Self-Assembled Au/CdSe Nanocrystal Clusters for Plasmon-Mediated Photocatalytic Hydrogen Evolution
Self-Assembled Au/CdSe Nanocrystal Clusters for Plasmon-Mediated Photocatalytic Hydrogen Evolution
复制标题
自组装Au/CdSe纳米晶簇用于等离子体介导的光催化析氢
DOI：
10.1002/adma.201700803
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发表时间：
2017-07-19
影响因子：
29.4
通讯作者：
Zhang, Tierui
中科院分区：
文献类型：
--
作者：
Shi, Run;Cao, Yinhu;Zhang, Tierui
由于等离子体金属和半导体之间的吸收重叠较弱，从而限制了等离子体金属和半导体之间的能量转移，等离子体介导的光催化系统通常效率较低。在这里，我们开发了一种近理想的等离子体介导光催化体系。采用乳液自组装法制备了尺寸分别为2.8、4.6、7.2、9.0 nm的Au纳米粒子和接近3.3 nm的CdSe量子点。在可见光照射下，含有7.2 nm Au纳米颗粒的Au/Cd Se纳米碳管具有非常稳定的工作特性和显著的析氢速率，其析氢速率为73 mmolg(CDSe)(-1)h(-1)(比裸Cd Se纳米碳管高10倍)。Au纳米粒子到CdSe量子点的等离子体共振能量转移，促进了半导体中载流子的产生，抑制了体复合，从而产生了优异的光催化性能。本文所采用的制备Au/CdSe纳米碳管的方法也适用于其他等离子体介导光催化剂的构建。
Plasmon-mediated photocatalytic systems generally suffer from poor efficiency due to weak absorption overlap and thus limited energy transfer between the plasmonic metal and the semiconductor. Herein, a near-ideal plasmon-mediated photocatalyst system is developed. Au/CdSe nanocrystal clusters (NCs) are successfully fabricated through a facile emulsion-based self-assembly approach, containing Au nanoparticles (NPs) of size 2.8, 4.6, 7.2, or 9.0 nm and CdSe quantum dots (QDs) of size approximate to 3.3 nm. Under visible-light irradiation, the Au/CdSe NCs with 7.2 nm Au NPs afford very stable operation and a remarkable H-2-evolution rate of 73 mmol g(CdSe)(-1)h(-1) (10x higher than bare CdSe NCs). Plasmon resonance energy transfer from the Au NPs to the CdSe QDs, which enhances charge-carrier generation in the semiconductor and suppresses bulk recombination, is responsible for the outstanding photocatalytic performance. The approach used here to fabricate the Au/CdSe NCs is suitable for the construction of other plasmon-mediated photocatalysts.