Durable photoelectrochemical CO2 reduction with water oxidation using a visible-light driven molecular photocathode
Durable photoelectrochemical CO2 reduction with water oxidation using a visible-light driven molecular photocathode
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DOI：
10.1039/d0ta07351b
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发表时间：
2021-01-21
影响因子：
11.9
通讯作者：
Ishitani, Osamu
中科院分区：
文献类型：
--
作者：
Kamata, Ryutaro;Kumagai, Hiromu;Ishitani, Osamu
以水为还原剂、可见光为能源的光催化还原CO2是人工光合作用的重要目标。在这项研究中，我们报告了一种高度稳定的光电化学CO2还原涉及一种新的分子光电阴极，包括NiO电极和聚合络合物的Ru（II）光敏剂和Ru（II）催化剂（NiO/PRu-聚-Ru-RuCAT 1）。在可见光照射和低偏压下，稳定和选择性地产生CO和HCOOH超过100 h。CO2还原产物的周转数超过1200，这代表了使用分子光电阴极的光电化学反应的最高耐久性。此外，NiO/PRu-poly-Ru-RuCAT 1分子光电阴极和CoOx/BiVO 4光电阳极的连接系统适合于水氧化促进稳定的CO2还原，以水作为电子供体和可见光作为能源，无偏压超过24 h。获得了1.7 × 10（-2）%的能量转换效率，这是利用分子光催化剂以水作为还原剂还原CO2的可见光驱动系统所报道的最高值。
Photocatalytic reduction of CO2 using water as a reductant and visible light as the energy source is an important target in artificial photosynthesis. In this study, we report a highly stable photoelectrochemical CO2 reduction involving a new molecular photocathode comprising a NiO electrode and polymerized complexes of the Ru(II) photosensitizer and Ru(II) catalyst (NiO/PRu-poly-Ru-RuCAT1). CO and HCOOH were stably and selectively produced for over 100 h under visible light irradiation and a low bias. The turnover number of CO2 reduction products exceeded 1200, which represents the highest durability reported for photoelectrochemical reactions using molecular photocathodes. Moreover, a connected system of the NiO/PRu-poly-Ru-RuCAT1 molecular photocathode and a CoOx/BiVO4 photoanode suitable for water oxidation facilitated stable CO2 reduction with water as an electron donor and visible light as the energy source, with no bias for over 24 h. An energy conversion efficiency of 1.7 x 10(-2)% was obtained, which is the highest value reported for visible light driven systems utilizing a molecular photocatalyst for CO2 reduction with water as the reductant.