INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Lu Lu,Xinlei Ji,Xuewei Wang,Fangming Jin,Xi Chen
5-Hydroxymethylfurfural (5-HMF) is one of the top valuable platform chemicals that can be derived from biomass. Herein, a facile, mild, and efficient catalytic conversion method was developed to convert chitin biomass into 5-HMF in lithium bromide molten salt hydrates (LiBr MSHs) with boric acid (BA) as the catalyst. About 49.6% 5-HMF yield was obtained from glucosamine (GlcN) in 65 wt % LiBr MSHs at 130 °C for 2 h with 800% BA addition. The system is applicable to other sugars, and the C2-substituted group of sugars played a significant role in the 5-HMF yield. The 5-HMF yields were 81.3, 40.3, and 3.9% from fructose, glucose, and N-acetyl glucosamine (GlcNAc), respectively, under identical conditions. Combined with acid addition and Box–Behnken experiment designs, the direct conversion of chitosan and chitin were achieved at 140 °C for 5 h to produce 5-HMF with 21.6 and 15.3% yield. Ammonia quantitative analysis and NMR tests have been conducted, based on which a plausible reaction pathway was proposed. The LiBr MSHs and the BA catalyst facilitated the hydrolysis, deacetylation, and ring-opening of chitin biomass. Especially, the catalyst BA played a key role in the formation of 5-HMF, as it was found to promote dehydration at the last step. The study put forward new avenues for chitin refinery to produce high-value furanic platform chemicals in cheap and green solvent systems.
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FOOD SCIENCE AND BIOTECHNOLOGY
·
2022
·Vol. 31
·期 13
·1741-1751
·
IF 3.231
Ding Haomiao,Zhang Yuzhe,Zha Yue,Zhou Sijia,Cao Chaoqing,Zhu Huajian,Xu Feng,Zhang Xiuqiang,Wang Caisheng
The cytoprotective and potential molecular mechanisms of Hylocereus polyrhizus protein (RFPP) were investigated on the hydrogen peroxide (H 2 O 2 )-triggered damage in normal human embryonic lung (MRC-5) cells. An MTT assay was conducted to assess the MRC-5 cell viability after exposure to H 2 O 2 or RFPP. Cell cycle distribution and apoptosis were explored via flow cytometry. The contents of related proteins were assessed via western blot. MRC-5 cells exhibited markedly decreased cellular viability after treatment with H 2 O 2 ; however, treatment with RFPP suppressed this decrease. Additionally, RFPP interference dampened H 2 O 2 -triggered intracellular apoptosis levels and increased H 2 O 2 -triggered intracellular S phase. In these processes, the contents of phosphorylated ( p )-AKT along with p -mTOR proteins were downregulated in 120 µM H 2 O 2 -treated cells compared with vehicle-treated cells. Nevertheless, in MRC-5 cells inoculated with RFPP, the levels expression of these proteins were reversed. To conclude, RFPP protected MRC-5 cells from H 2 O 2 -triggered damage via activation of the PI3K/AKT/mTOR cascade.
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PubMed
高影响因子
Microbial Cell Factories
·
2022
·Vol. 21
·期 1
·1-15
·
IF 6.352
Zhang Zhen,Yu Zichen,Wang Jinduo,Yu Yifa,Li Lanxiao,Sun Pengjie,Fan Xiaoguang,Xu Qingyang
Background 5-hydroxytryptophan (5-HTP), the direct biosynthetic precursor of the neurotransmitter 5-hydroxytryptamine, has been shown to have unique efficacy in the treatment of a variety of disorders, including depression, insomnia, and chronic headaches, and is one of the most commercially valuable amino acid derivatives. However, microbial fermentation for 5-HTP production continues to face many challenges, including low titer/yield and the presence of the intermediate L-tryptophan (L-Trp), owing to the complexity and low activity of heterologous expression in prokaryotes. Therefore, there is a need to construct an efficient microbial cell factory for 5-HTP production.Results We describe the systematic modular engineering of wild-type Escherichia coli for the efficient fermentation of 5-HTP from glucose. First, a xylose-induced T7 RNA polymerase-PT7 promoter system was constructed to ensure the efficient expression of each key heterologous pathway in E. coli. Next, a new tryptophan hydroxylase mutant was used to construct an efficient tryptophan hydroxylation module, and the cofactor tetrahydrobiopterin synthesis and regeneration pathway was expressed in combination. The L-Trp synthesis module was constructed by modifying the key metabolic nodes of tryptophan biosynthesis, and the heterologous synthesis of 5-HTP was achieved. Finally, the NAD(P)H regeneration module was constructed by the moderate expression of the heterologous GDHesi pathway, which successfully reduced the surplus of the intermediate L-Trp. The final engineered strain HTP11 was able to produce 8.58 g/L 5-HTP in a 5-L bioreactor with a yield of 0.095 g/g glucose and a maximum real-time productivity of 0.48 g/L/h, the highest values reported by microbial fermentation.Conclusion In this study, we demonstrate the successful design of a cell factory for high-level 5-HTP production, combined with simple processes that have potential for use in industrial applications in the future. Thus, this study provides a reference for the production of high-value amino acid derivatives using a systematic modular engineering strategy and a basis for an efficient engineered strain development of 5-HTP high-value derivatives.
