Oxygen vacancy induced interaction between Pt and TiO2 to improve the oxygen reduction performance

X射线光电子能谱 催化作用 氧气 密度泛函理论 解吸 化学 二氧化钛 质子交换膜燃料电池 材料科学 化学工程 物理化学 计算化学 吸附 复合材料 有机化学 工程类
作者
Ziyu Wang,Xuekun Jin,Fengjuan Chen,Xuanyu Kuang,Junyong Min,Haiming Duan,Junhua Li,Jianjun Chen
出处
期刊:Journal of Colloid and Interface Science [Elsevier BV]
卷期号:650: 901-912 被引量:14
标识
DOI:10.1016/j.jcis.2023.07.024
摘要

In proton exchange membrane fuel cells (PEMFCS), a Pt-based catalyst has been plagued by activity and durability, making it difficult to implement in large-scale commercial applications. In this paper, a composite material formed by titanium dioxide and carbon black containing oxygen vacancies (TiO2(OV)-C) was used as a functional support to successfully load Pt nanoparticles (NPS). The introduction of oxygen vacancies induces the formation of a connection between Pt and TiO2, which not only strengthens the fixation of Pt by the composite support but also optimizes the local charge density of Pt. Compared with Pt/C (0.842 V) and Pt/TiO2-C (0.841 V), the half-wave potential (E1/2) of Pt/TiO2(OV)-C (0.862 V) is increased by 20 mV and 21 mV, respectively. After a long-term durability test, the E1/2 of Pt/TiO2(OV)-C is only attenuated by 5 mV. In addition, the mass activity (MA) and specific activity (SA) decreased from 183.4 mA mg-1 and 0.565 mA cm-2 to 144.4 mA mg-1 and 0.483 mA cm-2 at 0.85 V, only decreasing by 21% and 17 %, showing good stability. X-ray photoelectron spectroscopies (XPS) and density functional theory (DFT) calculations show that the interaction between Pt and TiO2 reduces the d-band center of Pt, thereby improving the desorption of intermediates *OH, which in turn promotes the activity of alkaline ORR. This study not only shows that OV plays a key role in the process of inducing interaction, but also deeply studies the influence of this interaction on the active site Pt, which provides more choices for the design of excellent multiphase catalysts.
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