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Communications Chemistry · 2023 ·Vol. 6 ·期 1 ·1-9 · IF 5.9

Relationship between oxide identity and electrocatalytic activity of platinum for ethanol electrooxidation in perchlorate acidic solution

You Xinyu,Han Jiaxing,Del Colle Vinicius,Xu Yuqiang,Chang Yannan,Sun Xiao,Wang Guichang,Ji Chen,Pan Changwei,Zhang Jiujun,Gao Qingyu

Water and its dissociated species at the solid‒liquid interface play critical roles in catalytic science; e.g., functions of oxygen species from water dissociation are gradually being recognized. Herein, the relationship between oxide identity (PtOH ads , PtO ads , and PtO 2 ) and electrocatalytic activity of platinum for ethanol electrooxidation was obtained in perchlorate acidic solution over a wide potential range with an upper potential of 1.5 V (reversible hydrogen electrode, RHE). PtOH ads and α-PtO 2 , rather than PtO ads , act as catalytic centers promoting ethanol electrooxidation. This relationship was corroborated on Pt(111), Pt(110), and Pt(100) electrodes, respectively. A reaction mechanism of ethanol electrooxidation was developed with DFT calculations, in which platinum oxides-mediated dehydrogenation and hydrated reaction intermediate, geminal diol, can perfectly explain experimental results, including pH dependence of product selectivity and more active α-PtO 2 than PtOH ads . This work can be generalized to the oxidation of other substances on other metal/alloy electrodes in energy conversion and electrochemical syntheses.

研究领域: 催化科学 · 电化学 · 材料科学
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CHEMICAL ENGINEERING SCIENCE · 2026 · IF 5.1

Pt/PtO2 heterostructure enable heterolytic H2 activation for low-temperature hydrogenation of industrially relevant concentrated HMF to BHMF in water

Weizhen Xie,Yue Tang,Jiacheng Li,Yaqi Shi,Shigang Su,Yong Sun,Lu Lin,Xing Tang

The aqueous-phase hydrogenation of concentrated 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) is a crucial transformation for sustainable chemical production. However, this process is often limited by sluggish H 2 activation at low temperatures and poor selectivity arising from over-hydrogenation. Here, we develop a Pt catalyst supported on oxygen-deficient manganese oxide (Pt/MnO x –O v ), featuring finely dispersed Pt/PtO 2 domains in conjunction with abundant Pt–O–Mn interfacial ensembles. Under mild aqueous conditions (30–60 °C), the catalyst efficiently converts HMF at concentrations up to 40 wt%, delivering a BHMF yield of 90.9 %. In addition, continuous-flow operation at 30 °C sustains BHMF yields above 90 % over a cumulative operation time of 80 h, thereby demonstrating promising potential for industrial application. Mechanistic studies suggest that hydrogen is initially activated on Pt nanoparticles and subsequently undergoes in situ spillover, migrating across the Pt/PtO 2 heterostructure toward adjacent Pt–O–Mn interfacial sites. At these interfacial regions, the asymmetric electronic distribution, induced by nearby oxygen vacancies, facilitates the formation of polarized H δ+ –H δ- species. These reactive hydrogen species, together with the preferential adsorption of the carbonyl group, enable selective hydrogenation while suppressing undesired side reactions. This study demonstrates that tailoring interfacial structures is an effective strategy for improving catalytic performance in biomass upgrading.

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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2022 · IF 6.76

PtPd/molecular sieve as dual-functional monolithic adsorbent/catalyst for effective removal of trace toluene at low-temperature and their electric-heating performance

Shuangde Li,Tao Wang,Mu Zhou,Shaohua Chai,Linfeng Nie,Zhenjiang Wu,Ning Han,Yunfa Chen

A dual-functional adsorption–catalytic system for elimination of trace toluene is developed and realized over molecular sieve-hosted varied ratio of platinum and palladium catalysts. PtPd/molecular sieve exhibites PdO and PtO 2 around 2–3 nm particles with uniform loading verified by XRD, TEM, Raman and XPS. The adsorption–desorption–catalysis for trace toluene purification is evaluated on the quartz micro-reactor and the self-made electrically heated equipment. 3Pt1Pd/molecular sieve shows toluene adsorption capacity of 18.22 mg/g and desorption efficiency about 77%, together with the maximum desorption temperature at 100 °C. 3Pt1Pd/molecular sieve owns toluene conversion with 38.3% and 100% at 100 and 200 °C, accompanied with the higher CO 2 selectivity of 0.0% and 150.0%, separately, due to the higher Pd 2+ content. The catalyst displays water vapor endurance, reproducibility, and 83.0% carbon balance during the whole adsorption–desorption–catalysis within 150 min, which highlights the sustainable applicability in lean VOCs abatement. Furthermore, the possible catalytic reaction pathway of toluene oxidation is proposed based on the in-situ DRIFTS experiments.

CAS / MDL: 18496-40-7 313222-87-6
研究领域: 环境科学 · 催化 · 材料科学 · 化学工程
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