金属有机框架集成铜光敏剂和次级构筑单元负载的铁催化剂用于光催化析氢
Metal-Organic Frameworks Integrate Cu Photosensitizers and Secondary Building Unit-Supported Fe Catalysts for Photocatalytic Hydrogen Evolution.
作者信息
Pi Yunhong, Feng Xuanyu, Song Yang, Xu Ziwan, Li Zhong, Lin Wenbin
机构信息
Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States.
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China.
出版信息
J Am Chem Soc. 2020 Jun 10;142(23):10302-10307. doi: 10.1021/jacs.0c03906. Epub 2020 May 29.
We report here the synthesis of a series of metal-organic frameworks (MOFs), , comprising cuprous photosensitizing linkers (Cu-PSs) and catalytically active Fe centers supported on secondary building units (SBUs) for photocatalytic H evolution. Close proximity (∼1 nm) between Cu-PS and SBU-supported Fe sites and stabilization of Fe sites by periodically ordered SBUs led to exceptionally high H evolution activity for , with turnover numbers of up to 33 700 and turnover frequencies of up to 880 h. Photocatalytic H evolution activities of correlate with the lability of X counteranions, suggesting that open coordination environments of Fe sites generated by labile X groups facilitate the formation of Fe-hydride intermediates before hydrogen evolution. This work highlights the potential of using MOFs to integrate Earth-abundant components for solar energy utilization.
我们在此报告了一系列金属有机框架（MOF）的合成，该系列MOF由亚铜光敏连接体（Cu-PS）和负载于二级构筑单元（SBU）上的具有催化活性的铁中心组成，用于光催化析氢。Cu-PS与SBU负载的铁位点之间的紧密间距（约1 nm）以及周期性有序的SBU对铁位点的稳定作用，使得该系列MOF具有异常高的析氢活性，周转数高达33700，周转频率高达880 h⁻¹。其光催化析氢活性与X抗衡阴离子的活性相关，这表明由不稳定的X基团产生的铁位点的开放配位环境有助于在析氢之前形成氢化铁中间体。这项工作突出了利用MOF整合地球上储量丰富的组分用于太阳能利用的潜力。
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