JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2019
·Vol. 95
·期 4
·1153-1162
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IF 2.659
Yihu Ke,Xiaohua Li,Jifan Li,Chun-Ling Liu,Chunli Xu,Wen-Sheng Dong
BACKGROUND Glycerol, which is a coproduct of biodiesel production, has been identified as a key platform compound for producing various valuable chemicals. The selective catalytic oxidation of glycerol to dihydroxyacetone is very attractive. RESULTS A series of Au catalysts supported on metallic oxides, i.e. ZnO, CuO, Al 2 O 3 , Fe 2 O 3 and NiO, were studied for selective catalytic oxidation of glycerol to dihydroxyacetone under base-free conditions. Among the catalysts, Au/CuO showed the best catalytic activity (glycerol conversion of 89% and dihydroxyacetone selectivity of 82.6% at 80 °C under 10 bar of O 2 ), followed by Au/ZnO ≫ Au/NiO > Au/Al 2 O 3 ≈ Au/CuO-SD ≈ Au/Fe 2 O 3 . The catalytic behaviors of these supported Au catalysts varied depending on the Au particle size, Au oxidation state, Au–support interactions and lattice oxygen reducibility. CONCLUSION The main reasons for the high catalytic activity of Au/CuO are as follows. Firstly, the catalyst has small metallic Au particles, which are more active in cleavage of the secondary C H bond in glycerol molecules. Secondly, the interactions between Au and CuO facilitate lattice oxygen reduction, and this increases oxygen mobility, which may promote regeneration of Au–support perimeter active sites by gaseous oxygen. © 2019 Society of Chemical Industry
研究领域:
催化化学
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绿色化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2016
·
IF 7.354
Xiaomei Ning,Yuhang Li,Hao Yu,Feng Peng,Hongjuan Wang,Yanhui Yang
The group 15 metals, bismuth and antimony, play important roles in promoting noble-metal-catalyzed oxidation reactions toward high value-added chemicals. Herein, we report that the selective oxidation of glycerol to 1,3-dihydroxyacetone (DHA) catalyzed by Pt supported on N-doped carbon nanotubes (Pt/NCNT) can be significantly promoted in the presence of Bi or Sb in reaction solution. This catalyst system showed not only comparable even better performance to the Pt/NCNT with pre-loaded Bi, but also the greatly simplified catalyst preparation. It was found that the Bi-promoted Pt/NCNT underwent dynamic surface reconstruction through leaching and adsorption of Bi adatoms, due to the formation of glyceric acid. By characterizing the adsorption of Bi on Pt catalyst with high-resolution transmission electron microscopy, CO-stripping, horizontal attenuated total reflection infrared spectroscopy and X-ray photoelectron spectroscopy, it has been ascertained that Bi preferentially deposits on the step sites of Pt, and then blocks the terrace sites to promote the Pt catalyst mainly through a geometrical effect, which facilitates the activation and transformation of the secondary hydroxyl group of glycerol through the chelation between substrate and Pt–Bi sites.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Chemistry Letters
·
2018
·Vol. 16
·期 3
·1083-1088
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IF 3.125
Yi Yayi,Zhou Xuehua,Xue Likun,Wang Wenxing
Air pollution by industry and humans activities is a major health issue, notably in major cities. Secondary organic aerosols are formed by oxidation of volatile organic compounds, accounting for 20–80% of organic aerosols in the atmosphere. Secondary organic aerosols are contributing to photochemical smog in urban areas. However, the mechanisms of formation of secondary organic aerosols are still poorly understood. Here, we synthesized secondary organic aerosols by aqueous reaction of hydroxyacetone and methylamine in the dark. Products were analyzed by UV–Vis spectrophotometry and liquid chromatography–mass spectrometry-ion trap-time of flight. Results showed that all reactions fit first-order kinetics, and reactions were accelerated with reactants’ concentrations and pH. The main reaction mechanisms were aldolization of hydroxyacetone, and nucleophilic attack of methylamine to hydroxyacetone, followed by dehydration. The main products were imines, transforming the solution from colorless to deep brown, which is responsible for about 1% of light absorption by atmospheric brown carbon.
