Supramolecular photocatalysts fixed on the inside of the polypyrrole layer in dye sensitized molecular photocathodes: application to photocatalytic CO(2) reduction coupled with water oxidation.
Supramolecular photocatalysts fixed on the inside of the polypyrrole layer in dye sensitized molecular photocathodes: application to photocatalytic CO(2) reduction coupled with water oxidation.
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DOI：
10.1039/d1sc03756k
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发表时间：
2021-10-13
期刊：
影响因子：
8.4
通讯作者：
Ishitani O
中科院分区：
文献类型：
--
作者：
Kuttassery F;Kumagai H;Kamata R;Ebato Y;Higashi M;Suzuki H;Abe R;Ishitani O
以水为还原剂、以太阳光为能源的光催化二氧化碳还原系统的开发是人工光合作用道路上最重要的里程碑之一。虽然这种还原可以使用包含作为氧化还原光敏剂的金属络合物和固定在p型半导体电极上的催化剂单元的染料敏化分子光电阴极来进行，但是相应的光电化学电池的性能仍然较低，例如它们的最高入射光子到电流转换效率(IPCE)等于1.2%。在此，我们报道了一种用于水中光催化CO2还原的新型染料敏化分子光电阴极，其特征是聚吡咯层，[Ru(二亚胺)3]2+作为氧化还原光敏剂单元，Ru(二亚胺)(CO)2Cl2作为催化剂单元，并揭示了聚吡咯网络的结合显着提高了相对于之前报道的染料敏化分子光电阴极的反应性和耐久性。新型光电阴极在低偏压下用可见光照射，稳定地诱导 CO2 光催化还原为 CO 和 HCOOH，具有高法拉第效率和选择性（即使在水溶液中），最高 IPCE 为 4.7%。新型光电阴极与n型半导体光电阳极（CoOx/BiVO4和RhOx/TaON）耦合构建全电池，在零偏压下以可见光照射作为唯一能量输入，使用水作为还原剂来光催化还原二氧化碳。具有染料敏化分子光电阴极的人造Z型光电化学电池在两个电极均受到可见光照射下实现了8.3 × 10−2%的最高能量转换效率，而使用太阳光模拟器（AM 1.5，100 mW cm−2）的串联型电池实现了4.2 × 10−2%的太阳能到化学转化效率。一种具有聚吡咯网络的新型染料敏化分子光电阴极，通过使用水作为还原剂和可见光作为能量，在光催化二氧化碳还原方面表现出高效率和耐久性。
The development of systems for photocatalytic CO2 reduction with water as a reductant and solar light as an energy source is one of the most important milestones on the way to artificial photosynthesis. Although such reduction can be performed using dye-sensitized molecular photocathodes comprising metal complexes as redox photosensitizers and catalyst units fixed on a p-type semiconductor electrode, the performance of the corresponding photoelectrochemical cells remains low, e.g., their highest incident photon-to-current conversion efficiency (IPCE) equals 1.2%. Herein, we report a novel dye-sensitized molecular photocathode for photocatalytic CO2 reduction in water featuring a polypyrrole layer, [Ru(diimine)3]2+ as a redox photosensitizer unit, and Ru(diimine)(CO)2Cl2 as the catalyst unit and reveal that the incorporation of the polypyrrole network significantly improves reactivity and durability relative to those of previously reported dye-sensitized molecular photocathodes. The irradiation of the novel photocathode with visible light under low applied bias stably induces the photocatalytic reduction of CO2 to CO and HCOOH with high faradaic efficiency and selectivity (even in aqueous solution), and the highest IPCE is determined as 4.7%. The novel photocathode is coupled with n-type semiconductor photoanodes (CoOx/BiVO4 and RhOx/TaON) to construct full cells that photocatalytically reduce CO2 using water as the reductant upon visible light irradiation as the only energy input at zero bias. The artificial Z-scheme photoelectrochemical cell with the dye-sensitized molecular photocathode achieves the highest energy conversion efficiency of 8.3 × 10−2% under the irradiation of both electrodes with visible light, while a solar to chemical conversion efficiency of 4.2 × 10−2% is achieved for a tandem-type cell using a solar light simulator (AM 1.5, 100 mW cm−2). A novel dye-sensitized molecular photocathode with polypyrrole networks exhibits high efficiency and durability for photocatalytic CO2 reduction by using water as reductant and visible light as energy.
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影响因子：
4.6
作者：
ChardonNoblat, S;Deronzier, A;Zsoldos, D
通讯作者：
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影响因子：
3.9
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