Atomic-Layer-Confined Doping for Atomic-Level Insights into Visible-Light Water Splitting
Atomic-Layer-Confined Doping for Atomic-Level Insights into Visible-Light Water Splitting
复制标题
原子层限制掺杂用于原子级洞察可见光水分解
DOI：
10.1002/anie.201503410
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发表时间：
2015-08-03
影响因子：
16.6
通讯作者：
Xie, Yi
中科院分区：
文献类型：
--
作者：
Lei, Fengcai;Zhang, Lei;Xie, Yi
为了在原子水平上深入了解掺杂对光催化的影响，提出了一个限制在原子层中的掺杂模型。采用层状混合中间策略实现了限制在In2S3三个原子层中的Co掺杂。密度泛函计算表明，Co离子的引入带来了几个新的能级，增加了导带最小处的态密度，导致可见光吸收急剧增加，载流子浓度增加了三倍。超快暂态吸收光谱表明，Co掺杂使电子从价带到新形成的局域态的转移时间约为1.6ps。平均恢复寿命增加25倍被认为是电子-空穴分离增加的原因。合成的共掺杂In2S3(三原子层)在1.5V下产生了1.17mAcm(-2)的光电流，分别比完美的In2S3(三原子层)和体相对应的In2S3提高了近10倍和17倍。
A model of doping confined in atomic layers is proposed for atomic-level insights into the effect of doping on photocatalysis. Co doping confined in three atomic layers of In2S3 was implemented with a lamellar hybrid intermediate strategy. Density functional calculations reveal that the introduction of Co ions brings about several new energy levels and increased density of states at the conduction band minimum, leading to sharply increased visible-light absorption and three times higher carrier concentration. Ultrafast transient absorption spectroscopy reveals that the electron transfer time of about 1.6ps from the valence band to newly formed localized states is due to Co doping. The 25-fold increase in average recovery lifetime is believed to be responsible for the increased of electron-hole separation. The synthesized Co-doped In2S3 (three atomic layers) yield a photocurrent of 1.17mAcm(-2) at 1.5V vs. RHE, nearly 10 and 17 times higher than that of the perfect In2S3 (three atomic layers) and the bulk counterpart, respectively.