Direct and Selective Synthesis of Hydrogen Peroxide over Palladium-Tellurium Catalysts at Ambient Pressure
Direct and Selective Synthesis of Hydrogen Peroxide over Palladium-Tellurium Catalysts at Ambient Pressure
复制标题
常压钯碲催化剂直接选择性合成过氧化氢
DOI：
10.1002/cssc.201701238
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发表时间：
2017
期刊：
影响因子：
8.4
通讯作者：
Han Yi-Fan
中科院分区：
文献类型：
--
作者：
Tian Pengfei;Xu Xingyan;Ao Can;Ding Doudou;Li Wei;Si Rui;Tu Weifeng;Xu Jing;Han Yi-Fan
由H_2和O_2直接合成高选择性过氧化氢(H_2O_2)是绿色工艺中非常理想的反应。本文报道了一种高效的钯-碲(Pd-Te/Ti02)催化剂，在温和的条件下(283 K，0.1 Mpa，半间歇连续流动反应器)对H_2O_2的选择性接近100 %。Te的加入使Pd颗粒的尺寸从2.1 nm显著减小到1.4 nm。Te修饰的Pd表面可以显著削弱O2的解离活性，导致O2的非解离氢化。密度泛函理论计算揭示了Te在O2选择加氢反应中的关键作用，即由Pd和Te组成的活性中心可以显著抑制副反应。这项工作在开发常压下直接合成过氧化氢的高选择性催化剂方面取得了重大进展。
Highly selective hydrogen peroxide (H2O2) synthesis directly from H2and O2is a strongly desired reaction for green processes. Herein a highly efficient palladium–tellurium (Pd–Te/TiO2) catalyst with a selectivity of nearly 100 % toward H2O2under mild conditions (283 K, 0.1 MPa, and a semi‐batch continuous flow reactor) is reported. The size of Pd particles was remarkably reduced from 2.1 nm to 1.4 nm with the addition of Te. The Te‐modified Pd surface could significantly weaken the dissociative activation of O2, leading to the non‐dissociative hydrogenation of O2. Density functional theory calculations illuminated the critical role of Te in the selective hydrogenation of O2, in that the active sites composed of Pd and Te could significantly restrain side reactions. This work has made significant progress on the development of high‐selectivity catalysts for the direct synthesis of H2O2at ambient pressure.