Photochemical CO2 Reduction Driven by Water-Soluble Copper(I) Photosensitizer with the Catalysis Accelerated by Multi-Electron Chargeable Cobalt Porphyrin,ACS Catalysis

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Photochemical CO2 Reduction Driven by Water-Soluble Copper(I) Photosensitizer with the Catalysis Accelerated by Multi-Electron Chargeable Cobalt Porphyrin
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-11-11 , DOI: 10.1021/acscatal.9b04023
Xian Zhang _{1,

2} , Mihaela Cibian _{1,

3} , Arnau Call ₂ , Kosei Yamauchi _{1,

2} , Ken Sakai _{1,

2,

4}

Affiliation

Without using precious elements, a highly efficient and selective molecular-based photocatalytic system for CO₂-to-CO conversion in fully aqueous media has been developed. Our copper(I)-based water-soluble photosensitizer (CuPS) preserves its highly luminescent and long-lived excited state even in aqueous media. The CuPS-driven CO₂ reduction catalyzed by a water-soluble cobalt porphyrin possessing four N-methylpyridinium acceptors at the meso positions (CoTMPyP) achieves the highest catalytic activity among those reported for aqueous systems: TON_CO = 2680 and TOF_CO^max = 1600–2600 h^–1 with Sel_CO2 = 77–90% (selectivity for CO vs H₂). The observed photocatalytic enhancement is discussed in terms of the 6-electron chargeable character of CoTMPyP, permitting its rapid release of CO via reduction of Co^II to Co^I by intramolecular electron transfer from the reducing equivalent stored at one of the acceptors.

中文翻译：

水溶性铜（I）光敏剂驱动的多电子带电钴卟啉催化光化学还原CO ₂

在不使用珍贵元素的情况下，已经开发了用于在完全水性介质中将CO ₂转化为CO的高效且选择性的基于分子的光催化系统。我们的基于铜（I）的水溶性光敏剂（CuPS）即使在水性介质中也能保持其高发光度和长寿命的激发态。由水溶性钴卟啉在介观位置具有四个N-甲基吡啶鎓受体（CoTMPyP）催化的CuPS驱动的CO ₂还原在水性体系中达到最高的催化活性：TON _CO = 2680和TOF _CO^max = 1600 –2600小时^–1（带Sel）_CO2 = 77–90％（CO与H _2的选择性）。所观察到的光催化增强是在6-电子充电字符来讨论CoTMPyP，允许通过减少的Co其CO的快速释放^II对Co^我通过从还原当量存储在所述受体的一个分子内的电子转移。

更新日期：2019-11-13

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