Nanomaterials
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2022
·Vol. 12
·期 21
·3771
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IF 5.719
Shizhuo Wang,Jikang Jiang,Minyan Gu,Yuanbo Song,Jiang Zhao,Zheng Shen,Xuefei Zhou,Yalei Zhang
To substitute fossil resources, it is necessary to investigate the conversion of biomass into 1,2-propanediol (1,2-PDO) as a high-value-added chemical. The Pt/deAl-Beta@Mg(OH)2catalytic system is designed to obtain a higher 1,2-PDO production yield. The optimal yield of 1,2-PDO is 34.1%. The unique shell-core structure of the catalyst demonstrates stability, with a catalytic yield of over 30% after three times of use. The primary process path from glucose to 1,2-PDO, glucose-hexitol-1,2-PDO, is speculated by the experiments of intermediate product selectivity. The alkaline catalytic mechanism of the reaction process is elucidated by studying catalyst characterization and analyzing different time courses of products. The introduction of Mg(OH)2improves the target yield by promoting the isomerization from glucose to fructose and retro-aldol condensation (RAC) conversion, with pseudo-yield increases of 76.1% and 42.1%, respectively. By studying the processes of producing lactic acid and 1,2-PDO from glucose, the glucose hydrogenolysis flow chart is improved, which is of great significance for accurately controlling 1,2-PDO production in industrial applications. The metal, acid, and alkali synergistic catalytic system constructed in this paper can provide a theoretical basis and route reference for applying biomass conversion technology in practice.Keywords:1,2-propanediol;alkaline modification;core–shell catalyst
研究领域:
生物化学
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催化化学
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DOI
PubMed
高影响因子
Sustainable Energy & Fuels
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2023
·Vol. 7
·期 20
·5156-5165
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IF 5.6
Yong Liu,Lungang Chen,Dongfeng Chi,Chenguang Wang,Xinghua Zhang,Jianguo Liu,Qi Zhang,Longlong Ma
The conversion of fructose, derived from biomass, into 1,2-propanediol (1,2-PDO) offers a promising approach for reducing the carbon footprint and achieving high atom economy. However, effective regulation of this transformation to minimize side reactions remains a challenge. In this study, a biochar supported RuWCu catalyst was developed demonstrating high activity of converting fructose to 1,2-propanediol with a favorable yield of 48.1% under optimized reaction conditions of 4 MPa H2, 210 °C, and 3 h. The calcination temperature and reduction temperature affected the states of Ru, W, and Cu, which in turn affected the metal–acid sites. Optimal results were obtained with a calcination temperature of 400 °C and a reduction temperature of 300 °C, resulting in a high yield of 1,2-PDO. The Ru0.5W36Cu7/biochar showed a good reuse potential with negligible activity loss after the fifth run. These findings contribute to the development of efficient catalysts for biomass conversion and highlight the potential of biochar-supported catalysts in sustainable chemical transformations.
研究领域:
化学工程
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可再生资源与环境科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2025
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IF 5.2
Ye Wang,Jingxiao Zhang,Hongrui Zhang,Xianbin Zheng,Xingshuo Zhang,Xingshuo Zhao,Lilei Zhang
This study investigates the thermodynamic properties and intermolecular hydrogen transfer behavior in binary mixtures of 1,2-propanediol (1,2-PD) and diethylenetriamine (DETA). Experimental measurements of density, sound velocity, and viscosity reveal significant interactions between the hydroxyl group of 1,2-PD and the amino group of DETA, leading to non-ideal mixing behaviors. The excess molar volumes, apparent molar volumes, and viscosity deviations show clear evidence of intermolecular hydrogen bonding. Theoretical calculations using density functional theory (DFT) further support the formation of hydrogen bonds, with optimized molecular structures and pathways confirming a concerted hydrogen transfer mechanism. The study identifies the pathway for hydrogen transfer and provides insights into the thermodynamic and structural changes occurring in this mixture. These findings enhance our understanding of hydrogen transfer processes between alcohol and amine and offer valuable knowledge for the design of materials with tailored properties in industrial and research applications.
