Interlayer Photoelectron Transfer Boosted by Bridged Ru-IV Atoms in GaS Nanosheets for Efficient Water Splitting
Interlayer Photoelectron Transfer Boosted by Bridged Ru-IV Atoms in GaS Nanosheets for Efficient Water Splitting
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GaS 纳米片中桥接 Ru-IV 原子促进层间光电子转移，实现高效水分解
DOI：
10.1021/acsami.9b13678
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发表时间：
2019
影响因子：
9.5
通讯作者：
Yan Wensheng
中科院分区：
文献类型：
--
作者：
Li Guinan;Duan Hengli;Cheng Weiren;Wang Chao;Hu Wei;Sun Zhihu;Tan Hao;Li Na;Ji Qianqian;Wang Yao;Lu Ying;Yan Wensheng
层状纳米片（NS）催化剂上的光催化水分解在可再生氢燃料生产中引起了广泛的关注。然而，层间的弱范德华相互作用使得在光催化过程中实现光生激子的有效解离和层状催化剂内部的有效电荷转移成为一个巨大的挑战。在此，我们提出了一种高价ruiv原子的嵌入策略，以获得具有快速电子-空穴解离和光载流子寿命长的二维GaS NS光催化剂。实验和理论结果表明，嵌层的单点Ru具有“Ru1-S6”的六角形结构构型，可以作为电子捕获的高速通道，同时加速电子-空穴对的解离，促进光电子通过范德华层的输运。结果表明，制备的ru插层GaS NSs在可见光下的产氢率为340 μmol g - 1h - 1，在420 nm处的表观产率为7%，是纯GaS NSs的38倍。本研究为高效太阳能转换的高活性层状光催化剂的设计开辟了一条可行的途径。
Photocatalytic water splitting over layered nanosheet (NS) catalysts has caught a lot of attention for renewable hydrogen fuel production. However, the weak van der Waals interlayer interactions make it a great challenge to realize an effective dissociation of photogenerated excitons and efficient charge transfer across the interior of layered catalysts during the photocatalysis process. Here, we propose an intercalation strategy of high-valence RuIVatoms to render two-dimensional GaS NS photocatalysts with rapid electron–hole dissociation and long photocarrier lifetime in visible-light-driven water splitting. Experimental and theoretical results unravel that the intercalated single-site Ru, confined in interlayer of GaS NSs, with a hexagonal structural configuration of “Ru1–S6”, can serve as an electron-trapped high-speed channel toward simultaneously accelerating electron–hole pairs dissociation and promoting photoelectron transportation through the van der Waals interlayer. Consequently, the as-developed Ru-intercalated GaS NSs can give a notable H2production rate of 340 μmol g–1h–1under visible-light irradiation and an apparent yield of 7% at 420 nm, 38 times that of pure GaS NSs. This study opens up a feasible way for a new design of highly active layered photocatalysts toward high-efficiency solar energy conversion.