文献类型：期刊文献

英文题名：The Nature of Interfacial Catalysis over Pt/NiAl2O4 for Hydrogen Production from Methanol Reforming Reaction

作者：Wang, Xiuyi[1,2];Li, Didi[3,4];Gao, Zirui[5,6];Guo, Yong[3,4];Zhang, Hongbo[1,2];Ma, Ding[5,6]

机构：[1]Nankai Univ, Sch Mat Sci & Engn, Tianjin 300350, Peoples R China;[2]Haihe Lab Sustainable Chem Transformat, Tianjin 300350, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai Key Lab Funct Mat Chem, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[5]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China;[6]Peking Univ, Coll Engn, Beijing 100871, Peoples R China

年份：2023

卷号：145

期号：2

起止页码：905

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20230113342348);WOS:【SCI-EXPANDED(收录号:WOS:000906866500001)】；

基金：This work received financial support by National Key R&D Program of China (2021YFA1501102), "the Fundamental Research Funds for the Central Universities", Nankai University (63223022); the Haihe Laboratory of Sustainable Chemical Transformations; and National Natural Science Foundation of China (22172078, 22072041 ,21932002).

语种：英文

外文关键词：Aluminum compounds - Catalysis - Catalyst activity - Catalytic reforming - Chemical shift - Dehydrogenation - Hydrogen production - Methanol - Nickel compounds - Phase interfaces - Platinum compounds - Reaction intermediates

摘要：Reforming of methanol is one of the most favorable chemical processes for on-board H2 production, which alleviates the limitation of H2 storage and transportation. The most important catalytic systems for methanol reacting with water are interfacial catalysts including metal/metal oxide and metal/carbide. Nevertheless, the assessment on the reaction mechanism and active sites of these interfacial catalysts are still controversial. In this work, by spectroscopic, kinetic, and isotopic investigations, we established a compact cascade reaction model (ca. the Langmuir- Hinshelwood model) to describe the methanol and water activation over Pt/NiAl2O4. We show here that reforming of methanol experiences methanol dehydrogenation followed by water-gas shift reaction (WGS), in which two separated kinetically relevant steps have been identified, that is, C-H bond rupture within methoxyl adsorbed on interface sites and O-H bond rupture within OlH (Ol: oxygen-filled surface vacancy), respectively. In addition, these two reactions were primarily determined by the most abundant surface intermediates, which were methoxyl and CO species adsorbed on NiAl2O4 and Pt, respectively. More importantly, the excellent reaction performance benefits from the following bidirectional spillover of methoxyl and CO species since the interface and the vacancies on the support were considered as the real active component in methanol dehydrogenation and the WGS reaction, respectively. These findings provide deep insight into the reaction process as well as the active component during catalysis, which may guide the design of new catalytic systems.