Engineering the exposed facets and open-coordinated sites of brookite TiO2 to boost the loaded Ru nanoparticle efficiency in benzene selective hydrogenation
Engineering the exposed facets and open-coordinated sites of brookite TiO2 to boost the loaded Ru nanoparticle efficiency in benzene selective hydrogenation
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设计板钛矿 TiO2 的暴露面和开放配位位点，以提高苯选择性加氢中负载 Ru 纳米颗粒的效率
DOI：
10.1016/j.apsusc.2019.05.029
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发表时间：
2019-08
影响因子：
6.7
通讯作者：
Daiping He
中科院分区：
文献类型：
--
作者：
Gongbing Zhou;Lan Jiang;Yanlu Dong;Rong Li;Daiping He
通过改变板钛矿型TiO2的晶面和棱角原子的比例，使其暴露出更多的配位不饱和原子和开配位位点，对提高负载金属纳米粒子的催化效率具有重要意义，但由于板钛矿型TiO2结构对称性差和热力学亚稳性差，面临着巨大的挑战。在此，我们制备了具有纳米花（NF）、纳米棒（NR）和纳米片（NS）形状的板钛矿型TiO2，这些形状增加了高能面上的Ti原子的催化活性和边角原子上的开配位位点。发现这些增量在活性和选择性两方面都提高了负载的Ru NPs在苯选择性加氢为环己烯中的效率。结合综合表征，苯的周转频率增加归因于吸附在板钛矿TiO2的上述催化活性位点上的苯的量和强度的增加，其与从Ru NPs解离的溢出氢（Hso）反应。对于环己烯选择性的提高，据推测，这是源于提高加氢速率常数比的苯到环己烯和环己烯到环己烷的步骤和加速环己烯脱附一旦它形成在催化剂上的钛原子和开放的配位的板钛矿TiO 2。
Engineering the crystal facets and the proportion of edge and corner atoms of brookite TiO2to expose more coordinatively unsaturated (cus) atoms and open-coordinated sites is of significant importance in boosting the loaded metal nanoparticle (NP) efficiency in heterogeneous catalysis, but suffering tremendous challenge owing to the low structural symmetry and thermodynamic metastability of brookite TiO2. Herein, we prepared brookite TiO2with nanoflower (NF), nanorod (NR), and nanosheet (NS) shapes, which increased in the catalytically activecusTi atoms on high-energy facets and the open-coordinated sites on edge and corner atoms. These increments were found to boost the loaded Ru NPs efficiency in selective hydrogenation of benzene to cyclohexene both in activity and selectivity. Combined with comprehensive characterizations, the increased turnover frequency of benzene was ascribed to the increment in the amount and strength of benzene adsorbed on the above catalytically active sites of brookite TiO2, which reacted with spillover hydrogen (Hso) dissociated from Ru NPs. For the improvement in cyclohexene selectivity, it was speculated to be originated from the elevation of the hydrogenation rate constant ratios of benzene to cyclohexene and cyclohexene to cyclohexane steps and the acceleration of cyclohexene desorption once it is formed on the catalyst by thecusTi atoms and the open-coordinated sites on brookite TiO2.
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