Catalysis Science & Technology
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2020
·Vol. 10
·期 7
·2231-2241
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IF 5.721
Jie Yin,Quanquan Zhang,Changjun Yang,Bingguang Zhang,Kejian Deng
Selective oxidation of glucose into gluconic acid and glucaric acid with molecular oxygen under mild conditions in only water as the solvent remains a challenge. To achieve highly selective oxidation of glucose to gluconic acid and glucaric acid, a new TiO2/HPW/CoPz composite photocatalyst was prepared through modifying TiO2 with HPW (phosphotungstic acid) and CoPz (cobalt tetra(2-hydroxymethyl-1,4-dithiin)porphyrazine), which was well characterized by Raman spectroscopy, X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS), inductively coupled plasma-mass spectrometry (ICP-MS) and scanning electron microscopy energy-dispersive spectrometry (SEM-EDS). Remarkably, it was found that this composite photocatalyst can efficiently catalyze oxidation of glucose to gluconic acid and glucaric acid with atmospheric oxygen at high selectivity in water under simulated sunlight irradiation. For example, the total selectivity for both acids can reach up to 80.4% with 22.2% glucose conversion under the optimized conditions. The excellent photocatalytic performance of the TiO2/HPW/CoPz composite was attributed to the synergistic effect between the components. To elucidate the roles of HPW and CoPz in the photocatalytic process, a series of experiments including surface photocurrent, electrochemical impedance, electron spin resonance (ESR) spectroscopy, zeta potential and adsorption behavior measurements were performed. It has been demonstrated that the presence of HPW can effectively reduce the adsorption capacity of gluconic acid and glucaric acid on the surface of the catalyst and suppress their further oxidation, resulting in a high selectivity to both acids. Meanwhile the presence of CoPz can improve the separation efficiency of photogenerated charges and accelerate the production of active species, facilitating the conversion of glucose without sacrificing the acid selectivity.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 151
·期 2
·338-343
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IF 2.482
Shi Hexian,Zhang Linfeng,Wu Yudong,Yu Rui,Peng Yang,Wang Yantao,Li Teng,Yang Weiran
Abstract Glucose and its derivatives are valuable and sustainable carbon sources that can be converted into varieties of value-added chemicals. In this study, d -glucaric acid was selectively converted to 3-iodoadipic acid (3-IAA) by hydrodeoxygenation in HI-Rh/C-H 2 system. During this process, HI was a reducing reagent, which can be regenerated in situ by metal catalyzed hydrogenation. The reaction pathway was proposed based on the intermediates identification. Under the optimal conditions, 67.2% yield of 3-IAA was obtained at 130 ℃ for 4 h. As a platform molecule, 3-IAA can be further converted to varieties of building block efficiently, such as adipic acid (AA) and 3-hydroxyadipic acid (3-HAA). Graphic Abstract
研究领域:
化学工程
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可再生资源转化
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DOI
高影响因子
Fermentation-Basel
·
2023
·Vol. 9
·期 8
·764
·
IF 3.7
Xinchao Yang,Linlin Niu,Chunjiang Ye,Yuanxiu Wang,Yuehui Liu,Fang Wang,Naxin Sun
D-glucaric acid is an important bio-based building block of polymers and is a high value-added chemical that can be used in a variety of applications. In the present study, theUdhtarget genes fromPseudomonas putidaandPseudomonas syringaewere used together to construct the expression vector pETDuet-2 × Udh. The transformants of BL21 (DE3) with vector pETDuet-2 × Udh were applied to produce glucaric acid from glucuronic acid. After optimizing the induction conditions, the highest Udh expression was achieved when 0.4 mmol·L−1isopropyl-β-d–thiogalactoside (IPTG) was added to the cell cultures at an OD600value of 0.6 followed by culturing at 26 °C for 6 h. The production of glucaric acid substantially reached 5.24 ± 0.015 g·L−1in fed-batch cultures in a 30 L tank. In the present study, a new system for glucaric acid production was established, which was more economic and friendly to the environment.Keywords:urinate dehydrogenases;pETDuet-2 × Udh;D-glucaric acid;glucuronic acid;SDS-PAGE
研究领域:
生物技术
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微生物学
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生化工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Mingfu Li,Pingjun Zhang,Jiannan Qin,Hao Cheng,Qian Yu,Liqun Jiang
Photocatalysis has demonstrated great potential in the conversion of biomass, but the design of single-atom photocatalysts for the selective upgrading of glucose is rarely achieved. Here, we report a manganese doped g-C 3 N 4 (Mn SA -CN) single-atom photocatalyst by the impregnation-pyrolysis method, which achieves 34.6% glucaric acid (GAA) yield and 72.6% glucose conversion. Physicochemical characterizations indicate that the atomically dispersed Mn N 4 sites serve as the key catalytic centers, which not only optimize the electronic structure by narrowing the band gap, but also significantly promote the separation of photo-generated charge carriers. Additionally, the free radical scavenging experiments indicated that the hydroxyl radical is the main species for promoting the photocatalytic conversion of glucose. Furthermore, the GAA yield maintained over 33.0% after the catalyst was recycled five times. DFT calculation reveals that the Mn N 4 coordination structure increases the glucose adsorption and electron transfer, thereby reducing the overall reaction energy barrier and promoting the photocatalytic synthesis of GAA. This work offers fundamental insights at the atomic level for the rational design of single-atom photocatalysts toward sustainable biomass conversion.
