INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Liangqing Zhang,Jiarong Qiu,Jiahui Deng,Shunming Song,Zelong Hong,Wenlong Jia,Suchang Huang,Xianhai Zeng
The conversion of hemicellulosic biomass to sugar alcohols commonly applies homogeneous acids and noble metals as catalysts, which is neither economical nor environmentally friendly. In order to overcome the deficiencies of the reports, a series of non-precious catalysts were synthesized through the co-precipitation method and incipient wetness impregnation (IWI) method in converting hemicellulosic biomass, i.e., hemicellulose and xylose into sugar alcohols (i.e., xylitol and arabitol). Reaction experiments showed that the Ni 8.98 Fe 1 @ 1.54SiO 2 catalyst prepared by the IWI method has excellent catalytic performance for converting xylose to sugar alcohols in the neutral aqueous solution, and can be applied to the direct conversion of hemicellulose as well. Specifically, the optimum yield of xylitol and arabitol could obtain 99.48 mol% and 26.01 mol% for xylose as the substrate and 88.16 mol% and 20.55 mol% for hemicellulose as the substrate, respectively. Characterization techniques such as X-ray diffraction (XRD), N 2 adsorption-desorption isotherm, transmission electron microscopy (TEM), scanning electron microscope (SEM), H 2 temperature-programmed reduction (H 2 -TPR), NH 3 temperature-programmed desorption (NH 3 -TPD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy of pyridine (Py-FTIR), and SQUID vibrating sample magnetometry (SQUID -VSM) were performed to study physicochemical properties of the catalyst. N 2 adsorption-desorption isotherm and NH 3 -TPD characterizations indicated that the catalyst with mesoporous properties and proper acidic sites is vital for hydrolyzing hemicellulose to pentose (i.e., xylose and arabinose). TEM, H 2 -TPR, and XPS techniques revealed that the (111) plane of metallic Ni is the main active phase for the hydrogenation of pentose into sugar alcohols, and Fe 2+ and Fe 3+ species act as effective promoters to enhance the pentose hydrogenation. Py-FTIR characterization and reaction conditions indicated that the appropriate ratio of Brønsted to Lewis acidic sites could facilitate the conversion of xylose to arabitol. The reaction mechanisms for converting hemicellulosic biomass to sugar alcohols were proposed based on the systematic study of reaction conditions and characterizations. N 2 adsorption-desorption, H 2 -TPR, and XPS indicated that the catalyst with strong metal-support interaction, large specific surface area and pore volume could be beneficial for catalytic stability, which is verified in leaching and reusability tests. The catalyst has superparamagnetic, which can be quickly separated from the reaction system under the external magnetic field, facilitating the recovery and utilization of the catalyst.
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Molecular Catalysis
·
2023
·
IF 4.6
Shuxing Zhang,Jiali Zheng,Zhihui Li,Xiaoshu Ding,Yanji Wang
Herein, we reported a green catalytic reaction system for the synthesis of 5-amino-1-pentanol with furfural and ionic liquid hydroxylamine salt as the initial raw material. In addition, the method can obtain 2-furonitrile and furfurylamine in high yields. The reaction system comprises three new reactions, including the reaction of furfural with ionic liquid hydroxylamine salt to synthesize 2-furonitrile, the hydrogenation of 2-furonitrile to prepare furfurylamine, and the hydrogenolysis of furfurylamine to prepare 5-amino-1-pentanol. For the synthesis of 2-furonitrile, ionic liquid hydroxylamine salt (NH 2 OH) 2 ·[HSO 3 - b - mim ]·HSO 4 was prepared. The ionic liquid as co-solvents, catalysts, and hydroxylamine stabilizer has recovery and reusability. For the hydrogenation of 2-furonitrile to furfurylamine, high-efficiency Ru/g-C 3 N 4 catalyst was prepared. For the hydrogenolysis of furfurylamine to 5-amino-1-pentanol, high-efficiency Pt/ZrO 2 catalyst was prepared. Finally, the yield of 5-amino-1-pentanol based on furfural was 48.7%. A potential pathway for preparing drugs from biomass has been identified in this work.
