Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid

Yao, Shuang; Wang, Jinyao; Zhao, Shumin; Sun, Yinghao; Liu, Mengyuan; Zhou, Xin; Zhang, Guangyu; Jin, Xin; Feng, Xiang; Liu, Yibin; Chen, Xiaobo; Chen, De; Yang, Chaohe

doi:10.1016/j.apcatb.2020.119803

Cited by 44 publications

(36 citation statements)

References 56 publications

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“…Even for the highest studied MEG concentration of 30 wt% (4.5 M) a high GA selectivity of 85% at a very high educt to metal mole ratio of >25,000 mol MEG /mol metal was observed. In literature comparable GA selectivity is described, but significant lower MEG concentrations (0.1 M MEG [11] or 0.3 M MEG [16]) and a much lower educt to catalyst ratio of 970 mol MEG /mol metal were used [21].…”

Section: Reaction Conditionsmentioning

confidence: 99%

“…Only few works are available for the catalytic oxidation of MEG to GA or to its methyl ester. Gold, palladium, nickel, copper and platinum-based catalysts have been investigated in the catalysis of the oxidation of MEG [9][10][11][12][13][14][15][16]. Besides monometallic catalysts, which show lower activity in the oxidation of MEG to GA, more active bimetallic catalysts are also used [9,11,16].…”

Section: Introductionmentioning

confidence: 99%

“…Gold, palladium, nickel, copper and platinum-based catalysts have been investigated in the catalysis of the oxidation of MEG [9][10][11][12][13][14][15][16]. Besides monometallic catalysts, which show lower activity in the oxidation of MEG to GA, more active bimetallic catalysts are also used [9,11,16]. Griffin et al, as well as Yan et al, describe a high GA selectivity of >90%, but very low MEG concentrations are used [11,16].…”

Section: Introductionmentioning

confidence: 99%

“…Besides monometallic catalysts, which show lower activity in the oxidation of MEG to GA, more active bimetallic catalysts are also used [9,11,16]. Griffin et al, as well as Yan et al, describe a high GA selectivity of >90%, but very low MEG concentrations are used [11,16]. The liquid-phase oxidation of aldehydes and alcohols, e.g., MEG or 5-hydroxymethylfurfural (HMF), is usually carried out in alkaline solutions but also base-free conditions may be applied.…”

Section: Introductionmentioning

confidence: 99%

“…The liquid-phase oxidation of aldehydes and alcohols, e.g., MEG or 5-hydroxymethylfurfural (HMF), is usually carried out in alkaline solutions but also base-free conditions may be applied. Under base-free conditions the catalyst activity is quite low compared to alkaline conditions [16,17] which can be compensated by the use of high catalyst amounts and low educt concentrations, i.e., low educt to catalyst ratios [16,18]. Whereas the use of base-free conditions leads to low salt generation in down-stream processing to obtain the free carboxylic acid by neutralisation the need to apply high catalyst amounts is detrimental for cost reasons.…”

Section: Introductionmentioning

confidence: 99%

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Oxidation of Monoethylene Glycol to Glycolic Acid with Gold-Based Catalyst and Glycolic Acid Isolation by Electrodialysis

et al. 2021

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In this work, a highly selective and active gold-based catalyst for the oxidation of high concentrated monoethylene glycol (MEG) in aqueous solution (3 M, 20 wt%) is described. High glycolic acid (GA) selectivity was achieved under mild reaction conditions. The optimization of the catalyst composition and of the reaction conditions for the oxidation of MEG in semi-batch mode under alkaline conditions led to a GA yield of >80% with a GA selectivity of about 90% in short reaction time. The bimetallic catalyst 0.1 wt% AuPt (9:1)/CeO2 showed very high activity (>2000 mmolMEG/gmetalmin) in the oxidation of MEG and, contrary to other studies, an extremely high educt to metal mole ratio of >25,000 was used. Additionally, the gold–platinum catalyst showed a high GA selectivity over more than 10 runs. A very efficient and highly selective process for the GA production from MEG under industrial relevant reaction conditions was established. In order to obtain a GA solution with high purity for the subsequent polymerization, the received reaction solution containing sodium glycolate, unreacted MEG and sodium oxalate is purified by a novel down-stream process via electrodialysis. The overall GA yield of the process exceeds 90% as unreacted MEG can be recycled.

