首页|Earth-abundant Zn-dipyrrin chromophores for efficient CO2 photoreduction

Earth-abundant Zn-dipyrrin chromophores for efficient CO2 photoreduction

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The development of strong sensitizing and Earth-abundant antenna molecules is highly desirable for CO2 reduction through artificial photosynthesis.Herein,a library of Zn-dipyrrin complexes(Z-1-Z-6)are rationally designed via precisely controlling their molecular configuration to optimize strong sensitizing Earth-abundant photosensitizers.Upon visible-light excitation,their special geometry enables intramolecular charge transfer to induce a charge-transfer state,which was first demonstrated to accept electrons from electron donors.The resulting long-lived reduced photosensitizer was confirmed to trigger consecutive intermolecular electron transfers for boosting CO2-to-CO conversion.Remarkably,the Earth-abundant catalytic system with Z-6 and Fe-catalyst exhibits outstanding performance with a turnover number of＞20 000 and 29.7％quantum yield,representing excellent catalytic performance among the molecular catalytic systems and highly superior to that of noble-metal photosensitizer Ir(ppy)2(bpy)+under similar conditions.Experimental and theoretical investigations comprehensively unveil the structure-activity relationship,opening up a new horizon for the development of Earth-abundant strong sensitizing chromophores for boosting artificial photosynthesis.

Zn complexphotocatalysisCO2 reductioncharge transferphotosensitizer

Song Guo、Fu-Gui Zeng、Xiao-Di Li、Kai-Kai Chen、Ping Wang、Tong-Bu Lu、Zhi-Ming Zhang

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Institute for New Energy Materials and Low Carbon Technologies,School of Materials Science& Engineering,Tianjin University of Technology,Tianjin 300384,China

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNatural Science Foundation of Tianjin City of ChinaNatural Science Foundation of Tianjin City of China

22171209220711809216110318JCJQJC4770017JCQNJC05100

2024

10.1093/nsr/nwae130

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ISSN：
年,卷(期)：2024.11(6)
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