Unique Cation Exchange in Nanocrystal Matrix via Surface Vacancy Engineering Overcoming Chemical Kinetic Energy Barriers
Unique Cation Exchange in Nanocrystal Matrix via Surface Vacancy Engineering Overcoming Chemical Kinetic Energy Barriers
复制标题
通过表面空位工程克服化学动能障碍，在纳米晶体基质中进行独特的阳离子交换
DOI：
10.1016/j.chempr.2020.08.020
复制
发表时间：
2020-11-05
期刊：
影响因子：
23.5
通讯作者：
Zhang, Jiatao
中科院分区：
文献类型：
--
作者：
Bai, Bing;Zhao, Chongyang;Zhang, Jiatao
表面空位工程在半导体纳米晶体（SNCs）的结构定制和性能改善方面发挥着重要作用。开发可控的空位工程策略来克服多步反应中的动能障碍，有望进一步探索合成机制和功能纳米材料。在此，我们利用一种有效的表面空位工程初始化阳离子交换（SVEICE）策略，前所未有地实现了从三元CulnX(2) （X = S, Se）到Cu， In双掺杂二元CdX或ZnX SNCs的能量不利阳离子交换反应。在多组分SNC表面上顺序和选择性地形成Cu和In空位是突破动能势垒的关键。双掺杂CdS:Cu/In SNCs由于从掺杂In能级到Cu掺杂e-或t能级的辐射跃迁，其发射穿过可见-近红外区，并且该策略还可以定制辐射复合过程。进一步的能量分析和实验证实了它的多功能性。
Surface vacancy engineering played a significant role in tailoring the structure and improving the performance of semiconductor nanocrystals (SNCs). Developing controllable vacancy engineering strategies to overcome kinetic energy barriers in multi-step reactions is anticipated to explore further synthesis mechanisms and functional nanomaterials. Herein, we exploited an effective surface-vacancy-engineering-initialized cation exchange (SVEICE) strategy to realize energy-unfavored cation exchange reactions from ternary CulnX(2) (X = S, Se) to Cu, In dual-doped binary CdX, or ZnX SNCs, unprecedentedly. The sequential and selective creation of Cu and In vacancies on multi-component SNC surface is critical to break through kinetic energy barriers. The emission of dual-doped CdS:Cu/In SNCs crossed visible-NIR region due to the radiative transition from doped In level to Cu-doped e- or t-level, and the radiative recombination process could also be tailored by this strategy. Further energy analysis and experiments confirmed its versatility.