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高影响因子
Catalysts
·
2022
·Vol. 12
·期 8
·901
·
IF 4.501
Huaigang Su,Ze Zong,Wenjing Lou,Qin Zhao,Xiaobo Wang,Xiang Feng,Yanxing Qi,Zhaoning Song
In this study, Zr active species were implanted into a ZSM-5 zeolite framework to form a solid acid catalyst through steam treatment and the liquid-solid isomorphous substitution process. The as-synthesized Zr-ZSM-5-st catalyst ensured excellent esterification of trimethylolpropane and fatty acids (FAs) to achieve a polyol ester production yield of 94.41%. Combined with N2physisorption, X-ray diffraction, Fourier transform infrared spectroscopy, ultraviolet-visible spectroscopy, transmission electron microscopy mapping, X-ray photoelectron spectroscopy, NH3temperature-programmed desorption, and inductively coupled mass plasma spectroscopy were conducted. The results revealed that the excellent performance of Zr-ZSM-5-st catalyst could be attributed to the enhanced acidity and the developed surface area and pore structure.Keywords:Zr-containing solid acid catalyst;ZSM-5 zeolite;polyol ester;esterification;lubricating ester oils
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Junrong Zeng,Wenhao Chen,Gaowei Zhang,Liang Yu,Liubiao Zhong,Ya Liu,Sanfei Zhao,Yejun Qiu
Affected by the slow kinetic oxygen evolution reaction (OER), the cell voltage of water splitting is usually beyond 1.5 V, causing high energy consumption to produce hydrogen. Herein, heterostructural Ni3N–NiMoN nanowires supported on carbon cloth (Ni3N–NiMoN/CC) are successfully fabricated, and they can act as bifunctional electrocatalysts, exhibiting a low overpotential of 74 mV at 100 mA cm–2 for hydrogen evolution reaction (HER) and a low potential of 1.39 V at 50 mA cm–2 for 5-hydroxymethylfurfural oxidation reaction (HMFOR), respectively. The HMFOR//HER device constructed by Ni3N–NiMoN/CC achieves a very low cell voltage of ∼1.29 V at 10 mA cm–2, which is 0.32 V lower than that of the OER//HER device. Specially, a value-added product of 2,5-furandicarboxylic acid is obtained. Additionally, density functional theory calculations are carried out. This work provides a promising strategy to further reduce the cell voltage to generate hydrogen by replacing OER with biomass oxidation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Haoxiang Zhu,Youdi Zhang,Xusheng Guo,Youwei Cheng,Lijun Wang,Xi Li
5-Hydroxymethylfurfural (HMF) is a high-value biomass-derived platform chemical derived from renewable biomass, which is a great alternative to petroleum-based chemicals; however, it cannot be produced on a large scale at present because of the limitation of a low HMF yield and costly production. In this work, an experimental study of one-pot production of HMF from glucose in an acetone–water solvent was conducted. The effects of inorganic salts (in specific, NaCl) on miscible solvents were studied because inorganic salts could affect the phase structure of solvents. We also study the influence of the ratio between Lewis acid and Brønsted acid (L/B) on the dehydration reaction. After parameter optimization experiments, up to 64.5% HMF yield was obtained at the condition of C0 = 1.25 w/v %, CAlCl3 = 1.25 w/v %, CHCl = 10 mmol·L–1, T = 160 °C, and o/a = 80/20, and the optimized L/B was 1.25 kg·mol–1. Finally, an economic and efficient HMF production process including HMF purification and catalyst recycling was proposed; the HMF product could be produced and separated with high recovery (∼88%) and purity (∼85%) in the process. Our findings and analysis would provide support for the choice of the reaction system and bifunctional catalyst synthesis in the subsequent industrial demonstration development.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 97
·期 7
·1695-1704
·
IF 3.709
Bao Guo,Jidong Liu,Shixiong Tang,Yida Liu,Zenan Tian,Jianhua Lv
