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A new allotrope of carbon-graphdiyne, synthesis and application in photocatalytic hydrogen evolution with surface plasmon resonance enhancement
Sustainable Energy & Fuels ( IF 5.6 ) Pub Date : 2021-07-19 , DOI: 10.1039/d1se00668a
Zhiliang Jin 1 , Yue Cao 1
Affiliation  

Graphdiyne (GDY, g-CnH2n−2) is a new type of carbon material and is a promising material for efficient photocatalytic hydrogen evolution. In this work, the GDY was successfully synthesized using a unique method based on CuI as a template. The CuI had a catalytic effect, and it can deliver copper ions (Cu+) under pyridine conditions. In addition, eosin-Y (EY) sensitized GDY located with Au nanoparticles (NPs) (EY-GA-40) had the highest H2 evolution activities achieved: 319.1 μmol after five hours under visible light irradiation, and this was 245.4 times higher than the value achieved with unmodified GDY, due to the dual electron injection (DEI) effect. The DEI effect meant that both the EY and the Au NPs could supply electrons for the GDY under illumination. The GDY had a strong ability to absorb the dye molecules, which enabled the excitation state electron of the EY to transfer to the surface of the GDY. The conduction band (CB) of the GDY is lower than the surface plasmon resonance (SPR) state of the Au NPs. Hence, the excited energetic electrons in the SPR state can be injected into the CB of GDY and thus they can participate in the hydrogen evolution reaction (HER) on the surface of GDY. Meanwhile, the LUMO potential of EY is more negative than the CB of the GDY, so the electrons can be easily injected into the CB of the GDY. Hence, the photocatalytic hydrogen evolution activity of the GDY showed a great improvement because of the DEI effect. This work not only provides a novel approach for the application of GDY but also contributes a new strategy for the modification of catalysts.

中文翻译:

一种新型碳-石墨炔同素异形体、合成及在表面等离子体共振增强光催化析氢中的应用

石墨炔(GDY,gC n H 2 n -2)是一种新型的碳材料,是一种有前途的高效光催化析氢材料。在这项工作中,使用基于 CuI 作为模板的独特方法成功合成了 GDY。CuI具有催化作用,在吡啶条件下可以释放铜离子(Cu +)。此外,位于 Au 纳米粒子 (NPs) (EY-GA-40) 的曙红-Y (EY) 敏化 GDY 具有最高的 H 2达到的进化活性:在可见光照射下 5 小时后达到 319.1 μmol,由于双电子注入 (DEI) 效应,这比未修饰的 GDY 达到的值高 245.4 倍。DEI 效应意味着 EY 和 Au NPs 都可以在光照下为 GDY 提供电子。GDY具有很强的吸附染料分子的能力,使EY的激发态电子转移到GDY表面。GDY 的导带 (CB) 低于 Au NPs 的表面等离子体共振 (SPR) 状态。因此,处于 SPR 状态的激发态高能电子可以注入 GDY 的 CB 中,从而参与 GDY 表面的析氢反应(HER)。同时,EY 的 LUMO 电位比 GDY 的 CB 更负,因此电子可以很容易地注入 GDY 的 CB。因此,由于DEI效应,GDY的光催化析氢活性显示出很大的提高。这项工作不仅为GDY的应用提供了一种新方法,而且还为催化剂的改性提供了一种新的策略。
更新日期:2021-08-17
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