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作 者:Erwin Lam Kim Larmier Shohei Tada Patrick Wolf Olga V. Safonova Christophe Copéret Erwin Lam;Kim Larmier;Shohei Tada;Patrick Wolf;Olga V. Safonova;Christophe Copéret(苏黎世联邦理工学院化学与应用生物科学系,瑞士苏黎世CH-8093;保罗谢尔研究所,瑞士菲利根CH-5232;法国国际石油研究所,法国索莱兹69360;东京大学化工系统工程系,日本东京113-8656)
机构地区:[1]ETH Zürich, Department of Chemistry and Applied Biosciences, Vladimir-Prelog-Weg 1-5, CH-8093, Zürich, Switzerland [2]Paul Scherrer Institute, CH-5232 Villigen, Switzerland [3]IFP Energies Nouvelles, Rond-Point de l’échangeur de Solaize, BP3, 69360 Solaize, France [4]Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, 113-8656 Tokyo, Japan
出 处:《Chinese Journal of Catalysis》2019年第11期1741-1748,共8页催化学报(英文)
基 金:E.L.,K.L.,P.W.,and S.T.are supported by the SCCER-Heat and Energy Storage program
摘 要:Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carried out on the Cu and Zr K-edge. Under reaction conditions, Cu remains metallic, while Zr is present in three types of coordination environment associated with 1) bulk ZrO2, 2) coordinatively saturated and 3) unsaturated Zr(Ⅳ) surface sites. The amount of coordinatively unsaturated Zr surface sites can be quantified by linear combination fit of reference X-Ray absorption near edge structure (XANES) spectra and its amount correlates with CH3OH formation rates, thus indicating the importance of Zr(Ⅳ) Lewis acid surface sites in driving the selectivity toward CH3OH. This finding is consistent with the proposed mechanism, where CO2 is hydrogenated at the interface between the Cu nanoparticles that split H2 and Zr(Ⅳ) surface sites that stabilizes reaction intermediates.Cu/ZrO2/SiO2是有效的CO2选择加氢制甲醇催化剂.为了理解混合氧化物基催化剂中ZrO2的作用,在Cu和Zr的K边进行了原位X-射线吸收光谱测试.在反应条件下, Cu保持金属态,而Zr以三类配位环境的形式存在:体相ZrO2,配位饱和的、以及不饱和的Zr(Ⅳ)表面位.配位不饱和Zr表面位可通过线性拟合参比的X射线吸收近边结构光谱进行定量,发现其数量与甲醇生成速率有关,因而表明Zr(Ⅳ)Lewis酸表面位在驱动选择生成甲醇反应中的重要性.这与提出的机理是一致的:在裂解H2的Cu纳米颗粒与稳定反应中间体的Zr(Ⅳ)表面位之间的界面上进行CO2加氢.
关 键 词:CO2 hydrogenation ZrO2/SiO2 supported Cu nanoparticles Lewis acidic surface sites In situ X-ray absorption spectroscopy
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