研究领域:
环境科学
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大气化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 3.7
Kejin Li,Jiahui Liu,Dajian Li,Xiaolan Chen,Chunhui Zhou
Microreactors are extensively employed in different chemical reactions owing to their benefits of superior mass and heat transfer, increased yield, safety, and simplicity of control. However, immobilizing catalysts in microreactors remains a challenging issue. In this investigation, a technique for creating Cu 2 O/montmorillonite catalyst coating, using electrostatic attraction for layer-by-layer self-assembly, was proposed. The montmorillonite film's morphology and thickness could be efficiently regulated by adjusting the degree of exfoliation and surface charge of montmorillonite, alongside layer-by-layer coating times. The Cu 2 O nanoparticles were immobilized using the flow deposition approach. The resulting Cu 2 O@Mt-MR microreactor successfully transformed glycerol into dihydroxyacetone. The conversion of glycerol and product selectivity could be controlled by adjusting the molar ratio of reactants, temperature, residence time, and Cu 2 O loading. The maximum glycerol conversion observed was 47.6%, with a 27% selectivity towards dihydroxyacetone. The study presents a technique for immobilizing montmorillonite-based catalyst coatings in capillary tubing, which can serve as a foundation for the future application of microreactors in glycerol conversion.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2025
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IF 3.7
Yuanming Feng,Yunpeng Bi,Yifei Wang,Fang Yang,Guangxing Yang,Yuguang Jin,Xiaoyue Wan,Yihu Dai,Yanhui Yang,Dan Yang,Chunmei Zhou
Graphical Supported AuPd alloy, Au@Pd core-shell, Au−Pd Janus particle and Au+Pd mixture catalysts with different configurations were prepared to selectively oxidize GLY toward DHA, in which AuPd/CNT catalyst with the strongest interaction between the Au and Pd atoms afforded the superior catalytic performance. Gold/palladium binary catalysts have been widely used to the selective oxidation of glycerol to produce value-added chemicals. However, the essential effect of the structure of Au/Pd binary catalysts on the catalytic performance has not been elucidated yet. In this work, Au, Pd, AuPd alloy, Au@Pd core-shell, and Au−Pd Janus nanoparticle catalysts prepared by sol-immobilization and photochemical deposition methods were employed to the selective oxidation of glycerol toward dihydroxyacetone (DHA). The results showed that the activation of glycerol and oxygen molecule was significantly promoted with the appropriate interaction between Au and Pd atoms. That was, the turnover frequency of glycerol and DHA generation rate over the alloyed AuPd nanoparticles were remarkably higher than those of Au@Pd core-shell and Au−Pd Janus nanoparticle catalysts. It was due to the synergistic effect of Pd and Au atoms remarkably promoted the electron transfer from Pd to Au, resulting in increasing the activity of the exposed Au sites, and moderately inhibiting the activity of the exposed Pd sites, which benefited to generate DHA rapidly. After optimizing, up to 61 % yield of DHA was achieved at 87 % glycerol conversion over the alloyed AuPd catalyst.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 45
·19206-19219
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IF 2.7
Li Cui,Fei Wang,Xiaoli Zhang,Yuewen Chen,Hai Liu,Yihu Ke,Yimin Wang,Xiya Zhang
The oxidation of glycerol to dihydroxyacetone (DHA) represents an efficient and economical process route. Although preparing Au/CuO catalysts from plant constituents has emerged as a novel approach for synthesizing biocompatible products, the complexity of plant constituents means that the active components still need to be clarified, making it challenging to control catalytic activity. In this study, we effectively separated and identified the active components of Syringa oblata Lindl. (SoL) leaf using column chromatography, and synthesized a series of Au/CuO catalysts from the different separated samples. Glycerol catalytic evaluation experiments showed that the S3 fraction, mainly consisting of phenolic substances, exhibited the highest catalytic activity, with a glycerol conversion rate of 86.6% and DHA selectivity of 82.0%, exceeding the activity of most current catalysts. A series of experiments and characterizations demonstrated the differences in reducibility and protective ability among the separated samples, and the preparation and glycerol reaction conditions for optimal performance are systematically optimized. This work provides in-depth insights into the preparation of catalysts using plant-based methods.
