Controlled Decoration of Divalent Nickel onto CdS/CdSe Core/Shell Quantum Dots to Boost Visible-Light-Induced Hydrogen Generation in Water.

Controlled Decoration of Divalent Nickel onto CdS/CdSe Core/Shell Quantum Dots to Boost Visible-Light-Induced Hydrogen Generation in Water.
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DOI:
10.1002/cplu.201800389
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发表时间:
2018-11
期刊:
影响因子:
3.4
通讯作者:
Ping Wang;Chuanping Li;Minmin Wang;Yongdong Jin
Ping Wang;Chuanping Li;Minmin Wang;Yongdong Jin
中科院分区:
化学3区
文献类型:
--
作者:
Ping Wang;Chuanping Li;Minmin Wang;Yongdong Jin

文献摘要

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寻找一种低成本、不含贵金属的助催化剂来代替昂贵的Pt用于水中光生氢(H2)已经成为一个热门的研究课题,其中,Ni基助催化剂是有希望的和高度期望的。因此,开发新的策略和方案以获得具有高活性的镍基助催化剂是至关重要的。在此,我们开发了一种新的方法来有效地装饰二价镍到预合成的CdS/CdSe核/壳量子点(QD)。通过改变在合成过程中引入的Ni前体的量,可以容易地调节QD上的Ni浓度。进一步的分析表明,Ni ~(2+)可以很好地修饰到量子点上。令人印象深刻的是,与单独制备的两种组分相比,Ni修饰的QD显示出显著增强的H2光生性能。通过优化量子点上Ni的浓度,Ni的转换频率(TOF)和520 nm处的量子产率(Φ H2)分别达到322 h-1和12.3%。还提出了一种可能的机制,并进行了详细讨论。
The search for a low-cost, noble-metal-free cocatalyst to replace expensive Pt for hydrogen (H2 ) photogeneration in water has become a hot research topic, and among these, Ni-based cocatalysts are promising and highly desired. Developing new strategies and protocols to obtain Ni-based cocatalysts with high activity is therefore vitally important. Herein, we develop a new method to efficiently decorate divalent Ni onto pre-synthesized CdS/CdSe core/shell quantum dots (QDs). The concentration of Ni on the QDs can be easily tuned by varying the amount of the Ni precursor introduced during the synthesis. Further analyses reveal that Ni2+ can be strongly decorated onto QDs. Impressively, the Ni-decorated QDs displayed a significantly enhanced H2 photogeneration performance as compared to the two components prepared separately. Through the optimization of the Ni concentration on the QDs, the turnover frequency (TOF) with respect to Ni and quantum yield ( Φ H 2 ) at 520 nm for H2 evolution from water could reach 322 h-1 and 12.3 %, respectively. A possible mechanism has also been proposed and discussed in detail.