Li Jian Hong, Yu Zhi Wu, Gao Zhi, Li Jian Qiang, Tao Yuan, Xiao Yu Xin, Yin Wen Hui, Fan Ya Ling, Jiang Chao, Sun Li Jun, Luo Feng
China Institute of Atomic Energy , Beijing 100822 , P. R. China.
State Key Laboratory of Nuclear Resources and Environment, School of Chemistry, Biology and Materials Science , East China University of Technology , Nanchang 330013 , P. R. China.
Inorg Chem. 2019 Aug 19;58(16):10829-10836. doi: 10.1021/acs.inorgchem.9b01117. Epub 2019 Aug 1.
Developing noble-metal-based catalysts with ultralow loading to achieve excellent performance for selective hydrogenation of alkynes under mild reaction conditions is highly desirable but still faces huge challenges. To this end, a SOH-anchored covalent organic framework (COF-SOH) as the support was deliberately designed, and then ultralow-content Pd (0.38 wt %) was loaded by a wet-chemistry immersion dispersion method. The resulting Pd/COF-SOH composite exhibits outstanding performance for the selective hydrogenation of phenylacetylene with 97.06% conversion and 93.15% selectivity to styrene under mild reaction conditions (1 bar of H, 25 °C). Noticeably, the turnover frequency value reaches as high as 3888 h, which outperforms most of reported catalysts for such use. Moreover, such a catalyst also exhibits excellent activity for a series of other alkynes and high stability without obvious loss of catalytic performance after five consecutive cycles.
开发具有超低负载量的贵金属基催化剂，以在温和反应条件下实现炔烃选择性加氢的优异性能，这是非常可取的，但仍面临巨大挑战。为此，特意设计了一种以SOH为锚定的共价有机框架（COF-SOH）作为载体，然后通过湿化学浸渍分散法负载超低含量的钯（0.38 wt%）。所得的Pd/COF-SOH复合材料在温和反应条件（1 bar氢气，25°C）下对苯乙炔选择性加氢表现出优异性能，苯乙炔转化率为97.06%，对苯乙烯的选择性为93.15%。值得注意的是，其周转频率值高达3888 h⁻¹，优于大多数报道的此类用途催化剂。此外，这种催化剂对一系列其他炔烃也表现出优异活性，并且具有高稳定性，在连续五个循环后催化性能无明显损失。