研究领域:
化学工程
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材料科学
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植物学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
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2017
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IF 3.101
Jie Liu,Bei-Bei Yang,Xue-Qian Wang,Chun-Ling Liu,Rong-Zhen Yang,Wen-Sheng Dong
Various metal ion-exchanged montmorillonite catalysts were prepared, characterized, and evaluated in the conversion of glucose to methyl levulinate in methanol. The bulk and surface features of these catalysts were investigated using X-ray fluorescence spectroscopy, inductively coupled plasma optical emission spectroscopy , powder X-ray diffraction, Fourier-transform infrared (FT-IR) spectroscopy, thermogravimetric analysis , scanning electron microscopy, N 2 adsorption–desorption, temperature-programmed NH 3 desorption, and pyridine adsorption FT-IR spectroscopy. Al 3 + -exchanged montmorillonite had the best activity and maximum methyl levulinate selectivity because of presence of a large number of acid sites and a good balance of Brønsted and Lewis acid sites on the catalyst. The montmorillonite catalyst can be easily recovered from the reaction mixture by filtration, and reused at least five times without any loss of activity and selectivity after treatment with H 2 O 2 solution to remove carbon species deposited on the catalyst surface .
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
RSC Advances
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2021
·Vol. 11
·期 18
·10935-10940
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IF 3.361
Junjun Shi,Fukun Li,Jie Zhang,Ning Li,Xingmin Wang,Xianming Zhang,Yunqi Liu
Efficient strategies for producing bio-based reagents from sustainable biomass are highly attractive for cost-effective sustainable manufacturing. In this study, a series of eco-friendly Zr-based catalysts (basic zirconium carbonate, zirconium dioxide and zirconium hydroxide) were investigated for the efficient conversion of dihydroxyacetone to ethyl lactate in a one-pot system, in which basic zirconium carbonate exhibited the best performance with 100% dihydroxyacetone conversion and 85.3% EL (ethyl lactate) yield at 140 °C, 4.0 h and 1.0 MPa N2. The improved activity of basic zirconium carbonate could be attributed to the synergistic effect among acid and base active sites. Furthermore, this low-cost catalyst shows improved thermochemical stability and recyclability under optimal conditions, where no significant decrease in activity was observed after three runs. This catalytic process could be identified as a promising alternative to produce ethyl lactate from renewable biomass and its derivatives.
研究领域:
生物化学
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催化化学
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绿色化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Xilong Yang,Yadan Luo,Jiayue Xue,Zelin Yang,Tianxu Feng,Wei Shan,Hongwen Zhang,Hua Tang
Developing high-efficiency, long-term stable photoanodes to harness solar energy for photoelectrocatalytic (PEC) glycerol oxidation into value-added chemicals is pivotal for advancing green chemistry. However, controlling selectivity while achieving high efficiency and stability poses a significant challenge in photoelectrode design. Here, a BiVO 4 /CuWO 4 (abbreviated as BVO/CWO) heterojunction photoanode was synthesized via an electrodeposition method followed by spin-coating. Under AM 1.5G illumination, the BVO/CWO photoanode achieves a glycerol oxidation current density of 1.55 mA ∙ cm −2 at 1.23 V RHE , maintaining approximately 99 % stability after a 10-hour stability test. The production rate of 1,3-dihydroxyacetone (DHA) for BVO/CWO photoanode reaches 140.3 mmol m −2 h −1 at 1.4 V RHE , representing a nearly 12-fold increase compared to CuWO 4 (12.1 mmol m −2 h −1 ), while the DHA selectivity improves to 50.1 % from 12.5 %. This enhanced performance is attributed to the heterojunction with strong interface interaction within BVO/CWO, which generates a greater photovoltage driving force and improves bulk charge transport efficiency. Introducing the BiVO 4 layer on the CuWO 4 accelerates interfacial reaction rates and inhibits the photo-corrosion of CuWO 4 in strongly acidic conditions. Furthermore, a self-powered system, PEC coupled with a photovoltaic cell (PV-PEC), is developed using a dual-electrode configuration. A PV-PEC device with the BVO/CWO photoanode achieves a DHA productivity of 186.9 mmol m −2 and an H 2 productivity of 416.4 mmol m −2 at an operating voltage of 1.5 V over 2.5 h, indicating the application potential of the BVO/CWO photoanode under more realistic conditions.
