Single Site W(0) versus Re(I)-Dipyridophenazine- Based Conjugated Porous Polymer for CO2 Photoreduction

Ángela Matarín, Félix Sánchez, Laura Collado, Mariam Barawi, Victor A. de la Peña O'Shea, Avelina Arnanz, Marta Liras, Marta Iglesias
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Abstract

Herein, the synthesis and characterization of two robust tungsten and rhenium carbonyl complexes integrated into an organic polymer (CPP-Re, CPP-W) are reported. These polymers are obtained by a Suzuki coupling reaction between the corresponding dibromo metal-carbonyl substituted dipyrido[3,2-a:2′,3′-c]phenazine complex and 1,3,5-triphenylbenzene-4′,4″,4″,4‴-triboronic acid and integrated catalytic active sites and photosensitizer since they have not only nitrogen sites to coordinate metal active centers as rhenium or tungsten but photoactive units with good charge-separating ability which can significantly improve the CO2 photoreduction reaction (CO2PRR). These polymers show similar activity in solid–gas CO2PRR in absence of sacrificial agents to produce syn gas (CO + H2) but CPP-W selectivity to products change regarding CPP-Re being able to produce also large amount of more demanding electron products such as methane and ethane. Moreover, the single-site Re- or W-CPP catalysts could prevent the dimerization of complexes that produces its deactivation. This work shows the potential of CPPs as matrices to support single active centers for heterogeneous catalysis.

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用于二氧化碳光还原的单位点 W(0) 与 Re(I)- 二哒嗪基共轭多孔聚合物
本文报告了集成到有机聚合物(CPP-Re、CPP-W)中的两种坚固的钨和铼羰基复合物的合成和表征。这些聚合物是通过相应的二溴金属羰基取代二吡啶并[3,2-a:2′,3′-c]吩嗪络合物和 1,3,5-三苯基苯-4′,4″,4″,4‴-三硼酸之间的铃木偶联反应得到的,并集成了催化活性位点和光敏剂,因为它们不仅具有氮位点来配位金属活性中心(如铼或钨),还具有具有良好电荷分离能力的光活性单元,可显著改善二氧化碳光还原反应(CO2PRR)。在没有牺牲剂的情况下,这些聚合物在固体气体 CO2PRR 中显示出类似的活性,可产生合成气体(CO + H2),但 CPP-W 对产物的选择性发生了变化,CPP-Re 还能产生大量对电子要求更高的产物,如甲烷和乙烷。此外,单位点 Re- 或 W-CPP 催化剂可以防止复合物二聚化而导致失活。这项工作显示了 CPP 作为基质支持单活性中心进行异相催化的潜力。
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