研究领域:
物理化学
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材料科学
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产品关联
DOI
高影响因子
Polymers
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2022
·Vol. 14
·期 9
·1783
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IF 4.967
Qicheng Chen,Nan He,Jing Fan,Fenhong Song
Due to their splendid advantages, deep eutectic solvents have attracted high attention and are considered as analogues of ionic liquids. Deep eutectic solvents (DESs) are homogeneous mixtures formed by two or three green and cheap components through hydrogen bond, which is divided into hydrogen bond acceptors (HBA) and hydrogen bond donors (HBD). Recently, Betaine has been widely used as a hydrogen bond acceptor. In this work, four DESs were synthesized by blending betaine as HBA and 1,2-propanediol as HBD in four molar ratios (1:3.5, 1:4, 1:5, 1:6). Then, the physical properties of these DESs were measured. The density values were measured within the temperature range (293.15 K to 363.15 K) at atmospheric pressure, whereas the surface tension and viscosity data were determined in four and seven temperatures between 293.15 K and 353.15 K. The relationship between the density and surface tension with temperature have been analyzed and have been fitted as a linear function. The commonly used Arrhenius model was used to describe the dependence between viscosity and temperature. The results of this study are important not only for the DESs’ industrial applications but also for the research on their synthesis mechanism and microstructure.Keywords:deep eutectic solvents;betaine;1,2-propanediol;physical property
研究领域:
化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Polymers
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2023
·Vol. 15
·期 2
·413
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IF 5
Jialin Xu,Kuo Zhou,Linlin Qin,Zaiming Tan,Shijing Huang,Peigao Duan,Shimin Kang
The chemical recycling of end-of-life polylactic acid (PLA) plays roles in mitigating environmental pressure and developing circular economy. In this regard, one-pot tandem alcoholysis and hydrogenation of PLA was carried out to produce 1,2-propanediol, which is a bulk chemical in polymer chemistry. In more detail, the commercially available Raney Co was employed as the catalyst, and transformation was conducted in ethanol, which acted as nucleophilic reagent and solvent. Single-factor analysis and Box–Behnken design were used to optimize the reaction conditions. Under the optimized condition, three kinds of PLA materials were subjected to degradation. Additionally, 74.8 ± 5.5%, 76.5 ± 6.2%, and 71.4 ± 5.7% of 1,2-propanediol was yielded from PLA powder, particle, and straws, respectively, which provided a recycle protocol to convert polylactic acid waste into value-added chemicals.Keywords:polylactic acid;alcoholysis;hydrogenation;1,2-propanediol;PLA straws
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PROCESS BIOCHEMISTRY
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2015
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IF 2.516
Jiefeng Xiao,Zhibao Huo,Dezhang Ren,Song Zhang,Jiang Luo,Guodong Yao,Fangming Jin
A novel and efficient process for the production of 1,2-propylene glycol with high productivity and high selectivity from biomass-derived lactic acid over CuO was investigated. As a result, CuO exhibited a high catalytic activity while Zn acted as a reductant for the conversion of lactic acid to 1,2-propylene glycol. Among the various reaction parameters, such as catalysts, reductants, temperature, water filling and reaction time we investigated, a 93% yield of 1,2-propylene glycol in the presence of 0.83 mmol lactic acid, 5 mmol CuO and 30 mmol Zn with 35% water filling at 250 °C for 2 h was achieved. In addition, a carbon balance at optimum reaction conditions by TOC indicated that approximately 99% lactic acid was converted into liquid products in the transformation. In situ formed hydrogen by the oxidation of Zn in water is effective for the transformation compared to added gases hydrogen. The proposed mechanism for the conversion of lactic acid to 1,2-propylene glycol over CuO is also discussed.
研究领域:
生物化学
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催化化学
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产品关联
DOI
高影响因子
Science China-Chemistry
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2010
·Vol. 53
·期 7
·1497-1501
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IF 0
Ma Hong,Nie Xin,Cai JiaYing,Chen Chen,Gao Jin,Miao Hong,Xu Jie
The catalytic oxidation of biomass-derived polyhydroxyl compounds provides an efficient and green route for biomass resource utility. Gold nanocrystals supported on Mg(OH) 2 were synthesized by sol-immobilization method, characterized by XRD, TEM, UV-vis DRS, and tested in the selective oxidation of 1,2-propanediol to lactic acid. The gold particle size and the ratio of Au to 1,2-propanediol strongly influenced the catalytic activity. Over Au/Mg(OH) 2 with the majority of gold particles concentrated in 14–18 nm, excellent catalytic performance with 94.4% conversion and 89.3% selectivity to lactic acid has been achieved under 0.3 MPa O 2 at 60 °C for 6 h.
研究领域:
化学工程
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环境科学
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催化科学
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产品关联
DOI
CHINESE JOURNAL OF CHEMISTRY
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2020
·Vol. 38
·期 5
·439-444
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IF 3.826
Bin Zhang,Bin Chen,Mark Douthwaite,Lipeng Tang,Yibo Zhang,Meng Wang,Ding Ma
Summary of main observation and conclusion A dual-templating method was used to synthesize a series of hierarchical carbon supports containing different proportions of spherical macropores ( ca. 200 nm in diameter) and mesoporous channels ( ca. 4 nm in diameter). These and some other conventional carbon materials were subsequently impregnated with Ni and tested for the conversion of glycerol. The hierarchical catalysts exhibited a significantly higher conversion (96%) and selectivity (77%) to 1,2-propanediol, and the specificity selectivity coefficient (6.1) towards 1,2-propanediol against lactic acid was three times higher than that observed over a conventional Ni/C micro catalyst (2.1). The enhanced performance of these materials, compared with the Ni nanoparticles supported on conventional carbon supports, was attributed to their high surface areas (> 1110 m 2 ∙g −1 ) and large pore volumes ( ca . 0.4 cm 3 ∙g −1 ) permitting greater accessibility of substrate and/or intermediates to Ni active sites. Given that the concentration of accessible Ni sites in these materials is higher, a competitive benzilic-acid-rearrangement reaction to produce lactic acid was suppressed, leading to an enhanced hydrogenation selectivity to 1,2-propanediol. This study evidences the potential benefits, which can be established from utilizing hierarchical support materials in the valorization of biomass.
