ChemSusChem
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2018
·Vol. 12
·期 2
·495-502
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IF 7.411
Yunchao Feng,Mengzhu Li,Zhebang Gao,Xin Zhang,Xianhai Zeng,Yong Sun,Xing Tang,Tingzhou Lei,Lu Lin
Graphical Biomass valorization with bioderived catalysts ! Renewable and sustainable betaine-based catalysts (BX) are prepared for the production of 5-hydroxymethylfurfural (HMF) from various carbohydrates and biomass in satisfactory yields. The introduction of choline chloride (ChCl) significantly improves the HMF yield, and the catalytic activity of ChCl-derived choline-O-sulfate (ChOS) is also demonstrated. This work introduces a promising approach for the use of biomass-derived catalysts for effective valorization of biomass. Renewable and sustainable betaine-based catalysts (BX) derived from the betaine sugar industry or ChCl were developed for the production of 5-hydroxymethylfurfural (HMF) from various carbohydrates. The HMF yields in the BX-based media reached up to 88 %, 66 %, 37 % and 53 %, for the conversion of fructose, glucose, cellulose, and lignocellulosic biomass, respectively. In addition, choline-O-sulfate was synthesized and demonstrated to be an efficient catalyst for the conversion of fructose to HMF. From the perspective of green and sustainable chemistry, this work demonstrates benefits not only in the preparation of sustainable catalysts but also the green production of HMF from biomass.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Yannan Du,Hongjun Zang,Yimo Feng,Kai Wang,Yaxin Lv,Zhipeng Liu
This paper briefs the emerging strategies for the designing of catalytic systems, which direct conversion of chitin biomass monomer N -acetyl- d -glucosamine (NAG) to 3-acetylamino-5-acetylfuran was studied systemically. Twelve catalysts were investigated, and pyrazine hydrochloride ([Pyz]Cl) ionic liquid exhibited the good performance-achieving 3A5AF with yields of 36.94% from NAG . Further adding boric acid and CaCl 2 , treating at 190 °C for 60 min, the conversion rate of NAG is 100%, and the yield of 3A5AF can be increased to 69.54% in DMA. Furthermore, functional group changes before and after the reaction have been characterized by FTIR, HPLC-MS and 13 C NMR were applied to monitor the reaction process with [Pyz]Cl as the catalyst. The reactive intermediate was clearly detected by these techniques. Accordingly, a possible reaction pathway was proposed. The results of this experiment provide a mild and efficient reaction route for the degradation of biomass, and enrich the theoretical research of quaternary amine catalysts in the conversion of biomass waste into high value-added chemicals.
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Catalysts
·
2019
·Vol. 9
·期 11
·899
·
IF 3.444
Wei Xu,Lijing Gao,Guomin Xiao
Nano-sized HZSM-5 (n-HZSM-5) was synthesized and applied in the aromatization of glycerol. The effects of additives (carboxymethylcellulose sodium, NaCl, sodium alginate, etc.) on the chemical and physic properties of n-HZSM-5 during preparation were investigated. Metal modification was also investigated based on the synthesized n-HZSM-5. The results showed that the addition of carboxymethylcellulose sodium (CMC-Na), NaCl and sodium alginate (SA) led to forming smaller sizes of HZSM-5 and promoted the acid amounts of the catalysts, which increased its catalytic activities for obtaining BTX. The highest BTX yield of ~35% was obtained by SA derived n-HZSM-5, and the life of the catalyst were both obviously promoted by the additives with a highest of ~11 h by γ-(2,3-epoxypropoxy)propytrimethoxysilane (KH-560) derived n-HZSM-5. BTX yields could be improved by 40%by the addition of Zn and Cd in n-HZSM-5 while having little effect on the catalyst life.
