catalysts by first-principles calculations, and succeeded in clarifying therelationship between the metal species in the metal and metal sulfide catalysts and the productsof the CO hydrogenation processes. Our results indicated that Co, Mo, Ru, Rh, Ir, and Pd sulfidecatalysts selectively produce methanol, while Re and Os sulfide catalysts selectively producehydrocarbons. The above results are in good agreement with the experimental results of Koizumiand co-workers. Moreover, we proposed that the Pd sulfide catalyst has the highest selectivityfor methanol from the CO hydrogenation process. This result strongly supports the experimentalresults by Koizumi and co-workers. Moreover, we propose that the metal sulfide catalysts, whichrealize the bridge-site adsorption of the CO molecule on both the metal and sulfur atoms, havehigh selectivity for methanol. This proposed guidance for designing the highly selective metalsulfide catalysts for methanol may be useful for the experiments.