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用于碱性光催化析氢的NiOTe纳米点上HO和H吸附的同步优化。

Synchronous optimization of HO and H adsorption on NiOTe nanodots for alkaline photocatalytic H evolution.

作者信息

Yang Xian, Long Haoyu, Zhang Xidong, 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.

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

出版信息

J Colloid Interface Sci. 2025 Jan;677(Pt A):359-368. doi: 10.1016/j.jcis.2024.07.223. Epub 2024 Jul 29.

Abstract

Suitable HO and H adsorption on the surface of transition metal chalcogenide cocatalyst is highly required to achieve their excellent alkaline H-evolution rate. However, the weak adsorption of HO and H atoms on NiTe surface greatly hinders its alkaline H-evolution efficiency. Herein, an electron-deficient modulation strategy is proposed to synchronously improve the adsorption of HO and H atoms on NiTe surface, which can greatly improve the alkaline photocatalytic H evolution of TiO. In this case, highly electronegative oxygen atoms are introduced into the NiTe cocatalysts to induce the formation of electron-deficient Ni and Te sites in the ultra-small-sized NiOTe nanodots (0.5-2 nm), which can be uniformly loaded onto the TiO surface to prepare the NiOTe/TiO photocatalysts by a facile complexation-photodeposition strategy. The resulting NiOTe/TiO (0.6:0.4) photocatalyst exhibits the optimal activity (2143.36 μmol g h), surpassing the activity levels of TiO and NiTe/TiO samples by 42.3 and 1.8 times, respectively. The experimental and theoretical investigations have revealed that the presence of highly electronegative O atoms in the NiOTe cocatalyst can redistribute the charges of Ni and Te atoms for the formation of electron-deficient Ni and Te active sites, thereby synchronously enhancing the adsorption of HO on Ni sites and H on Te sites and promoting alkaline photocatalytic H evolution. The current research about the synchronous optimization of the HO and H adsorption offers a significant approach to design high-performance H-evolution materials.

摘要

为了实现优异的碱性析氢速率,过渡金属硫族化物助催化剂表面需要合适的羟基(HO)和氢(H)吸附。然而,HO和H原子在NiTe表面的弱吸附极大地阻碍了其碱性析氢效率。在此,提出了一种缺电子调制策略,以同步提高HO和H原子在NiTe表面的吸附,这可以大大提高TiO的碱性光催化析氢性能。在这种情况下,将高电负性的氧原子引入NiTe助催化剂中,以诱导在超小尺寸的NiOTe纳米点(0.5 - 2纳米)中形成缺电子的Ni和Te位点,这些位点可以通过简便的络合 - 光沉积策略均匀地负载在TiO表面上,从而制备出NiOTe/TiO光催化剂。所得的NiOTe/TiO(0.6:0.4)光催化剂表现出最佳活性(2143.36 μmol g⁻¹ h⁻¹),分别比TiO和NiTe/TiO样品的活性水平高出42.3倍和1.8倍。实验和理论研究表明,NiOTe助催化剂中高电负性O原子的存在可以重新分布Ni和Te原子的电荷,形成缺电子的Ni和Te活性位点,从而同步增强HO在Ni位点上的吸附以及H在Te位点上的吸附,并促进碱性光催化析氢。目前关于HO和H吸附同步优化的研究为设计高性能析氢材料提供了一种重要方法。

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