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RARE METALS
·
2023
·
IF 8.8
Li Wu-Lin,Zhang Qing-Qing,Dong Lin,Zhang Wen-Jun,Lin Li-Li,Chen Zu-Peng
Photocatalytic reductive amination of biomass-derived aldehydes is a desirable way to selectively upgrade biomass into value-added nitrogen-containing chemicals under mild conditions. However, it is challenging to produce imines in high selectivity because of the undesirable side reactions caused by the activity of functional groups. Here, we demonstrate the highly reactive and selective production of imines from biomass derived aldehydes via the photocatalytic reductive amination, using a defective TiO 2 supported nickel catalyst. The employment of methanol as the hydrogen donor and ammonia solution as the nitrogen source avoids the use of high-pressure H 2 and expensive amines, rendering the current catalytic process safe, economical, and environmentally friendly. In depth investigations attribute the improved separation and transfer of photogenerated charge carriers to the presence of oxygen vacancies and decorated Ni nanoparticles, thereby accelerating the production of imines from benzaldehyde amination (conversion, 95.8%; selectivity, 95.2%). Furthermore, the developed system could be easily translated to the photocatalytic conversions of various biomass derived aldehydes, which provided an example of a cost-effective and sustainable approach for the valorization of biomass derived feedstocks. Graphic abstract
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INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Xiaoxuan Ma,Tianyang Guo,Peng Fu,Zhiyu Li,Kaiwei Sun,Liang Zheng,Huiyan Zhang
Aromatic hydrocarbons (AHs) production from in-situ catalytic co-pyrolysis (CCP) of biomass and plastics is a promising technology. However, the combined effects of the mixing mode and proportion of raw materials in catalytic co-pyrolysis and the double-size effect of micro-mesoporous core-shell catalysts on AHs production remain questionable. The formation characteristics and mechanism of AHs in CCP process were studied from mass transfer and free radial direction. The results showed that the yield of BTEX (benzene, toluene, ethylbenzene, and xylene) was 20.44 wt% when the mass ratio of cellulose/polyethylene/cellulose (C-P-C) was 0.5:1:0.5 at 500 ℃. The free radicals generated during the breaking of polyethylene bonds can promote the transfer of hydrogen atoms to cellulose pyrolysis intermediates, which results in mass transfer effect. The C-P-C loading mode makes hydrogen atoms always pass through the cellulose without escaping, and the increase of polyethylene ratio makes the number of hydrogen free radicals increase significantly, both of which jointly regulate the hydrogen free radical mass transfer efficiency. However, the high concentration of hydrogen free radicals can quench the pyrolysis of cellulose. The conjugated double size effect of ZSM-5 @MCM-41 leads to their greater catalytic capacity for free radical carrying co-pyrolysis products compared to ZSM-5. With the increase of mesoporous shell, the yield of BTEX increases first and then decreases, but the yield of coke is opposite. The BTEX yield of 1.0SH-Z5 @ M41 is 3.15 times that of ZSM-5, and the coke yield is only 14.70% that of ZSM-5. The reaction pathway of promoting cellulose pyrolysis by polyethylene and the mechanism of hydrogen free radical - mass transfer co-pyrolysis involved were put forward.
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BIORESOURCE TECHNOLOGY
·
2023
·
IF 11.4
Hossain M. Zabed,Suely Akter,Mudasir A. Dar,Jamila A. Tuly,Mukesh Kumar Aswathi,Junhua Yun,Jia Li,Xianghui Qi
This study aimed to produce enhanced fermentable sugars from a novel stover system through the bioprocessing of its soluble sugars and insoluble carbohydrates. The pretreatment conditions were optimized for this high sugar-containing stover (HSS) to control inhibitor formation and obtain enhanced fermentable sugar concentrations. The optimum temperature, acid loading, and reaction time for the pretreatment were 155 °C, 0.5%, and 30 min, respectively, providing up to 97.15% sugar yield and 76.51 g/L total sugars at 10% solid-load. Sugar concentration further increased to 126.9 g/L at 20% solid-load, generating 3.89 g/L acetate, 0.92 g/L 5-hydroxymethyl furfural, 0.82 g/L furfural, and 3.75 g/L total phenolics as inhibitors. To determine the effects of soluble sugars in HSS on fermentable sugar yield and inhibitor formation, sugar-removed HSS was further studied under the optimum conditions. Although prior removal of sugars exhibited a reduction in inhibitor generation, it also decreased total fermentable sugar production to 115.45 g/L.
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PubMed
高影响因子
FOOD RESEARCH INTERNATIONAL
·
2023
·
IF 8.1
Huan Liu,Junke Li,Fang Wang,Xuemei Sun,Dengyong Liu,Zhongshuai Wang,Hansheng Gong
Myosin is an ideal binding receptor for aroma compounds and its functional properties are easily affected by glucose. The study comprehensively clarified the effects of glucose glycation-induced structural modifications of myosin on its binding ability with furan derivatives, including 2-methylfuran, 2-furfural, and 2-furfurylthiol. The results demonstrated that the binding levels of furan derivatives were obviously affected by the glycation levels of myosin due to the changes of myosin structure and surface. The increased glycation levels caused the unfolding of myosin structure and accelerated the aggregation, as were exhibited by the data of zeta potential, particle size, microstructure, and secondary structure. The glycated myosin with wrinkled surfaces favored the significant increase of hydrophobic interactions (31.59–69.50 μg), the more exposure of amino acid residues (3459–6048), the formation of free sulfhydryl groups (16.37–20.58 mmol/10 4 g) and hydrogen bonds. These key (non)covalent linkages accounted for the generation of glycated myosin-odorants complex, including 2-furfurylthiol (29.17–47.87 %), thus enhancing the resultant binding ability as evidenced by the free furan derivatives concentrations, fluorescence quenching and molecular docking simulation analysis. The glycated myosin for 8 h bound highest concentrations of furan derivatives. The results will provide comprehensive data on the retention of aroma compounds in meat products.