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Section: Reaction Conditionsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Oxidation of Monoethylene Glycol to Glycolic Acid with Gold-Based Catalyst and Glycolic Acid Isolation by Electrodialysis

et al. 2021

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Modulating acid site spatial location of Zn/ZSM‐5 catalyst to boost the stable aromatization of hexane

et al. 2022

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Engineering acid site spatial location of zeolite catalyst harbors tremendous potential to boost catalytic performance but still remains a grand challenge for aromatization reaction. Herein, we successfully manipulate acid site spatial location inside the ZSM‐5 channels to promote the hexane aromatization via the simple SiO2 coating treatment. Multi‐techniques demonstrated that the medium strong L acid in the channel originated from the Si(Al)OZn structure is mainly retained in the Zn/ZSM‐5‐Si catalyst by covering the acid sites outside the channel. Surprisingly, there is a good linear relationship between BTEX yield and this medium strong L acid content. Based on the reaction kinetics, in situ FT‐IR and theoretical calculations, it is found that the L acid with confinement effect served as the main active site could prominently enhance the cyclization of propene intermediate and the dehydrogenation of cycloalkane due to the strong affinity between the C/H and ZnOx, and control the desorption of BTEX (mainly benzene, toluene, ethylbenzene, and p‐xylene) by weakening the binding of hydrogen proton to π electrons. Compared with the ordinary Zn/ZSM‐5 catalyst, the yield of BTEX is increased by nearly 10%, and the Zn/ZSM‐5‐Si catalyst exhibits excellent anti coking deactivation ability. This strategy together with mechanistic results may pave the rational design of efficient Zn/ZSM‐5 catalysts for aromatization reaction.

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A hybrid deep learning framework driven by data and reaction mechanism for predicting sustainable glycolic acid production performance

Zhou

Feng

et al. 2023

AIChE Journal

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Selective oxidation at low temperatures without alkali of biomass is a promising and sustainable avenue to manufacture glycolic acid (GA), a biodegradable functional material to protect the environment. However, producing glycolic acid with high selectivity and yield using the traditional research and development approach is timeconsuming and labor-intensive. To this context, a hybrid deep learning framework driven by data and reaction mechanisms for predicting GA production was proposed, considering the lack of related reaction mechanisms in the machine learning algorithms. The proposed hybrid deep learning framework involves the kinetic reaction mechanism, catalyst properties, and reaction conditions. Results showed that the fully connected residual network exhibited superior performance (average R 2 = 0.98) for the prediction of conversion rate and product yields. Then, the multi-objective optimization and experimental verification guided the research are carried out. The experimental verification is comparable to the modeling results, with errors of less than 4% for conversion rate and GA yields. The life cycle assessment further identifies that using the optimized operating parameters, the fossil energy demand and greenhouse emissions have decreased by 2.96% and 3.00%, respectively. This work provides new insight and strategy to accelerate the engineered selective oxidation for desired GA production.

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Engineering Pt-Mn2O3 interface to boost selective oxidation of ethylene glycol to glycolic acid

Cited by 44 publications

References 56 publications

Oxidation of Monoethylene Glycol to Glycolic Acid with Gold-Based Catalyst and Glycolic Acid Isolation by Electrodialysis

Oxidation of Monoethylene Glycol to Glycolic Acid with Gold-Based Catalyst and Glycolic Acid Isolation by Electrodialysis

Modulating acid site spatial location of Zn/ZSM‐5 catalyst to boost the stable aromatization of hexane

A hybrid deep learning framework driven by data and reaction mechanism for predicting sustainable glycolic acid production performance

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