Improving Singlet Oxygen Resistance during Photochemical Water Oxidation by Cobalt Porphyrin Catalysts

Improving Singlet Oxygen Resistance during Photochemical Water Oxidation by Cobalt Porphyrin Catalysts
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DOI:
10.1002/chem.201500716
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发表时间:
2015-04-27
影响因子:
4.3
通讯作者:
Sakai, Ken
Sakai, Ken
中科院分区:
化学2区
文献类型:
--
作者:
Nakazono, Takashi;Parent, Alexander R.;Sakai, Ken

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通过人工光合作用在全球范围内生产太阳能燃料需要开发具有显著改善的稳定性的水氧化催化剂。光系统的稳定性通常由于在光捕获期间产生的单线态氧的攻击而降低。在这里,我们报告的光化学水氧化CoFPS,氟化钴卟啉的设计抵抗攻击单线态氧。CoFPS相对于其非氟化类似物表现出显著改善的稳定性,如营业额大幅增加所示。这种增加的稳定性是由于CoFPS对单线态氧攻击的抗性,单线态氧的形成通过使用9,10-二苯基蒽作为化学探针原位监测。动态光散射(DLS)证实CoFPS保持均匀,证明其在水氧化催化期间的稳定性。
Enabling the production of solar fuels on a global scale through artificial photosynthesis requires the development of water oxidation catalysts with significantly improved stability. The stability of photosystems is often reduced owing to attack by singlet oxygen, which is produced during light harvesting. Here, we report photochemical water oxidation by CoFPS, a fluorinated Co-porphyrin designed to resist attack by singlet oxygen. CoFPS exhibits significantly improved stability relative to its non-fluorinated analogue, as shown by a large increase in turnover numbers. This increased stability results from resistance of CoFPS to attack by singlet oxygen, the formation of which was monitored in situ by using 9,10-diphenylanthracene as a chemical probe. Dynamic light scattering (DLS) confirms that CoFPS remains homogeneous, proving its stability during water oxidation catalysis.