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Catalysis Science & Technology
·
2017
·Vol. 7
·期 8
·1776-1791
·
IF 5.773
Yanming Jia,Junwen Wang,Kan Zhang,Shibin Liu,Guoliang Chen,Yufei Yang,Chuanmin Ding,Ping Liu
ZnSiF6-modified nano-sized HZSM-5 zeolites (NZ2, NZ3 and NZ4 catalysts) were prepared and investigated as catalysts for the conversion of methanol to aromatics. Moreover, the ZnNZ1 catalyst, prepared by ion exchange using zinc nitrate, was also introduced as a reference sample. The effects of modification on the framework, textural properties and acidity of the parent nano-sized HZSM-5 zeolite (NZ1) were investigated by XRD, FT-IR, 29Si MAS-NMR, SEM, N2 adsorption–desorption, ICP, NH3-TPD, infrared spectroscopy of adsorbed pyridine (Py-IR), UV-vis spectra, X-ray photoelectron spectroscopy (XPS) and n-butylamine and tert-butylamine titration. The results showed that the amount of total acid sites, especially the external surface acid sites of the NZ2, NZ3 and NZ4 catalysts, significantly decreased, which may largely be attributed to the passivation effect of SiF62− on the surface acidity of the parent NZ1 catalyst. Moreover, the amount of Lewis acid sites (L acid sites) increased, whereas the amount of Brønsted acid sites (B acid sites) obviously decreased with the introduction of zinc species. The emergence of new Zn-Lewis acid sites (⊖ZO⋯H⋯O–Zn⊕ species) was beneficial to improving the selectivity to BTX (benzene (B), toluene (T) and xylene (X)) due to their high activity for dehydroaromatization. The FT-IR spectra in the OH− vibration region and the 29Si MAS-NMR spectra show that the treatment of ZnSiF6 could effectively repair partial lattice defects of zeolite and could thus improve the catalyst stability. TG analysis of all the deactivated catalysts showed that the coke amount and the average rate of coke formation decreased over NZ2, NZ3 and NZ4 catalysts, and this may largely be ascribed to their lower surface acidity. The catalytic performance of these materials on the conversion of methanol to aromatics showed that the NZ3 catalyst had the highest selectivity to BTX of about 51.3% and the longest catalytic lifetime of about 234 h under the operating conditions of T = 425 °C, p = 0.1 MPa and WHSV = 0.8 h−1. The improvement in the selectivity to BTX and the catalyst lifetime of the NZ3 catalyst could be ascribed to the synergistic effect among the Zn-Lewis acid sites (⊖ZO⋯H⋯O–Zn⊕ species), external surface acidity and intact framework structure.
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Advanced Science
·
2024
·
IF 14.3
Qiwen Yu,Jiakai Zhang,Jiye Li,Yaodong Song,Jie Pan,Chaopeng Mei,Mengwei Cui,Qianqian He,Haifeng Wang,Huihui Li,Bo Cheng,Yan Zhang,Wenzhi Guo,Changju Zhu,Sanyang Chen
Acetaminophen (APAP) overdose is a major cause of drug-induced liver injury. Sirtuins 5 (SIRT5) has been implicated in the development of various liver diseases. However, its involvement in APAP-induced acute liver injury (AILI) remains unclear. The present study aimed to explore the role of SIRT5 in AILI. SIRT5 expression is dramatically downregulated by APAP administration in mouse livers and AML12 hepatocytes. SIRT5 deficiency not only exacerbates liver injury and the inflammatory response, but also worsens mitochondrial oxidative stress. Conversely, the opposite pathological and biochemical changes are observed in mice with SIRT5 overexpression. Mechanistically, quantitative succinylome analysis and site mutation experiments revealed that SIRT5 desuccinylated aldehyde dehydrogenase 2 (ALDH2) at lysine 385 and maintained the enzymatic activity of ALDH2, resulting in the suppression of inflammation and mitochondrial oxidative stress. Furthermore, succinylation of ALDH2 at lysine 385 abolished its protective effect against AILI, and the protective effect of SIRT5 against AILI is dependent on the desuccinylation of ALDH2 at K385. Finally, virtual screening of natural compounds revealed that Puerarin promoted SIRT5 desuccinylase activity and further attenuated AILI. Collectively, the present study showed that the SIRT5-ALDH2 axis plays a critical role in AILI progression and might be a strategy for therapeutic intervention.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Linlin Yu,Jiawei Ji,Ruoyu Chen,Qian Jia
Frequent oil spill incidents and increasing amounts of industrial wastewater pose a serious threat to the environment. The use of superhydrophobic materials to separate oil/water mixtures has attracted widespread attention. In this work, a superhydrophobic sponge based on MOF-5 was prepared to achieve efficient continuous oil–water separation and emulsion purification. HDTMS-MOF-5@PDA@MS (H-MOF-5@PDA@MS) not only exhibited superhydrophobic property (WCA = 153.8°, SA = 6.5°) but also exhibited excellent saturated adsorption capacity, with an oil adsorption capacity of 66 (petroleum ether)-168 (chloroform) g/g and oil–water separation efficiency of 99.2%. It also demonstrated efficient performance in various emulsion purification processes. Furthermore, it maintained a stable superhydrophobicity in some extreme environments. H-MOF-5@PDA@MS is expected to have wide application perspective in the fields of environmental pollution control and wastewater treatment due to its low cost, simple process, excellent oil–water separation efficiency, reusability, and environmental friendliness.