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高影响因子
IRANIAN POLYMER JOURNAL
·
2023
·Vol. 32
·期 10
·1307-1319
·
IF 3.1
Li Qinsheng,Li Yupeng,Li Yaru,Huang Qinghua,Hu Zhongyu,Yang Yuping,Xiong Zhenhua,Cheng Chuanjie
It is urgent and important to design and prepare functional polymers utilizing biomass or bio-based platform chemicals due to fossil resource/energy crisis. We designed and synthesized two linear polymers LP 1 and LP 2 from bio-based platform chemical furfural as well as other biomass-derived feedstock adipic acid and 1,6-hexadiamine using efficient and 100% atom-economy Passerini three-component reaction. The number-average molecular weights of LP 1 and LP 2 are 2189 da and 5464 da, respectively. The products LP 1 and LP 2 were crosslinked with N,N ´-4,4´-diphenylmethyene bismaleimide (BMI) through Diels–Alder cycloaddition reactions to form the corresponding polymer networks CP 1 and CP 2 , respectively. Both CP 1 and CP 2 showed good chemical resistance to acid and ethyl acetate, but relatively poor resistance toward base and THF. Gel fraction values of CP 1 and CP 2 were 82% and 74%, respectively, indicating that most of the linear segments of LP 1 and/or LP 2 were crosslinked after Diels–Alder reactions. Thermal property analysis indicated that the two polymer networks were at rubbery state as their T g values were 14.78 and 7.00 °C, respectively. Td 10 values of CP 1 and CP 2 were 151 °C and 131 °C, respectively. The presence of dynamic D–A bonds caused both CP 1 and CP 2 to exhibit intrinsic self-healable performance at 60 °C or higher. Furthermore, CP 2 also showed rapid self-healing behavior (within 3 min) under UV (360 nm) irradiation due to the existence of dynamic disulfide bonds in the main chain. Graphical abstract
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Biotechnology for Biofuels and Bioproducts
·
2023
·Vol. 16
·期 1
·1-12
·
IF 0
Deng Hai-Qing,Lin Xiao-Hui,Fan Jun-Tao,Fu Ping-Zhang,Guan Jia-Jun,Lei Han-Lin,Liu Li-Hao,Lai Lin-Hao,Hou Xue-Dan,Lou Wen-Yong
Background Xylo-oligomers are a kind of high value-added products in biomass fractionation. Although there are several chemical methods to obtain xylo-oligomers from biomass, the reports about the deep eutectic solvents (DESs)-mediated co-production of xylo-oligomers and fermentable sugars and the related kinetic mechanism are limited. Results In this work, glycolic acid-based DESs were used to obtain xylo-oligomers from corncob. The highest xylo-oligomers yield of 65.9% was achieved at 120 °C for 20 min, of which the functional xylo-oligosaccharides (XOSs, DP 2–5) accounted for up to 31.8%. Meanwhile, the enzymatic digestion of cellulose and xylan in residues reached 81.0% and 95.5%, respectively. Moreover, the addition of metal inorganic salts significantly accelerated the hydrolysis of xylan and even the degradation of xylo-oligomers in DES, thus resulting in higher selectivity of xylan removal. AlCl 3 showed the strongest synergistic effect with DES on accelerating the processes, while FeCl 2 is best one for xylo-oligomers accumulation, affording the highest xylo-oligomers yield of 66.1% for only 10 min. Furthermore, the kinetic study indicates that the ‘potential hydrolysis degree’ model could well describe the xylan hydrolysis processes and glycolic acid/lactic acid (3:1) is a promising solvent for xylo-oligomers production, in particular, it worked well with FeCl 2 for the excellent accumulation of xylo-oligomers. Conclusions Glycolic acid-based deep eutectic solvents can be successfully applied in corncob fractionation with excellent xylo-oligomers and fermentable sugars yields on mild conditions, and the large amount of xylo-oligosaccharides accumulation could be achieved by specific process controlling. The strategies established here can be useful for developing high-valued products from biomass.