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DOI
高影响因子
Molecular Catalysis
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2021
·
IF 5.062
Teng Li,Guangyu Sun,Lu Xiong,Boying Zheng,Yaqi Duan,Rui Yu,Jun Jiang,Yantao Wang,Weiran Yang
As a useful chemical, furan can be produced from bio-based chemicals, such as furfural and furoic acid (FA). There were few reports on the preparation of furan from bio-based C6 aldaric acids . Herein, a new method was developed to produce furan from D-glucaric acid (GA) without transition metals, and nearly 80% yield of furan was produced in the water/toluene biphasic system with SnCl 4 at 200 °C in 2 h. 3-Hydroxy-2-pyrone (3-HP) and FA were proved to be the key intermediates in the formation of furan from GA, and the reaction pathway was proposed to be GA→ 3-HP→ FA→ furan based on the kinetic study , model substrate reaction, and isotope labeling experiments. SnCl 4 gave the highest furan yield among the common acid catalysts, and the contrast experiments suggested that H + , Cl − and Sn 4+ all have promoting effect on GA conversion to furan. This method was also applicable with other C6 aldaric acids.
研究领域:
生物化学
·
有机化学
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产品关联
DOI
高影响因子
FOOD CHEMISTRY
·
2016
·
IF 4.052
Baogang Xie,Yalan Liu,Huiqin Zou,Yong Son,Huiyun Wang,Haipeng Wang,Jianghua Shao
d -Glucaric acid (GA) derivatives exhibit anti-cancerogenic properties in vivo in apples, but quantitative information about these derivatives is limited. Hydrophilic interaction-based HPLC with ultraviolet detection or mass spectrometry was developed to quantify GA and/or d -glucaro-1,4-lacton (1,4-GL) in apples. Although the formation of 1,4-GL from GA could be the prerequisite to exert biological effects in vivo , only a small portion of GA (<5%) was identified and converted to 1,4-GL in the rat stomach. The 1,4-GL content in apples ranged from 0.3 mg/g to 0.9 mg/g, and this amount can substantiate health claims associated with apples. The amount of 1,4-GL was 1.5 times higher in Gala and the ratio of 1,4-GL to GA was lower in Green Delicious apples than those in the other varieties. Our findings suggested that the variety and maturity of apples at harvest are factors that determine 1,4-GL content.
研究领域:
食品科学
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植物化学
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营养学
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产品关联
DOI
PubMed
高影响因子
Nano Research
·
2023
·Vol. 16
·期 8
·10748-10755
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IF 9.9
Li Junhua,Jiang Yi,Zhang Xu,Huo Yidan,Du Fanglin,Tuo Yongxiao,Guo Zhiyan,Chen Dawei,Chen Shenghua
The electrooxidation of the alcohol and aldehyde molecules instead of water coupled with H 2 production has been proven to be effective for producing high-value fine chemicals under alkaline conditions. It is also noteworthy that under acidic conditions, the stability of non-noble metal water oxidation catalysts remains a great challenge due to the lattice oxygen mechanism. Hence, we coupled the biomass-derived glucose oxidation for high-value D-glucaric acid (GRA) with ultra-durable hydrogen in acid solution over a Yb-MnO 2 catalyst. The Mn 3+ regulated by Yb atoms doped in MnO 2 can effectively optimize the adsorption and desorption processes of the alcohol and aldehyde group and improve the intrinsic activity but cannot for H 2 O. The catalyst exhibited extremely high activity and stability after 50 h for glucose oxidation, inhibiting the lattice oxygen process and MnO 4− formation, while the activity was quickly lost within 0.5 h for water oxidation. Density functional theory (DFT) calculations further demonstrated that glucose oxidation reaction proceeds preferentially due to the oxidation of aldehyde group with lower adsorption-free energy (−0.4 eV) than water (Δ G > 0 eV), avoiding the lattice oxygen mechanism. This work suggests that biomass-derived glucose oxidation not only provides a cost-effective approach for high-value chemicals, but also shows an extremely potential as an alternative to acidic oxygen evolution reaction (OER) for ultradurable H 2 production.
研究领域:
生物化学
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催化化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Xinyu Bai,Qidong Hou,Hengli Qian,Yifan Nie,Tianliang Xia,Ruite Lai,Guanjie Yu,Mian Laiq Ur Rehman,Haijiao Xie,Meiting Ju
Photocatalysis has exhibited huge potential in many reactions, but the design of metal-free photocatalytic material for selective upgrading of biomass is rarely achieved. Here, we report that the metal-free photocatalyst consisted of nitrogen-deficient carbon nitride (BNCN) and chlorin e6 (Ce6) can efficiently and selectively oxidize glucose into gluconic acid and glucaric acid. Introducing nitrogen defects could significantly enhance the optical absorption and modulate the band structure. In addition, the combination of Ce6 with BNCN further improve the optical absorption property and promote effective separation of photon-generated carriers. As expected, the resultant Ce6@BNCN catalyst gave a total selectivity of gluconic acid, glucaric acid and arabinose as high as 70.9% at glucose conversion up to 62.3%, as is superior to previously reported photocatalytic systems. The mechanism for the enhancement of catalytic performance and the reaction pathway were revealed by experimental studies combined with DFT calculations.
研究领域:
化学
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材料科学
·
催化
·
可持续化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）