研究领域:
绿色化学
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材料科学
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能源转换
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
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2016
·Vol. 6
·期 17
·6551-6560
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IF 5.287
Xincheng Wang,Fengbing Liang,Chongpin Huang,Yingxia Li,Biaohua Chen
Methods to catalytically convert carbohydrates into lactic acid (LA), which is a versatile platform chemical, have been widely investigated. In this study, siliceous tin phosphates were utilized as reusable Brønsted–Lewis acid bifunctional catalysts during the conversion of 1,3-dihydroxyacetone (DHA) to LA under hydrothermal conditions. The product distribution closely depended on the reaction temperature, catalyst loading and substrate concentration. The highest LA yield of 93.8% was achieved with a complete DHA conversion at 140 °C after 5 h. The reaction was facilitated by the vast presence of Brønsted and Lewis acid sites that were confirmed by both pyridine FTIR and NH3-TPD analysis. The incorporation of silica significantly lowered the Sn content and improved the thermal stability of the tin phosphate catalysts. A possible reaction mechanism was proposed in that the Lewis and Brønsted acid sites synergistically catalyzed the conversion of pyruvaldehyde to LA, which was found to be the rate-determining step. The method allows for facile catalyst separation and recycling while expanding the applicability of silica in the field of biomass-to-chemical conversion.
研究领域:
生物化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Li Cui,Yimin Wang,Zhen Yuan,Xiaoli Zhang,Yuewen Chen,Xiya Zhang,Yihu Ke,Zhile Xiong,Hai Liu
Oxidizing glycerol (the primary by-product of biodiesel production) into 1,3-dihydroxyacetone (DHA) can significantly boost the economic feasibility of the biodiesel industry, but the catalyst deactivation remains a significant challenge. Herein, we present a novel approach that achieves a breakthrough in the conversion of glycerol to DHA through the integration of porous zeolite platform (bio-ZSM-5), derived from corn straw templates, with the traditional Au/CuO catalyst via mechanical milling. Under alkali-free conditions, the synthesized Au/CuO@bio-ZSM-5 catalyst exhibits remarkable glycerol conversion rate of 97.3% and DHA selectivity of 92.2%. Notably, the catalyst retains its efficacy with a glycerol conversion of 89.7% and DHA selectivity of 90.3% even after three regeneration cycles, surpassing all previously documented catalysts for this specific reaction. Serial characterizations and density-functional theory (DFT) calculations reveal that the incorporation of bio-ZSM-5 can modify the electronic structure of surface Au, reduce the adsorption energy of glycerol, and elevate the reduction temperature. This work is expected to provide an effective perspective for the design of catalysts with high cyclic stability.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
Nature Nanotechnology
·
2025
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IF 34.9
Teng Zhenyuan,Zhang Zhenzong,Tu Ying,Zhang Qitao,Jian Nan,Yang Liujun,Xiao Jiadong,Ding Jie,Huang Longzhen,Teruhsia Ohno,Wang Chengyin,Zhang Dengsong,Yu Han,Lu Jianmei,Su Chenliang,Liu Bin
Selective asymmetric oxidation of glycerol (GLY) to hydroxypyruvic acid (HPA) offers an attractive approach for chiral drug synthesis, but this process is highly challenging. Here we develop a photocatalytic method to achieve heterogeneous selective photooxidation of GLY to HPA over rubidium (Rb) and iridium (Ir) catalytic pairs decorated on a poly(heptazine imide) framework. The Rb sites effectively adsorb GLY molecules through the terminal –OH groups, thus inhibiting their oxidation during photoreaction, while the Ir sites enhance the oxygen reduction reaction and the in situ generated surficial oxygen-reduction radicals on Ir can protect the reactive C-centred radical intermediates produced during photooxidation. The spatial arrangement of Rb and Ir sites facilitates hydrogen extraction—an essential rate-determining step for GLY photooxidation—and protects C3 radical intermediates from overoxidation. This photocatalytic system achieves a remarkable productivity for HPA synthesis (~8,000 μmol of HPA per gram of photocatalyst per hour) under visible-light illumination.
研究领域:
化学工程
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材料科学
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光催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）