Identification of Prime Factors to Maximize the Photocatalytic Hydrogen Evolution of Covalent Organic Frameworks
Identification of Prime Factors to Maximize the Photocatalytic Hydrogen Evolution of Covalent Organic Frameworks
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DOI：
10.1021/jacs.0c02633
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发表时间：
2020-05-27
影响因子：
15
通讯作者：
Seki, Shu
中科院分区：
文献类型：
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作者：
Ghosh, Samrat;Nakada, Akinobu;Seki, Shu
可见光驱动的水制氢(H-2)是一种很有前途的将太阳能转化为化学能并将其储存起来的策略。共价有机骨架(COF)是各类有机光催化剂中的领跑者。COFS的光催化活性取决于许多因素，如电子带隙、结晶度、比表面积、激子迁移、过渡物种的稳定性、电荷分离和传输等，然而，要同时微调所有这些因素来提高光催化活性是具有挑战性的。因此，在这份报告中，我们努力了解这些因素的相互作用，并通过结构-性质活性关系确定高效光催化H-2生产的关键因素。仔细的分子工程使我们能够优化以上所有可能影响一系列等网状COF的整体催化活性的因素。本研究确定了三个主要因素：光吸收、载流子产生及其传输，这三个因素对COFS光催化产生H-2的影响比其他因素大得多。
Visible-light-driven hydrogen (H-2) production from water is a promising strategy to convert and store solar energy as chemical energy. Covalent organic frameworks (COFs) are front runners among different classes of organic photocatalysts. The photocatalytic activity of COFs depends on numerous factors such as the electronic band gap, crystallinity, surface area, exciton migration, stability of transient species, charge separation and transport, etc. However, it is challenging to fine tune all of these factors simultaneously to enhance the photocatalytic activity. Hence, in this report, an effort has been made to understand the interplay of these factors and identify the key factors for efficient photocatalytic H-2 production through a structure-property activity relationship. Careful molecular engineering allowed us to optimize all of the above plausible factors impacting the overall catalytic activities of a series of isoreticular COFs. The present study determines three prime factors: light absorption, charge carrier generation, and its transport, which influence the photocatalytic H-2 production of COFs to a much greater extent than the other factors.