Bi Wentuan, Li Xiaogang, Zhang Lei, Jin Tao, Zhang Lidong, Zhang Qun, Luo Yi, Wu Changzheng, Xie Yi
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, Anhui, China.
Nat Commun. 2015 Oct 21;6:8647. doi: 10.1038/ncomms9647.
In artificial photocatalysis, sluggish kinetics of hole transfer and the resulting high-charge recombination rate have been the Achilles' heel of photocatalytic conversion efficiency. Here we demonstrate water-soluble molecules as co-catalysts to accelerate hole transfer for improved photocatalytic H2 evolution activity. Trifluoroacetic acid (TFA), by virtue of its reversible redox couple TFA·/TFA(-), serves as a homogeneous co-catalyst that not only maximizes the contact areas between co-catalysts and reactants but also greatly promotes hole transfer. Thus K4Nb6O17 nanosheet catalysts achieve drastically increased photocatalytic H2 production rate in the presence of TFA, up to 32 times with respect to the blank experiment. The molecular co-catalyst represents a new, simple and highly effective approach to suppress recombination of photogenerated charges, and has provided fertile new ground for creating high-efficiency photosynthesis systems, avoiding use of noble-metal co-catalysts.
在人工光催化中，空穴转移动力学缓慢以及由此产生的高电荷复合率一直是光催化转化效率的致命弱点。在此，我们展示了水溶性分子作为助催化剂来加速空穴转移，以提高光催化析氢活性。三氟乙酸（TFA）凭借其可逆氧化还原对TFA·/TFA(-)充当均相助催化剂，它不仅使助催化剂与反应物之间的接触面积最大化，还极大地促进了空穴转移。因此，在TFA存在的情况下，K4Nb6O17纳米片催化剂的光催化产氢速率大幅提高，相对于空白实验提高了32倍。这种分子助催化剂代表了一种抑制光生电荷复合的全新、简单且高效的方法，并为创建高效光合作用系统提供了肥沃的新土壤，避免了使用贵金属助催化剂。
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