Rhenium-Metalated Polypyridine-Based Porous Polycarbazoles for Visible-Light CO2 Photoreduction

Rhenium-Metalated Polypyridine-Based Porous Polycarbazoles for Visible-Light CO2 Photoreduction
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用于可见光 CO2 光还原的铼金属化聚吡啶基多孔聚咔唑

DOI:
10.1021/acscatal.8b04032
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发表时间:
2019-05-01
期刊:
影响因子:
12.9
通讯作者:
Han, Bao-Hang
Han, Bao-Hang
中科院分区:
化学1区
文献类型:
--
作者:
Liang, Hai-Peng;Acharjya, Amitava;Han, Bao-Hang

文献摘要

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将二氧化碳转化为有价值的化学品,特别是燃料,被认为是减少我们对化石燃料的依赖和缓解气候变化的一种有前途的方法。通过简单的氧化偶联反应构建了带有铼金属化聚吡啶官能团的咔唑基多孔聚合物。这些多孔聚合物用作固定催化活性铼络合物的多相载体,并且还提供高CO2吸附能力和光吸收能力,即光敏性能。因此,这种铼金属化微孔聚咔唑网络在可见光照射下表现出高CO2光还原效率,CO释放速率高达623 μmol g–1 h–1,选择性为97.8%。与分子催化剂相比,微孔固体光催化剂在长期使用过程中表现出增强的稳定性和光催化性能。
Transformation of CO2 into valuable chemicals and especially fuels is deemed as a promising approach to reduce our dependence on fossil fuels and to alleviate climate change. Carbazole-based porous polymers bearing rhenium-metalated polypyridine functionalities were constructed via simple oxidative coupling reaction. These porous polymers are employed as heterogeneous supports for immobilization of catalytically active rhenium complexes and furthermore provide high CO2 adsorption capabilities and light absorption abilities, i.e., photosensitizing properties. Consequently, such rhenium-metalated microporous polycarbazole networks show high efficiencies for CO2 photoreduction upon visible-light irradiation, with a CO evolution rate up to 623 μmol g–1 h–1 and selectivity of 97.8%. The microporous solid photocatalyst shows enhanced stability and photocatalytic performance compared to the molecular catalysts during long-term use.