Unravelling the reaction mechanism and structure-performance relationship for selective oxidation of ethylene glycol over Pt/Al2O3 catalyst

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-03-19 DOI:10.1016/j.mcat.2025.115035
Shiping Wu , Yanhong Quan , Shunan Yin , Jun Ren
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Abstract

A series of Pt/Al2O3 catalysts were fabricated by finely adjusting the amount of platinum and investigated in the selective oxidative of ethylene glycol (EG) to glycolic acid (GA) under mild neutral conditions. The 0.90Pt/Al2O3 catalyst showed the maximum turnover frequency (TOF: 1106.6 h−1) with the EG conversion of 74.2 % and GA selectivity of 90.2 %. A strong linear relationship between TOF values and Pt0concentration was revealed, confirming that Pt0 species serves as the active sites for GA formation. In addition, in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) results verify the reaction pathways of EG oxidation as follows: C2H6O2 → HOCH2CHO → HOCH2COOH. This work unraveled structure-performance relationship for the selective EG oxidation over Pt/Al2O3 catalyst, providing important guidance for the design of efficient noble catalysts especially for the oxidation reaction of polyols.

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Pt/Al2O3催化剂上乙二醇选择性氧化反应机理及结构性能关系的研究
通过精细调节铂的用量,制备了一系列Pt/Al2O3催化剂,并研究了在温和中性条件下乙二醇(EG)选择性氧化制乙醇酸(GA)的性能。0.90Pt/Al2O3催化剂表现出最大转换频率(TOF: 1106.6 h−1),EG转化率为74.2%,GA选择性为90.2%。TOF值与Pt0浓度之间存在较强的线性关系,证实Pt0是GA形成的活性位点。此外,原位漫反射红外傅里叶变换光谱(DRIFTS)结果验证了EG氧化的反应途径为:C2H6O2→HOCH2CHO→HOCH2COOH。本研究揭示了Pt/Al2O3催化剂选择性氧化EG的结构-性能关系,为设计高效贵金属催化剂,特别是多元醇氧化反应催化剂提供了重要的指导。
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阿拉丁
Chloroplatinic acid
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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