研究领域:
材料科学
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催化化学
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生物质能
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产品关联
DOI
高影响因子
Catalysis Science & Technology
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2022
·Vol. 12
·期 21
·6495-6506
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IF 6.177
Chao Peng Fu,Qi Ming She,Riccardo Tesser,Chun Hui Zhou
Efficient conversion of glycerol, an inevitable by-product in the transesterification process producing biodiesel, to acrylic acid (AA) and 1,2-propanediol (1,2-PDO) via a cleaner process is attractive and challenging. In this work, the simultaneous production of AA and 1,2-PDO from glycerol over Cu2O/acid-activated montmorillonite (Cu2O/MMT-H) catalysts without external oxygen and hydrogen was first reported. A 100% conversion of glycerol, 72% selectivity to AA, and 10% selectivity to 1,2-PDO were obtained under optimal conditions. The nanostructure and chemical state of Cu2O and MMT-H played important roles in the conversion of glycerol. The corresponding mechanism for the oxydehydration and hydrogenolysis of glycerol to AA and 1,2-PDO over the Cu2O/MMT-H catalysts was proposed. Dehydration of glycerol occurred at the primary carbon to form acetol which was subsequently hydrogenated to form 1,2-PDO. Acrolein was obtained by a dehydration reaction of glycerol at secondary carbon, followed by the oxidation of acrolein to AA. The Cu2O/MMT-H-150 catalysts were reused three times without significant deactivation and structural changes. This work provides a new route for producing AA and 1,2-PDO simultaneously from glycerol in a one-pot way.
研究领域:
化学工程
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催化反应
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绿色化学
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产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2014
·Vol. 111
·期 2
·633-645
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IF 0.983
Yue Chuan-Jun,Gu Li-Ping,Su Yang,Zhu Shao-Ping
Cu/MgO and MgO nested on the surface of Raney Cu were prepared by a wet-mixing method and used as catalyst for glycerol hydrogenolysis. The texture of Raney Cu/MgO was characterized by X-ray diffraction and transmission electron microscopy, Brunauer–Emmett–Teller, and CO 2 -temperature-programmed desorption techniques. Results indicated that MgO was well dispersed in the pores of Raney Cu. Moreover, Raney Cu with large specific surface area had a larger contact surface for MgO, and a new phase of Cu–MgO was produced. Glycerol hydrogenolysis was selectively catalyzed under the synergistic effect of Cu and MgO in Cu/MgO catalyst. Under the moderate conditions of 180 °C and 1 MPa H 2 , the conversion of glycerol was 36.2 wt% and the selectivity for 1,2-propanediol was ~85 wt% when chemical equilibrium.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMISTRY
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2020
·Vol. 38
·期 5
·453-457
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IF 3.826
Chuang Li,Guangyue Xu,Xiang Zhang,Yao Fu
Summary of main observation and conclusion The conversion of fructose to 1,2-propylene glycol (PG) is an important process from cellulosic biomass to high-value added chemicals. Herein, Ru-WO x /hydroxyapatite (HAP) catalyst was employed for this reaction and reached up to 91.3% yield of PG at 180 °C, 1 MPa initial hydrogen for 8 h in water. On this catalyst, Ru and WO x were highly dispersed on HAP support and they interacted with each other to form a special catalytic center. The lack of isolated Ru or RuW alloy site led to a moderate activity for hydrogenolysis and hindered the further conversion of PG to propanol. The weak basic HAP support efficiently prevented the humin formation. This precisely controlled catalyst has potential in green PG production.
研究领域:
化学工程
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可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
·
2023
·
IF 6
Jianbin Huang,Jian Zhang,Shiyao Lu,Yehao Liang,Feng-Shou Xiao
Catalytic conversion of glycerol to 1,2-propanediol is an important issue for sustainable production of fine chemicals and biodiesel . Here it is found that pure silica Beta zeolite supported copper species via hydrothermal treatment (Cu/Si-Beta-HT) are highly efficient for hydrogenolysis of glycerol to 1,2-propanediol, achieving 96.0% conversion and more than 99.9% selectivity after reaction at 240 °C for 3 h. TEM images and N 2 O titration experiments confirm the high dispersion of Cu nanoparticles in the catalyst. In addition, pyridine-adsorption FT-IR spectra and NH 3 -TPD profiles suggest the presence of copper species as Lewis acidic sites in the catalyst. The hydrogenolysis of glycerol to 1,2-propanediol mainly includes the dehydration of glycerol to acetol and hydrogenation of acetol into 1,2-propanediol, which are catalyzed by copper cations and Cu nanoparticles, respectively. In situ FT-IR spectra and kinetic studies suggest that the dehydration rate is slower than the hydrogenation rate, and the dehydration is a key step for the hydrogenolysis of glycerol to 1,2-propanediol.
研究领域:
催化化学
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可再生化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）