Crystal-Plane-Controlled Selectivity of Cu2O Catalysts in Propylene Oxidation with Molecular Oxygen
Crystal-Plane-Controlled Selectivity of Cu2O Catalysts in Propylene Oxidation with Molecular Oxygen
复制标题
Cu2O 催化剂在分子氧氧化丙烯中的晶面控制选择性
DOI：
10.1002/anie.201402374
复制
发表时间：
2014-05-05
影响因子：
16.6
通讯作者：
Huang, Weixin
中科院分区：
文献类型：
--
作者：
Hua, Qing;Cao, Tian;Huang, Weixin
丙烯与O-2选择氧化制环氧丙烷和丙烯醛是一个很有意义的研究课题。报道了无封端配体的均匀Cu_2 O八面体、立方体和菱形十二面体催化丙烯氧化反应的晶面控制选择性：暴露于{111}晶面的Cu_2 O八面体对丙烯醛的选择性最高，暴露于{100}晶面的Cu_2 O立方体对CO_2的选择性最高;暴露{110}晶面的Cu 2 O菱形十二面体对环氧丙烷的选择性最高。一配位的Cu在Cu 2 O（111）上、三配位的O在Cu 2 O（110）上和二配位的O在Cu 2 O（100）上分别被确定为丙烯醛、环氧丙烷和CO2的催化活性位。这些结果表明，氧化物催化剂的晶面工程可能是一个有用的策略，用于开发选择性催化剂，并在分子水平上获得复杂的多相催化反应的基本理解。
The selective oxidation of propylene with O-2 to propylene oxide and acrolein is of great interest and importance. We report the crystal-plane-controlled selectivity of uniform capping-ligand-free Cu2O octahedra, cubes, and rhombic dodecahedra in catalyzing propylene oxidation with O-2: Cu2O octahedra exposing {111} crystal planes are most selective for acrolein; Cu2O cubes exposing {100} crystal planes are most selective for CO2; Cu2O rhombic dodecahedra exposing {110} crystal planes are most selective for propylene oxide. One-coordinated Cu on Cu2O(111), three-coordinated O on Cu2O(110), and two-coordinated O on Cu2O(100) were identified as the catalytically active sites for the production of acrolein, propylene oxide, and CO2, respectively. These results reveal that crystal-plane engineering of oxide catalysts could be a useful strategy for developing selective catalysts and for gaining fundamental understanding of complex heterogeneous catalytic reactions at the molecular level.