Unraveling TiO2 phase effects on Pt single-atom catalysts for efficient CO2 conversion

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis Pub Date : 2025-06-01 DOI:10.1016/S1872-2067(25)64699-7

Xiaochun Hu , Longgang Tao , Kun Lei , Zhiqiang Sun , Mingwu Tan

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引用次数: 0

Abstract

Single-atom catalysts (SACs) offer a promising approach for maximizing noble metals utilization in catalytic processes. However, their performance in CO₂ hydrogenation is often constrained by the nature of metal-support interactions. In this study, we synthesized TiO₂ supported Pt SACs (Pt₁/TiO₂), with Pt single atoms dispersed on rutile (Pt₁/R) and anatase (Pt₁/A) phases of TiO₂ for the reverse water-gas shift (RWGS) reaction. While both catalysts maintained 100% CO selectivity over time, Pt₁/A achieved a CO₂ conversion of 7.5%, significantly outperforming Pt₁/R (3.6%). In situ diffuse reflectance infrared Fourier-transform spectroscopy and X-ray photoelectron spectroscopy revealed distinct reaction pathways: the COOH pathway was dominant on Pt₁/A, whereas the –OH + HCO pathway was more competitive on Pt₁/R. Analysis of electron metal-support interactions and energy barrier calculations indicated that Pt₁/A better stabilized metallic Pt species and facilitates more favorable reaction pathways with lower energy barriers. These findings provide valuable insights for the design of more efficient SAC systems in CO₂ hydrogenation processes.

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揭示TiO2对Pt单原子催化剂CO2高效转化的影响

单原子催化剂（SACs）为催化过程中贵金属的最大化利用提供了一种很有前途的方法。然而，它们在CO2加氢中的性能往往受到金属-载体相互作用性质的限制。在这项研究中，我们合成了TiO2负载的Pt SACs (Pt1/TiO2)，将Pt单原子分散在TiO2的金红石（Pt1/R）和锐钛矿（Pt1/A）相上，进行反向水气转换（RWGS）反应。随着时间的推移，两种催化剂都保持了100%的CO选择性，Pt1/A的CO2转化率为7.5%，明显优于Pt1/R（3.6%）。原位漫反射红外傅里叶变换光谱和x射线光电子能谱显示了不同的反应途径：COOH途径在Pt1/A上占优势，而-OH + HCO途径在Pt1/R上更具竞争性。电子金属载体相互作用分析和能量势垒计算表明，Pt1/A能更好地稳定金属Pt，并在较低的能量势垒下促进更有利的反应途径。这些发现为在CO2加氢过程中设计更高效的SAC系统提供了有价值的见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chinese Journal of Catalysis 工程技术-工程：化工

CiteScore

25.80

自引率

10.30%

发文量

235

审稿时长

1.2 months

期刊介绍： The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.