Maneuvering Intrinsic Instability of Metal Nanoclusters for Boosted Solar-Powered Hydrogen Production.
Maneuvering Intrinsic Instability of Metal Nanoclusters for Boosted Solar-Powered Hydrogen Production.
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DOI：
10.1021/acs.jpclett.0c02460
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发表时间：
2020-10
期刊：
影响因子：
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通讯作者：
Xiaoguo Fu;Zhiquan Wei;Shuai Xu;Xin Lin;Shuo Hou;Fang‐Xing Xiao
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文献类型：
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作者：
Xiaoguo Fu;Zhiquan Wei;Shuai Xu;Xin Lin;Shuo Hou;Fang‐Xing Xiao
原子精密金属纳米团簇(NCS)作为一种新型的光敏剂最近被开发出来，但不可避免地会受到光诱导自转变为金属纳米晶体(NYS)的影响，导致光氧化还原活性显著降低。在这里，我们从概念上演示了如何控制金属纳米管的内在不稳定性，从而巧妙地利用插入在金属纳米管与半导体界面的超薄聚二甲基氯化铵(PDDA)层辅助形成长程级联电荷转移链。肖特基型自转变金属NYS赋予的单向电子流动和PDDA层出人意料的吸电子能力同时促进了电荷转移级联，从而显著提高了可见光照射下光催化析氢性能的净效率。我们的工作开辟了新的领域，明智地利用金属纳米管固有的有害不稳定性，促进电荷转移到太阳能到氢的转化。
Atomically precise metal nanoclusters (NCs) have recently been unleashed as novel photosensitizers but inevitably suffer from light-induced self-transformation to metal nanocrystals (NYs), leading to substantially reduced photoredox activities. Herein, we conceptually demonstrate how to manipulate the intrinsic instability of metal NCs for smartly crafting long-range cascade charge transfer chain assisted by an ultrathin poly(dialyldimethylammonium chloride) (PDDA) layer that was intercalated at the interface of metal NCs and semiconductor. The unidirectional electron flow endowed by Schottky-type self-transformed metal NYs and unexpected electron-withdrawing capability of PDDA layer concurrently foster the charge transfer cascade, resulting in the markedly enhanced net efficiency of photocatalytic hydrogen evolution performances under visible light irradiation. Our work opens new frontiers for judiciously harnessing the inherent detrimental instability of metal NCs for boosted charge transfer toward solar-to-hydrogen conversion.