Ultralow-Content Palladium Dispersed in Covalent Organic Framework for Highly Efficient and Selective Semihydrogenation of Alkynes
Ultralow-Content Palladium Dispersed in Covalent Organic Framework for Highly Efficient and Selective Semihydrogenation of Alkynes
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超低含量钯分散在共价有机骨架中用于高效选择性炔烃半氢化
DOI：
10.1021/acs.inorgchem.9b01117
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发表时间：
2019
影响因子：
4.6
通讯作者：
Luo Feng
中科院分区：
文献类型：
--
作者：
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
开发超低负载量的贵金属基催化剂以在温和的反应条件下实现优异的炔选择性加氢性能是非常可取的，但仍然面临巨大的挑战。为此，特意设计了SO 3 H锚定的共价有机骨架（COF-SO 3 H）作为载体，然后通过湿化学浸渍分散法负载超低含量Pd（0.38wt%）。所得Pd0.38/COF-SO 3 H复合物在温和反应条件（1巴H2，25 °C）下表现出苯乙炔选择性氢化的优异性能，转化率为97.06%，苯乙烯选择性为93.15%。值得注意的是，转换频率值高达3888 h-1，这超过了大多数报道的用于此类用途的催化剂。此外，该催化剂对一系列其它炔类也表现出优异的活性和高稳定性，连续5次循环后催化性能没有明显损失。
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 SO3H-anchored covalent organic framework (COF-SO3H) 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 Pd0.38/COF-SO3H 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 H2, 25 °C). Noticeably, the turnover frequency value reaches as high as 3888 h–1, 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.