Surface modification of γ-Al2O3 with bimetallic Pt–Cu nanoparticles: role of Pt–Cu interaction in the catalytic oxidation of C3H8

IF 2.1 4区 化学 Q4 CHEMISTRY, PHYSICAL
Roberto Camposeco, Aldo. A. Rivera Cabrero, Jazmin. N. Castillo Cervantes, Rodolfo Zanella
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Abstract

The incorporation of Cu into the Pt/Al2O3 catalyst significantly promoted its performance in the catalytic oxidation of C3H8. The bimetallic Pt-Cu catalyst supported on non-reducible γ-Al2O3 revealed strong Pt-Cu interaction, as well as the highest activity toward the total oxidation of C3H8. Its performance surpassed that of the monometallic Pt/Al2O3 and Cu/Al2O3 catalysts, showing a synergetic effect while maintaining excellent stability under both dry and wet reaction conditions. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) revealed that Pt sites act as the main active centers, facilitating C3H8 adsorption due to the low-frequency bands associated with CO adsorption on low-coordination bridging Pt sites. Also, the adsorption of both C3H8 and O2 was more favorable on the Pt–Cu bimetallic surface than on the individual Pt or Cu catalysts, presumably because of the lower coordination environment of the active sites. During the in-situ reaction, intermediates such as acetates and enolates were detected, which were rapidly oxidized to CO2. Furthermore, strong Lewis acid sites and surface hydroxyl groups seemed to promote C–H bond cleavage at low temperatures.

双金属Pt-Cu纳米颗粒对γ-Al2O3的表面改性:Pt-Cu相互作用在C3H8催化氧化中的作用
Cu在Pt/Al2O3催化剂中的掺入显著提高了Pt/Al2O3催化剂对C3H8的催化氧化性能。不可还原性γ-Al2O3负载的双金属Pt-Cu催化剂表现出较强的Pt-Cu相互作用,对C3H8的总氧化活性最高。其性能优于单金属Pt/Al2O3和Cu/Al2O3催化剂,表现出协同效应,同时在干湿反应条件下均保持优异的稳定性。原位漫反射红外傅里叶变换光谱(DRIFTS)显示,Pt位是主要的活性中心,由于低配位桥接Pt位上CO吸附的低频带,促进了C3H8的吸附。此外,C3H8和O2在Pt - Cu双金属表面的吸附比单独的Pt或Cu催化剂更有利,这可能是由于活性位点的配位环境较低。在原位反应过程中,检测到醋酸酯和烯醇酯等中间体,这些中间体被迅速氧化成CO2。此外,在低温下,强路易斯酸位点和表面羟基似乎促进了C-H键的裂解。
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来源期刊
CiteScore
3.30
自引率
5.60%
发文量
201
审稿时长
2.8 months
期刊介绍: Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields: -kinetics of homogeneous reactions in gas, liquid and solid phase; -Homogeneous catalysis; -Heterogeneous catalysis; -Adsorption in heterogeneous catalysis; -Transport processes related to reaction kinetics and catalysis; -Preparation and study of catalysts; -Reactors and apparatus. Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.
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