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Accelerating Surface Lattice Oxygen Activation of Pt/TiO2–x by Modulating the Interface Electron Interaction for Efficient Photocatalytic Toluene Oxidation
ACS ES&T Engineering ( IF 7.4 ) Pub Date : 2023-08-31 , DOI: 10.1021/acsestengg.3c00251 Haifang Mao 1 , Mengli Xu 1 , Shuangjun Li 2 , Yuqing Ren 2 , Yun Zhao 1 , Jun Yu 1 , Qizhong Zhang 3 , Wenshu Zhao 4 , Gui Zhang 3 , Lan Yan 5 , Zhenmin Xu 1 , Zhenfeng Bian 2
ACS ES&T Engineering ( IF 7.4 ) Pub Date : 2023-08-31 , DOI: 10.1021/acsestengg.3c00251 Haifang Mao 1 , Mengli Xu 1 , Shuangjun Li 2 , Yuqing Ren 2 , Yun Zhao 1 , Jun Yu 1 , Qizhong Zhang 3 , Wenshu Zhao 4 , Gui Zhang 3 , Lan Yan 5 , Zhenmin Xu 1 , Zhenfeng Bian 2
Affiliation
The activation of surface lattice oxygen is crucial for designing highly efficient photocatalysts for volatile organic compound (VOC) purification. Herein, the Pt/TiO2–x catalyst with abundant oxygen vacancies was successfully prepared via the pyrolysis of the Pt-modified Ti metal–organic framework (MOF) under an air atmosphere. Detailed experimental results and density functional theory calculations revealed that the introduction of oxygen vacancies modulated the electronic configuration of the Pt site and enhanced the charge transfer from Ti to Pt, which created an electronic metal–support Pt–Ti interaction interface (EMSI). The established Pt–Ti interface is favorable for the activation of the surface lattice oxygen adjacent to the Pt site [identified by H2 temperature-programmed reduction (TPR), electron paramagnetic resonance (EPR), and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS)] and subsequently facilitates toluene oxidation via a direct ring opening process. This study offers a promising strategy for the design of high-performance photocatalysts for VOC oxidation.
中文翻译:
通过调节界面电子相互作用加速 Pt/TiO2–x 的表面晶格氧活化,实现高效光催化甲苯氧化
表面晶格氧的活化对于设计用于净化挥发性有机化合物(VOC)的高效光催化剂至关重要。在此,通过在空气气氛下热解Pt修饰的Ti金属有机骨架(MOF),成功制备了具有丰富氧空位的Pt/TiO 2– x催化剂。详细的实验结果和密度泛函理论计算表明,氧空位的引入调节了 Pt 位点的电子构型,增强了从 Ti 到 Pt 的电荷转移,从而形成了电子金属-载体 Pt-Ti 相互作用界面 (EMSI)。建立的 Pt-Ti 界面有利于激活 Pt 位点附近的表面晶格氧 [通过 H 2程序升温还原 (TPR)、电子顺磁共振 (EPR) 和原位漫反射红外傅里叶变换光谱鉴定(DRIFTS)],随后通过直接开环过程促进甲苯氧化。这项研究为设计用于 VOC 氧化的高性能光催化剂提供了一种有前景的策略。
更新日期:2023-08-31
中文翻译:
通过调节界面电子相互作用加速 Pt/TiO2–x 的表面晶格氧活化,实现高效光催化甲苯氧化
表面晶格氧的活化对于设计用于净化挥发性有机化合物(VOC)的高效光催化剂至关重要。在此,通过在空气气氛下热解Pt修饰的Ti金属有机骨架(MOF),成功制备了具有丰富氧空位的Pt/TiO 2– x催化剂。详细的实验结果和密度泛函理论计算表明,氧空位的引入调节了 Pt 位点的电子构型,增强了从 Ti 到 Pt 的电荷转移,从而形成了电子金属-载体 Pt-Ti 相互作用界面 (EMSI)。建立的 Pt-Ti 界面有利于激活 Pt 位点附近的表面晶格氧 [通过 H 2程序升温还原 (TPR)、电子顺磁共振 (EPR) 和原位漫反射红外傅里叶变换光谱鉴定(DRIFTS)],随后通过直接开环过程促进甲苯氧化。这项研究为设计用于 VOC 氧化的高性能光催化剂提供了一种有前景的策略。