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Graphene supported plasmonic photocatalyst for hydrogen evolution in photocatalytic water splitting

机译：石墨烯负载型等离激元光催化剂在光催化水分解中析氢

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摘要

It is well known that the noble metal nanoparticles show active absorption in the visible region because of the existence of the unique feature known as surface plasmon resonance (SPR). Here we report the effect of plasmonic Au nanoparticles on the enhancement of the renewable hydrogen (H_2) evolution through photocatalytic water splitting. The plasmonic Au/graphene/ TiO_2 photocatalyst was synthesized in two steps: first the graphene/TiO_2 nanocomposites were developed by the hydrothermal decomposition process; then the Au was loaded by photodeposition. The plasmonic Au and the graphene as co-catalyst effectively prolong the recombination of the photogenerated charges. This plasmonic photocatalyst displayed enhanced photocatalytic H_2 evolution for water splitting in the presence of methanol as a sacrificial reagent. The H_2 evolution rate from the Au/graphene co-catalyst was about 9 times higher than that of a pure graphene catalyst. The optimal graphene content was found to be 1.0 wt %, giving a H_2 evolution of 1.34 mmol (i.e., 26 μmolh~(?1)), which exceeded the value of 0.56 mmol (i.e., 112 μmolh?1) observed in pure TiO_2. This high photocatalytic H_2 evolution activity results from the deposition of TiO2 on graphene sheets, which act as an electron acceptors to efficiently separate the photogenerated charge carriers. However, the Au loading enhanced the H_2 evolution dramatically and achieved a maximum value of 12 mmol (i.e., 2.4 mmolh~(?1)) with optimal loading of 2.0 wt% Au on graphene/TiO_2 composites. The enhancement of H_2 evolution in the presence of Au results from the SPR effect induced by visible light irradiation, which boosts the energy intensity of the trapped electron as well as active sites for photocatalytic activity.
机译：众所周知，由于存在称为表面等离子体激元共振（SPR）的独特特征，贵金属纳米颗粒在可见光区域显示出主动吸收。在这里，我们报告等离子Au纳米粒子通过光催化水分解对可再生氢（H_2）释放的增强作用。分两步合成了等离子Au /石墨烯/ TiO_2光催化剂：首先通过水热分解工艺制备了石墨烯/ TiO_2纳米复合材料。然后通过光沉积法加载金。等离子Au和石墨烯作为助催化剂可有效延长光生电荷的重组。这种等离子体光催化剂在甲醇作为牺牲剂的情况下，对于水分解显示出增强的光催化H_2生成。 Au /石墨烯助催化剂的H_2析出速率比纯石墨烯催化剂高约9倍。最佳石墨烯含量为1.0 wt％，H_2析出为1.34 mmol（即26μmolh〜（？1）），超过纯TiO_2中观察到的0.56 mmol（即112μmolh？1）。 。这种高的光催化H_2放出活性是由于TiO2在石墨烯片上的沉积所致，石墨烯片充当电子受体以有效分离光生电荷载流子。但是，Au负载量极大地促进了H 2的析出，并且在石墨烯/ TiO 2复合材料上的最佳负载量为2.0wt％的Au时达到了12mmol（即2.4mmolh〜（Δ1））的最大值。在金的存在下，H_2析出的增强是由可见光辐照引起的SPR效应引起的，它提高了被俘获电子的能量强度以及光催化活性的活性位点。

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