Cu3Pt1 alloys confined by penta-coordinate Al3+ on Al2O3 realize CO oxidation at room temperature

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-11-05 DOI:10.1016/j.mcat.2024.114664
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Abstract

CO is a ubiquitous air pollutant, frequently encountered in the fields of automotive exhaust purification, especial in the cold-start-emission stage. Pt based catalysts are widely used to purify CO into CO2 owing to their exceptional performance. But they can be few excited to exhibit reasonable catalytic activity due to the low temperature at the cold-start-emission stage. In exhaust gas purification catalysts used by fossil fuel-based vehicles, Al2O3 is used frequently. But there are rarely reports of Pt loaded Al2O3 catalysts achieving feasible activity of CO oxidation at room temperature. Herein, we prepared CuxPty alloy/Al2O3 catalysts (with high penta-coordinated Al3+ (AlV)), AlV centers as binding sites for Cu3Pt1 alloys on Al2O3 enable the high dispersion and stability of Cu3Pt1 alloy. The adsorption capacity of O2 and CO molecules on Cu3Pt1 surface are stronger than the case on Pt surface, which may make O2 and CO molecules more easily activated, making the CO oxidation reaction easier. In addition, the desorption of CO2 from CuxPty surface is easier compared to that on Pt surface, increasing the frequency of use of active sites there. Therefore, this Cu3Pt1/Al2O3 catalyst exhibits 100 % conversion of CO with a GHSV of 6×103 mL·g−1cat·h−1 at room temperature. This work provides a feasible guideline for the design and synthesis of Pt loaded Al2O3 catalysts toward room temperature CO oxidation.

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五配位 Al3+ 在 Al2O3 上限制的 Cu3Pt1 合金在室温下实现 CO 氧化
一氧化碳是一种无处不在的空气污染物,在汽车尾气净化领域,特别是在冷启动排放阶段经常会遇到。铂基催化剂由于性能优异,被广泛用于将 CO 净化为 CO2。但由于冷启动排放阶段的温度较低,这些催化剂很少能表现出合理的催化活性。在化石燃料汽车使用的废气净化催化剂中,Al2O3 被频繁使用。但很少有报道称负载铂的 Al2O3 催化剂能在室温下实现可行的 CO 氧化活性。在此,我们制备了 CuxPty 合金/Al2O3 催化剂(具有高五配位 Al3+(AlV)),AlV 中心是 Cu3Pt1 合金在 Al2O3 上的结合位点,使 Cu3Pt1 合金具有高分散性和稳定性。Cu3Pt1 表面对 O2 和 CO 分子的吸附能力比 Pt 表面强,这可能使 O2 和 CO 分子更容易被激活,从而使 CO 氧化反应更容易进行。此外,与铂表面相比,CuxPty 表面更容易解吸 CO2,从而增加了活性位点的使用频率。因此,这种 Cu3Pt1/Al2O3 催化剂在室温下的 CO 转化率为 100%,GHSV 为 6×103 mL-g-1cat-h-1。这项工作为设计和合成用于室温 CO 氧化的负载铂的 Al2O3 催化剂提供了可行的指导。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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