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铂诱导的铂@金助催化剂中的纳米化及缺电子金用于高效光催化过氧化氢生成

Platinum-induced nanolization and electron-deficient gold in platinum@gold cocatalyst for efficient photocatalytic hydrogen peroxide production.

作者信息

Yin Xinyu, Gao Duoduo, Xu Jiachao, Zhao Binbin, Wang Xuefei, Yu Jiaguo, Yu Huogen

机构信息

Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, 68 Jincheng Street, Wuhan 430078, PR China.

School of Materials Science and Engineering, and School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, PR China.

出版信息

J Colloid Interface Sci. 2025 Jan 15;678(Pt C):1249-1258. doi: 10.1016/j.jcis.2024.09.195. Epub 2024 Sep 25.

Abstract

Simultaneous optimization of the number and intensity of oxygen (O) adsorption on gold (Au) cocatalyst is highly required to greatly improve their interfacial hydrogen peroxide (HO)-production activity. However, it is a great challenge to realize the above effective modulation of Au by traditional photodeposition route. In this study, a platinum (Pt)-induced selective photodeposition method was designed to simultaneously regulate the particle size and electronic structure of Au cocatalyst for boosting the photocatalytic HO-production activity of bismuth vanadate (BiVO) via the selective deposition of Pt@Au core-shell cocatalyst. The photocatalytic results indicate that the as-prepared BiVO/Pt@Au photocatalyst achieves a considerable HO-production activity with a rate of 2752.13 μmol L (AQE = 13.76 %), which is obviously higher than that of BiVO/Pt (137.63 μmol L) and BiVO/Au (475.33 μmol L). It was found that the introduction of Pt successfully induced the formation of Au nanoparticles for enhancing the number of O adsorption. Meanwhile, the spontaneous transfer of free electrons of Au to Pt induces the generation of electron-deficient Au sites, which spontaneously enhances the O-adsorption intensity for facilitating the 2-electron oxygen reduction reaction (ORR), resulting in efficient HO production. The present strategy may be useful for more comprehensively regulating the intensity and number of O adsorption on cocatalysts to facilitate artificial photosynthesis.

摘要

为了大幅提高金(Au)助催化剂上氧(O)吸附的数量和强度,迫切需要对其进行同步优化。然而,通过传统的光沉积路线实现对Au的上述有效调控是一项巨大挑战。在本研究中,设计了一种铂(Pt)诱导的选择性光沉积方法,通过选择性沉积Pt@Au核壳助催化剂,同步调节Au助催化剂的粒径和电子结构,以提高钒酸铋(BiVO)的光催化产过氧化氢(HO)活性。光催化结果表明,所制备的BiVO/Pt@Au光催化剂具有相当可观的产HO活性,产率为2752.13 μmol L(表观量子效率AQE = 13.76%),明显高于BiVO/Pt(137.63 μmol L)和BiVO/Au(475.33 μmol L)。研究发现,Pt的引入成功诱导了Au纳米颗粒的形成,从而增加了O吸附的数量。同时,Au的自由电子自发转移到Pt上,诱导产生缺电子的Au位点,自发增强了O吸附强度,促进了2电子氧还原反应(ORR),从而实现高效的HO生成。本策略可能有助于更全面地调节助催化剂上O吸附的强度和数量,以促进人工光合作用。

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