Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution,Journal of the American Chemical Society

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Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-03-24 , DOI: 10.1021/jacs.6b12976
Xu-Bing Li ₁ , Yu-Ji Gao ₁ , Yang Wang ₁ , Fei Zhan ₂ , Xiao-Yi Zhang ₃ , Qing-Yu Kong ₄ , Ning-Jiu Zhao ₅ , Qing Guo ₁ , Hao-Lin Wu ₁ , Zhi-Jun Li ₁ , Ye Tao ₂ , Jian-Ping Zhang ₅ , Bin Chen ₁ , Chen-Ho Tung ₁ , Li-Zhu Wu ₁

Affiliation

Colloidal quantum dots (QDs) have demonstrated great promise in artificial photosynthesis. However, the ultrasmall size hinders its controllable and effective interaction with cocatalysts. To improve the poor interparticle electronic communication between free QD and cocatalyst, we design here a self-assembled architecture of nanoparticles, QDs and Pt nanoparticles, simply jointed together by molecular polyacrylate to greatly enhance the rate and efficiency of interfacial electron transfer (ET). The enhanced interparticle electronic communication is confirmed by femtosecond transient absorption spectroscopy and X-ray transient absorption. Taking advantage of the enhanced interparticle ET with a time scale of ∼65 ps, 5.0 mL of assembled CdSe/CdS QDs/cocatalysts solution produces 94 ± 1.5 mL (4183 ± 67 μmol) of molecular H2 in 8 h, giving rise to an internal quantum yield of ∼65% in the first 30 min and a total turnover number of >1.64 × 107 per Pt nanoparticle. This study demonstrates that self-assembly is a promising way to improve the sluggish kinetics of the interparticle ET process, which is the key step for advanced H2 photosynthesis.

中文翻译：

自组装框架增强了超小型纳米粒子的电子通信，以实现卓越的太阳能氢进化

胶体量子点 (QD) 在人工光合作用中表现出巨大的潜力。然而，超小尺寸阻碍了其与助催化剂的可控和有效相互作用。为了改善游离量子点和助催化剂之间较差的粒子间电子通信，我们在这里设计了一种纳米粒子、量子点和 Pt 纳米粒子的自组装结构，通过分子聚丙烯酸酯简单地连接在一起，以大大提高界面电子转移 (ET) 的速率和效率。飞秒瞬态吸收光谱和 X 射线瞬态吸收证实了增强的粒子间电子通信。利用时间尺度为~65 ps 的增强粒子间 ET，5.0 mL 组装的 CdSe/CdS QDs/助催化剂溶液在 8 小时内产生 94 ± 1.5 mL (4183 ± 67 μmol) 的分子 H2，在前 30 分钟内产生约 65% 的内部量子产率，并且每个 Pt 纳米颗粒的总周转数 >1.64 × 107。这项研究表明，自组装是改善粒子间 ET 过程缓慢动力学的一种有前途的方法，这是高级 H2 光合作用的关键步骤。

更新日期：2017-03-24

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