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具有嵌入结构的用于耐水甲苯燃烧的Pt/CeO催化剂中的活性界面周长

Active Interfacial Perimeter in Pt/CeO Catalysts with Embedding Structure for Water-Tolerant Toluene Combustion.

作者信息

Xiao Menglan, Han Dawei, Yang Xueqin, Yu Jing, Shi Bo, Guo Yucong, Yu Xiaolin, Ge Maofa

机构信息

Flavors and Fragrance Engineering and Technology Research Center of Henan Province, College of Tobacco Science, Henan Agricultural University, Zhengzhou 450046, P. R. China.

Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China.

出版信息

Environ Sci Technol. 2024 Dec 24;58(51):22808-22817. doi: 10.1021/acs.est.4c06977. Epub 2024 Dec 9.

Abstract

Supported Pt catalysts are often subjected to severe deactivation under the conditions of high temperature and water vapor in catalytic oxidation; thus, the superior stability and water-resistant ability of catalysts have great significance for the effective degradation of volatile organic compounds (VOCs). Herein, we constructed a Pt/CeO-N catalyst with an active interfacial perimeter, in which Pt species were partially embedded in the defective CeO-N support to prevent the sintering. A significant charge transfer between Pt species and ceria in the embedding structure occurred via the Pt-CeO interface, which induced the formation of a Pt-O-Ce interfacial structure. Experimental research and theoretical calculations demonstrated that the active Pt-O-Ce interface promoted the activation and migration of lattice oxygen, thus facilitating the participation of oxygen species in toluene oxidation. Consequently, Pt/CeO-N showed excellent catalytic performance for toluene degradation. DRIFTS and DFT calculation proved that the Pt-Ov-Ce interfacial sites served as the intrinsic active center in the dissociation of HO to generate ·OH, which contributed to the formation of benzaldehyde, thus remarkably improving the water-resistant property. This study provided a facile strategy for fabricating the interfacial embedding structure to enhance the catalytic activity and water tolerance for eliminating VOCs in practical application.

摘要

负载型铂催化剂在催化氧化的高温和水蒸气条件下常常会发生严重失活;因此,催化剂优异的稳定性和耐水能力对于挥发性有机化合物(VOCs)的有效降解具有重要意义。在此,我们构建了一种具有活性界面周长的Pt/CeO-N催化剂,其中铂物种部分嵌入缺陷CeO-N载体中以防止烧结。通过Pt-CeO界面,嵌入结构中的铂物种与二氧化铈之间发生了显著的电荷转移,这诱导形成了Pt-O-Ce界面结构。实验研究和理论计算表明,活性Pt-O-Ce界面促进了晶格氧的活化和迁移,从而有利于氧物种参与甲苯氧化。因此,Pt/CeO-N对甲苯降解表现出优异的催化性能。漫反射红外傅里叶变换光谱(DRIFTS)和密度泛函理论(DFT)计算证明,Pt-Ov-Ce界面位点是HO解离生成·OH的本征活性中心,这有助于苯甲醛的形成,从而显著提高了耐水性能。本研究提供了一种简便的策略来制备界面嵌入结构,以增强催化活性和耐水性,从而在实际应用中消除VOCs。

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