Exact stoichiometry high surface area mesoporous AlPO4 glass for efficient catalysis
Exact stoichiometry high surface area mesoporous AlPO4 glass for efficient catalysis
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DOI：
10.1007/s10853-022-07577-y
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发表时间：
2022-09-17
影响因子：
4.5
通讯作者：
Avnir，David
中科院分区：
文献类型：
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作者：
He，Jin;Guo，Wei;Avnir，David
介孔AlPO4材料由于具有较高的热稳定性和化学稳定性，在催化领域引起了人们的广泛关注。特别令人感兴趣的是通过无模板水溶液溶胶-凝胶合成路线制备的纯化学计量比高比表面(>； 500m2/g)介孔磷酸铝(MAlPO_4)玻璃。为了将这种材料应用于催化，我们开发了将催化金属纳米颗粒(NPs)-Pd和Rh-负载到它身上的方法，并通过一系列分析方法对所得到的掺杂材料进行了详细的表征研究，包括同步X射线吸收光谱、非弹性中子散射等。然后对该材料本身和作为催化纳米颗粒载体的催化适用性进行了评价。纯的mAlPO4表现出良好的酸催化的[3 + 2]环加成反应。负载Pd纳米粒子的mAlPO4催化剂能非常有效地催化苯甲醇的脱氧反应。负载Rh纳米粒子的MAlPO4催化剂具有高选择性，可用于苯酚和甲酚的加氢反应，并可将工业上大量的甲苯加氢为甲基环己烷。对这些成功的催化剂的材料科学方面进行了详细的研究，例如，导致了对界面Rh/Pd-O-P键的重要作用的理解。
Mesoporous AlPO4materials have attracted much attention in catalysis due to their high thermal and chemical stability. Of particular interest for catalysis is the pure stoichiometry high surface area (> 500 m2/g) mesoporous AlPO4(mAlPO4) glass prepared via a template-free aqueous sol–gel synthetic route. Toward the application of this material for catalysis, we have developed methods for loading it with nanoparticles (NPs) of catalytic metals—Pd and Rh—and carried out a detailed characterization study of the resulting doped materials by a wide array of analytical methods, including synchrotron X-ray absorption spectroscopy, inelastic neutron scattering and more. The applicability of this material for catalysis, both by itself and as a support for catalytic NPs, was then evaluated. The pure mAlPO4exhibited excellent acid-catalyzed [3 + 2] cycloaddition of nitriles and sodium azide. mAlPO4loaded with the Pd NPs catalyzed very efficiently deoxygenation reactions of benzyl alcohols. mAlPO4loaded with Rh NPs catalyzed with high selectivity, the hydrogenation of phenols and cresols and full conversion the hydrogenation of the industrially very high-volume toluene to methylcyclohexane. The materials-science aspects of these successful catalysts were studied in detail, leading, for instance, to the understanding of the important role of the interfacial Rh/Pd–O-P bonds.Graphical abstract