BACKGROUND Whether waste polyethylene terephthalate (PET) can be effectively recycled is one of the main challenges of the current environmental problems. The hydrolysis of dimethyl terephthalate (DMT) to terephthalic acid (TPA) over Nb-modified HZSM-5 zeolite was studied. Nb/HZSM-5 zeolites with different loadings were prepared and characterized by X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, NH 3 -temperature programmed desorption and pyridine adsorption infrared spectroscopy. The effects of different reaction conditions on the conversion of DMT and TPA yield were investigated. RESULTS The yield of TPA strongly depends on the reaction conditions and the loading of Nb. The niobium phase exists in the form of Nb 2 O 5 on the zeolite and interacts with the surface of HZSM-5 to produce the active site of Brønsted acid. The yield of TPA is closely related to the concentration of Brønsted acid sites. On 0.6Nb/HZSM-5 catalyst, the yield of TPA is highest, at about 94%. CONCLUSION Nb/HZSM-5 catalyst has excellent catalytic activity and high stability for DMT hydrolysis. In addition, the product TPA prepared in this study can be directly applied to the current PET production supply chain, providing a promising catalytic route. © 2022 Society of Chemical Industry (SCI).
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2022
·
IF 3.119
Guangyu Xu,Fanyuan Zhang,Zhenghui Li
In this study, the solubility of 5-chloropyrazin-2-amine in four aqueous solutions (methanol, ethanol, n-propanol, and ethylene glycol (EG)) plus water was determined by a gravimetric method at temperatures ranging from T = 278.15 to 323.15 K at 101.2 kPa pressure. Experimental results indicated that 5-chloropyrazin-2-amine solubility positively increased with increasing temperature at a given solvent composition and decreased with increasing mass fraction of water in each system. The order of solubility from high to low on the mole fraction scale was as follows: methanol (0.02007, 323.15 K) > ethanol (0.01308, 323.15 K) > n-propanol (3.827 × 10–3, 323.15 K) > water (1.569 × 10–3, 323.15 K). Similarly, the solubility of 5-chloropyrazin-2-amine was higher in (methanol + water) than in the other three cosolvent mixtures. The solid phase crystal of 5-chloropyrazin-2-amine was tested by X-ray powder diffraction (XPRD) and the results showed no polymorphic transformation, solvate formation, or crystal transition during entire experiments. The experimental solubility values of 5-chloropyrazin-2-amine were correlated by three thermodynamic models. The results show that the largest relative average deviation (RAD) and root mean square deviation (RMSD) data were no more than 5.38% and 2.34 × 10–4, respectively. The Jouyban–Acree model gave the best correlation result in this study.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenlei Gu,An Pei,Shiyi Zhang,Feifei Jiang,Yanyan Jia,Qizhen Qin,Ruian Du,Zhengjian Li,Renfeng Liu,Yongcai Qiu,Keyou Yan,Yun Zhao,Cheng Liang,Guangxu Chen
The development of single-atom catalysts with effective interfaces for biomass conversion is a promising but challenging research area. In this study, a Ru1/CoOx catalyst was successfully fabricated with the impregnation method, which featured Ru single atoms on a cobalt oxide substrate. The Ru1/CoOx catalyst showed superior performance in the selective electrooxidation of 5-hydroxymethylfurfural (HMF) to produce 2,5-furandicarboxylic acid (FDCA), a high value-added product. The introduction of Ru single atoms with an ultralow loading of ∼0.5 wt % was revealed to accelerate the electroredox of Co2+/Co3+/Co4+ and improve the intrinsic activity of the CoOx substrate with an FDCA selectivity of 76.5%, which is better than that of the pristine CoOx electrocatalysts (62.7%). The interfacial synergistic effect of the Ru1/CoOx interface clarified that Ru single atoms can enhance the adsorption of HMF at the Ru1/CoOx interface, which promoted the rate-determining step of the selective C–H bond activation for FDCA production. This finding provides valuable insights into the rational design of single-atom catalysts with functional interfaces for biomass upgrading.
