催化作用
合理设计
氧化物
钼
沸石
氧化钼
金属
密度泛函理论
甲烷
限制
材料科学
碳化物
无机化学
化学工程
纳米技术
化学
计算化学
有机化学
冶金
机械工程
工程类
作者
Emanuele J. Hiennadi,Fateme Molajafari,Rachita Rana,Adam S. Hoffman,Simon R. Bare,Joshua D. Howe,Sheima J. Khatib
标识
DOI:10.1021/acs.chemmater.3c01545
摘要
Metal oxide-impregnated zeolites are employed in a wide variety of catalytic reactions, including methane dehydroaromatization (MDA). The most studied catalysts for MDA are Mo carbides supported on H-ZSM-5, formed through the carburization of Mo-oxide-loaded H-ZSM-5. A complete structural understanding of these materials has not yet been achieved, limiting the potential for rational catalyst design for improved performance. We hereby pursue experimental and theoretical investigations of these catalyst precursors to uncover rational design principles. We employ temperature-programmed oxidation and extended X-ray absorption fine-structure experiments, density functional theory calculations, and QuantEXAFS analysis to unveil Mo-oxide speciation in H-ZSM-5. We demonstrate that Mo-oxides exist within these systems as a combination of various motifs, and the relative abundance of these species is controlled through tailored preparation methods. The synergies exploited in this work may be leveraged in other related catalysts. The conclusions drawn are applicable to other relevant applications of zeolite-supported metal oxides.
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