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Marine Drugs
·
2025
·Vol. 23
·期 2
·64
·
IF 5.4
Xuedong Zhang,Guangwei Yan,Xinming Liu,Jiewen Fu,Xiang Shi,Pei Cao,Yuqian Sun,Shengping Zhong,Jiale Nong,Peiqi Jiang,Yonghong Liu,Baoshun Zhang,Qingxia Yuan,Longyan Zhao
The depolymerized products and oligosaccharide fractions from sea cucumber fucosylated glycosaminoglycans (FGs) are promising anticoagulant candidates, and more novel FG-derived oligosaccharides from low-priced sea cucumbers are expected to be obtained. This study isolated 5−12 oligomers (OF1−OF3) with unusual branches from β-eliminative depolymerized products ofColochirus quadrangularisFG (CqFG). Detailed NMR analyses showed that OF1−OF3 consisted of a chondroitin 4,6-sulfates backbone and some sulfated fucosyl branches (FucS), including monosaccharides (α-l-Fuc2S4S, α-l-Fuc3S, α-l-Fuc4S, α-l-Fuc2S3S4S, and α-l-Fuc2S) and a disaccharide D-Gal3S4S-α1,3-l-Fuc2S4Swith the ratio of ~36:35:10:7:3:9, attached to the C-3 position of β-d-GlcA or its derivatives, such as α-l-Δ4,5GlcA and β-d-GlcA-ol. Unusually, α-l-Fuc3Swas the main FucS branch; no α-l-Fuc3S4Sbranch was found, and α-l-Fuc2S3S4Sand α-l-Fuc2Sbranches were also found in OF1–OF3. The OF2 and OF3 could strongly inhibit the intrinsic and common coagulation pathways. Intrinsic FXase is a target of OF2 and OF3 inhibiting the intrinsic coagulation pathways, and the unusual side chains may increase the intrinsic FXase inhibitory activity. OF2 and OF3 showed negligible bleeding risk, and less bleeding than heparin (HP), low-molecular-weight heparins (LMWHs), and CqFG. These findings support novel FG oligosaccharides with some unusual branches from low-priced sea cucumbers to be prepared as safer anticoagulants.
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ChemSusChem
·
2024
·
IF 7.5
Guo Xusheng,Qin Chuan,Si Yuxi,Lyu Xilei,Youwei Cheng
5-Hydroxymethylfurfural(HMF) is a versatile chemical synthesized from glucose dehydration catalyzed by metal chloride (MClx) in deep eutectic solvents (DESs). However, the low glucose concentration and high catalyst dosage hinder large-scale HMF production. Herein, we report an aqueous DES of tetraethylammonium bromide(TEAB)-glucose for converting concentrated glucose (40 wt%, relative to TEAB) using ultra-dilute SnCl4 (0.25 mol%), achieving a 62% yield of HMF. Ultra-dilute MClx-catalyzed selective conversion of glucose is feasible only when combining SnCl4 with Br-based DES, which is elucidated by density functional theory and molecular dynamic calculations. Using SnCl4 is essential due to its higher glucose isomerization activity than AlCl3 and CrCl3, which can be attributed to its low-barrier coordination with glucose and its barrier-free separation from fructose. Halide anions in DESs strongly interact with glucose, hindering the MClx-glucose coordination and thereby reducing MClx’s activity for glucose isomerization. Consequently, Br-based DESs facilitate higher activity of MClx than Cl-based DESs, due to the weaker interaction between halide anion and glucose. In addition, we elucidated the side reactions including condensation, polymerization, and isomerization, and proposed a reaction network. Our findings clarify the differential activity of MClx and the impact of halide anions in DESs on MClx’s activity.
