Selective Catalytic Oxidation of Methanol on Pt-modified Cu/SSZ-13 Zeolites: A Strategy to Change the Catalytic Performance by Impregnation Sequential

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-09-03 DOI:10.1007/s10562-025-05162-x

Qingliang Zeng, Zhitao Han, Tingjun Liu, Shoujun Zhang, Shaoqin Sheng, Liangzheng Lin, Junhao Jing, Sihan Yin

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引用次数: 0

Abstract

The use of methanol as an alternative fuel for marine diesel engines increases unregulated CH₃OH emissions. A series of Pt-modified Cu/SSZ-13 catalysts were prepared using different impregnation method, which selectively catalyzed oxidation of CH₃OH (CH₃OH-SCO) to CO₂ and H₂O. Activity tests showed that Cu/Pt/SSZ-13 catalyst (Pt impregnated first, followed by Cu) displayed exceptional CH₃OH-SCO performance, achieving 100% methanol conversion at 150 °C with negligible CO and HCHO byproduct formation (< 5 ppm) across the tested temperature range. Additionally, Cu/Pt/SSZ-13 catalyst exhibited excellent SO₂ resistance and high synergistic activity for simultaneous CH₃OH and NO_x removal. Characterization results demonstrated that Cu/Pt/SSZ-13 catalyst exhibited larger pore size, higher specific surface area, abundant strong alkaline site density and elevated surface-adsorbed oxygen (O_ads) proportion. It was originated from the preferential introduction of Pt and subsequent doping of Cu enhanced the synergistic interaction at the interface of PtO_x and CuO species, which facilitated the rapid migration of reactive oxygen species, thus accelerating the methanol dehydrogenation and deep oxidation. In-situ DRIFTS results indicated that Cu/Pt/SSZ-13 inhibited the deposition of formate while promoting the rapid conversion of intermediates such as formaldehyde and formic acid to CO₂.

Graphical Abstract

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pt改性Cu/SSZ-13沸石选择性催化氧化甲醇：通过浸渍顺序改变催化性能的策略

使用甲醇作为船用柴油发动机的替代燃料增加了不受管制的CH3OH排放。采用不同浸渍法制备了一系列pt改性Cu/SSZ-13催化剂，选择性催化CH3OH （CH3OH- sco）氧化为CO2和H2O。活性测试表明，Cu/Pt/SSZ-13催化剂（先浸渍Pt，后浸渍Cu）表现出优异的CH3OH-SCO性能，在150°C下实现100%的甲醇转化率，在测试温度范围内，CO和HCHO副产物的生成（< 5ppm）可以忽略不计。此外，Cu/Pt/SSZ-13催化剂表现出优异的SO2抗性和同时去除CH3OH和NOx的高协同活性。表征结果表明，Cu/Pt/SSZ-13催化剂具有更大的孔径、更高的比表面积、丰富的强碱性位点密度和更高的表面吸附氧（Oads）比例。这是由于Pt的优先引入和随后Cu的掺杂增强了PtOx和CuO的界面协同作用，促进了活性氧的快速迁移，从而加速了甲醇的脱氢和深度氧化。原位漂移结果表明，Cu/Pt/SSZ-13抑制甲酸沉积，同时促进甲醛和甲酸等中间体快速转化为CO2。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.