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PubMed
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 10
·4167-4177
·
IF 1.6
Peng Yinyin,Pan Ting,Chen Chuang,Zhou Mi,Liu Derong,Feng Jian,Xiong Wei,Liu Ning,Yuan Guoyuan
In this work, MOFs materials functionalized (HC-MOFs) with heterocyclic ligands (thiophene-TPC, pyrrole-PCA and furfural-FUR) were prepared by a one-step method and used for cobalt ion separation studies. The results showed that the maximum adsorption of cobalt ions by the three adsorbents was 141.0 mg/g (UiO-66-TPC), 146.0 mg/g (UiO-66-PCA), and 150.6 mg/g (UiO-66-FUR), respectively, at pH 8.3 and a temperature of 298 K. In addition, The HC-MOFs showed good stability under different doses (0 ~ 200 kGy) of γ-ray irradiation and have great potential for application in the separation of practical radioactive wastewater containing 60 Co.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Wanying Liang,Guangyue Xu,Yao Fu
A series of metal-TS-1 zeolite catalysts were designed to selectively catalyze the photo oxidation of furfural to C 4 carboxylic acid derivatives at ambient temperature and pressure. The photocatalytic preparation of malic acid from furfural was realized for the first time. The selective distribution of products could be controlled by adjusting the physical and chemical characteristics of the catalyst. Smaller pore size prevented the further conversion of maleic acid to malic acid; moderate acidity was beneficial for the preparation of malic acid; lower valence band was in favor of maleic acid production while higher valence band tended to form malic acid. The synergistic effect of pore structure, acidity and energy band structure of catalysts affected the product distribution. The yield of maleic acid reached as high as 40% over Fe-TS-1, meanwhile, the yield of malic acid reached as high as 63% over Ni-TS-1. The doping of metal was believed to be an effective procedure to adjust the structure and physicochemical properties of zeolite. Matel-TS-1 zeolite was also expected to be widely used in photocatalytic system to achieve more selective reactions.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 18
·7126-7140
·
IF 9.8
Jiao Chen,Jiali Cai,Feng Sha,Wenjun Sun,Xilei Lyu,Yonghui Chang,Fei Cao,Lili Zhao,Hongli Wu,Pingkai Ouyang
As a potential substitute for petroleum-based terephthalic acid (TPA) in the manufacture of polyesters, 2,5-furandicarboxylic acid has been obtained through several feasible routes. Herein, a new chemo-enzymatic strategy for generating furan-2,5-dicarboxylic acid (FDCA) precursors from sodium gluconate via bio-oxidation and dehydration is presented. By coupling the bio-oxidation of gluconate 5-dehydrogenase with carbonyl reductase PsCR for cofactor regeneration, 5-keto-D-gluconic acid (5KGA), a specific product of D-gluconic acid bio-oxidation and a stable intermediate, was obtained in 99% yield. The statin intermediate ethyl (S)-4-chloro-3-hydroxybutanoate was simultaneously generated as a co-product via cycling cascade catalysis. Subsequently, the yield of the FDCA precursor n-butyl-5-formyl-2-furancarboxylate (nBu-FFCA) generated via5KGA dehydration and esterification reached 77.9%. Key intermediate characterization and theoretical calculations revealed that the decarboxylation and dehydration of cyclic 5KGA to furfural was the main side-reaction that prevented a better yield of dehydrated 5KGA. This route demonstrates good sustainability and market competitiveness compared to the existing FDCA synthesis methods.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Ziqi Ren,Lu Fang,Miao Cui,Tianming Lv,Huifang Wu,Ziyi Feng,Zhaochi Feng,Changgong Meng,Limin Ren
Catalyst engineering plays a key role in bridging gaps between the structure of the Lewis acid center and its corresponding catalytic performance. In this regard, work that has been done in tuning active sites of Hf-containing zeolites, which hold promising catalytic activity for a variety of hydrogen-shift reactions, is far from complete. Herein, a Hf-B-BEA catalyst was rapidly prepared (within hours) by a hydrothermal semi-reconstruction strategy, involving partial framework etching of parent B-BEA and Hf grafting during the reassembling process. Then, an acid treatment was performed for expelling the boron atoms from the framework; more importantly, Hf migration into the silanol nests was triggered. The acid treatment worked powerfully as the driving force for transforming the semi-framework Hf into well-defined tetrahedrally coordinated framework Hf, thus endowing Lewis acidity of the obtained Hf-BEA. Consequently, this operation greatly boosted the Meerwein–Ponndorf–Verley reduction performance of Hf-BEA, which was almost inactive over the pristine Hf-B-BEA. The rational regulation of Hf sites provides new concepts in designing Hf-containing zeolites and understanding the structural–activity relationship.
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危险品化学品经营许可证（带存储）