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NEW JOURNAL OF CHEMISTRY
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2025
·
IF 2.5
Qianjiao Yin,Ke Yin,Sijia Weng,Fanghe Ye,Haomin Huang,Leneng Yang,Mingli Fu
Considering the significant reduction in VOCs adsorption capacity of zeolites under high humidity conditions, this study employs an optimized liquid deposition method to hydrophobically modify ZSM-5 zeolite. The effects of deposition solvent and trimethylchlorosilane (TMCS) dosage on the hydrophobicity of ZSM-5 were evaluated using a series of characterization techniques, the adsorption performance for toluene was assessed at 80% relative humidity. The results showed that grafting Si-(CH₃)₃ using the eco-friendly solvent ethyl acetate (EA) significantly improved the adsorptive capacity of ZSM-5 for toluene. The modified ZSM-5, treated with 5 ml/g TMCS and EA, exhibited superior dynamic adsorption capabilities, achieving breakthrough and saturation adsorption capacities of 64.09 mg/g and 108.21 mg/g for toluene, respectively. The ZSM-5-EA-5 material demonstrated robust thermal stability, retaining over 90% of its toluene adsorption capacity after five cycles of adsorption and desorption. Fourier transform infrared spectroscopy, in situ infrared spectroscopy, and density functional theory calculations indicate that after hydrophobic modification, the increased content of Si-(CH₃)₃ enhances the adsorption of toluene while reducing the adsorption of water, thereby improving the sieve's adsorptive efficiency for toluene.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jianlong Zhang,Jinlv Wei,Zhixiang Zhai,Huan Wen,Boyao Feng,Xizi Wu,Dexin Meng,Jia Wu,Shibin Yin
NiOOH generated in situ from pre-catalysts plays a key role in the 5-hydroxymethylfurfural electrooxidation reaction. However, the dynamic structural evolution of NiOOH remains relatively difficult and unclear. In this work, we focus on V-Ni 3 N as a case study. Density functional theory calculations, in-situ spectroscopy, and experimental results demonstrate that the V doping modulates the charge redistribution between the nickel and nitrogen in Ni 3 N and weakens the covalency of the Ni−N bonds, leading to easier formation of N vacancies and enhanced adsorption of OH* on Ni 3 N catalyst. This facilitates the transformation of the Ni−N bond into the Ni−O bond, thereby promoting the formation of active NiOOH for HMF oxidation. In addition, the doped V atoms enhance the interaction between NiOOH and HMF molecules and reduce the energy barrier of the rate-determining step. Thus, V-Ni 3 N/CC presents an excellent catalytic performance in terms of high 2,5-furandicarboxylic acid selectivity.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xu Yue,Sheng Wang,Shudong Wang
ZSM-5 zeolite adsorbents exhibit limited adsorption capacity for volatile organic compounds (VOCs) under high-humidity conditions, constraining their industrial applicability. In this study, a series of hierarchical ZSM-5 zeolites with high silica-to-alumina ratios (SARs) were successfully prepared via a facile acid pretreatment followed by surface methyl grafting. Using toluene as a representative VOC, the adsorption and desorption properties of these samples were assessed through dynamic adsorption breakthrough curves and temperature-programmed desorption (TPD) experiments. It was found that the two-step modification significantly enhanced both the breakthrough time and saturation adsorption capacity of high-SAR ZSM-5 for toluene in the presence of water vapor. AHFS-TZ5 and HCl-TZ5 exhibited superior performance, showing 53.9 % and 59.5 % enhancements in breakthrough time over ZSM-5, respectively. Specifically, the toluene adsorption capacity of AHFS-TZ5 under humid conditions (4 vol% H 2 O) reached 67.38 mg·g −1 , approximately 1.47 times higher than that of the unmodified ZSM-5. However, the hydrophobic -CH 3 groups grafted onto the ZSM-5 surface moderately hindered toluene diffusion due to increased steric hindrance. Additionally, AHFS-TZ5 exhibited excellent regeneration ability after desorption at 180 ºC, retaining 95 % of its initial adsorption capacity. This study provided a promising approach for preparing hydrophobic zeolites, offering a potential solution for efficient VOC adsorption in high-humidity flue gas environments.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2025
·
IF 4.6
Mintong Tian,Huan Gao,Purui Yu,Mingming Li,Zehua Li,Qipeng Yuan
Sulforaphane (SFA), an isothiocyanate compound derived from cruciferous plants, has garnered significant attention owing to its cancer-preventive, anti-inflammatory, and antibacterial properties. However, the presence of complex impurities, including hydrolysis by-products of glucosinolates, structural analogues of SFA, and 5-vinyl-2-thioxazolidinone (VOT), in plant extracts significantly hinders both the efficiency of purification and the safety of application. In this study, 14 compounds were successfully isolated and identified from broccoli seed extracts using preparative high-performance liquid chromatography. Additionally, an efficient separation method was developed for removing the crucial impurity VOT based on the temperature-responsive properties of β-cyclodextrin (β-CD). The results demonstrated that the selective binding of β-CD to SFA at elevated temperatures achieved a VOT removal efficiency exceeding 97% following low-temperature precipitation. Additionally, the purity of SFA was enhanced from 55.8% to 90.1%. The separation mechanism at the molecular level was validated through density functional theory calculations. The binding energy of β-CD-SFA (-81.2 kJ/mol) was significantly higher than that of β-CD-VOT (-25.6 kJ/mol). The scanning electron microscopy and energy dispersive spectroscopy results confirmed the homogeneous distribution of SFA within the complexes. This study provides an innovative approach for the large-scale preparation of high-purity SFA and ensures its safe application in functional foods.
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