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高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Quan Zhang,Wei Huang,Wenhao Cui,Xingzong Dong,Guangye Liu,Yunpeng Xu,Zhongmin Liu
The acidity and porosity of zeolite catalysts are crucial parameters affecting the catalytic performance. In this work, alkali treatment and metal species loading were used to modify the porosity and acidity of ZSM-5 zeolite to prepare an efficient catalyst for the 1,2-dichloroethane cracking reaction. After optimization, the highly active catalyst Zn (1%) /ZSM-5-120 was obtained, and 78% conversion of EDC and 99% selectivity toward VCM could be achieved under the conditions of 300 °C and 3.0 h −1 (WHSV). A detailed investigation was conducted on the effects of acidity, texture properties and metal species loaded on ZSM-5 zeolite on the 1,2-dichloroethane cracking reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yuechao Yang,Danxia Xu,Baolong Zhang,Zhimin Xue,Tiancheng Mu
Electrochemical oxidation of alcohol and aldehyde to carboxylic acids is one of the most important classes of catalytic reaction. The key point for such reactions lies in the fine tailoring the catalysts to improve the reaction and energy efficiency. For such a destination, identifying descriptors which are highly related to the catalytic efficiency is a prerequisite for designing electrocatalysts. In this work, taking 5-hydroxymethylfurfural (HMF), a biomass derived platform molecule containing alcohol and aldehyde, as the main research object, we revealed for the first time that the adsorption energy of substrate molecule is an activity descriptor for electrochemical alcohol and aldehyde oxidation. Too weak substrate adsorption is not favorable to C–H/O–H bond activation and dissociation, while too strong substrate adsorption hinders the formation of enough OH ads (an important intermediate) due to the competitive adsorption of substrate molecules and OH – at limited reaction sites. The optimal catalytic activity can be achieved by adjusting the adsorption energy of substrate molecules to make them properly adsorbed on the catalyst surface. This work not only offers a guideline for the design of advanced catalysts towards the electrochemical alcohol and aldehyde oxidation (e.g., methanol, ethanol, benzyl alcohol, glycerol, glucose, furfural and HMF) for the utilization and production of renewable resources, but also benefits the design of other electrochemical catalysts.
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Molecular Catalysis
·
2021
·
IF 5.062
Qian Wang,Jie Zhang,Wenlong Jia,Xin Yu,Jiahong Chen,Yong Sun,Zuojun Wei,Shuliang Yang,Xing Tang,Xianhai Zeng,Lu Lin
Generally, 5-hydroxymethylfurfural (HMF) is used as feedstock to produce 2,5-furandicarboxylic acid (FDCA). Whereas, its poor stability in alkaline environment results in low yield of FDCA. By contrast, 5-[(formyloxy)methyl]furfural (FMF), a novel platform compound derived from HMF, with higher thermal and alkaline stability than HMF, is more promising to replace HMF as substrate for the production of FDCA. In this study, FMF was successfully converted into FDCA over MoCuO x by using NaClO as oxidant, undergoing 2,5-diformylfuran (DFF) and 5-hydroxymethylfuran-2-carboxylic acid (HMFCA) as intermediates. Under optimization condition (30 min, 40 °C), 100% yield of FDCA was obtained. Furthermore, it was also demonstrated that the yield of FDCA up to 90% was gained in 5 wt % FMF concentration. Higher oxygen species mobility and lattice oxygen ratio endowed MoCuO x excellent catalytic activity. The synergy of Mo and Cu species in MoCuO x ensured an efficient conversion of HMF to FDCA through synergistic redox couple of Mo 6+ /Mo 5+ and Cu 2+ /Cu + .
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