CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuchao Shao,Weizhong Huo,Rong Ye,Yanqing Liu,Muhammad Ajmal,Wenjing Lu
The humification behavior of lignocellulosic components ( i.e. , cellulose, hemicellulose and lignin) under acid-alkali two-step hydrothermal treatment was investigated with particular interest of revealing the contribution of single components as well as their interaction to hydrothermal humic acid (HHA). Lignin with its rich aromatic structures, had the highest HHA contribution (51.8 ± 1.0 wt%), while cellulose and hemicellulose only contributed 8.8 ± 1.6 wt% and 20.1 ± 4.4 wt% HHA yields, respectively. The conversion pathway of these components toward humification indicated that the hydrochar (HC) rather than the hydrothermal solution (HS) had higher humification capability under alkaline hydrothermal conditions because the hydrochar-derived HHA yields of 40.8 ± 2.0 wt% (cellulose), 66.2 ± 6.4 wt% (hemicellulose) and 55.4 ± 6.1 wt% (lignin) were achieved. In addition, co-hydrothermal treatment of cellulose, hemicellulose and lignin under this process improved the HHA production ascribing to the increased HC yield (23.1–53.1 %). The chemical characteristics of HHA products from lignocellulosic components (cellulose, hemicellulose, lignin) and their combinations were similar to the acknowledged natural humic acids. The hydrothermal humification of biowaste mainly passes through a top-down pathway ( i.e. , HHA forms from the oxidation of large fragments of hydrochar) as well as two bottom-up pathways ( i.e. , the soluble chemicals conduct the polymerization reaction for HHA production and react with the fragments from HC to synthesize the HHA). This study filled the lack of knowledge in the field of biowaste humification.
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Catalysts
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2022
·Vol. 13
·期 1
·37
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IF 4.501
Qizhen Yang,Zhengyu Tang,Jiale Xiong,Yucai He
Valorization of the abundant renewable lignocellulose through an efficient chemoenzymatic strategy to produce the furan-based platform compounds has raised great interest in recent years. In this work, a newly prepared sulfonated tin-loaded rice husk-based heterogeneous chemocatalyst UST-Sn-RH was utilized to transform corncob (75.0 g/L) into furfural (72.1 mM) at 170 °C for 30 min in an aqueous system. To upgrade furfural into furfuryl alcohol, whole cells of recombinantE. coli KPADH harboring alcohol dehydrogenase were employed to transform corncob-derived furfural into furfuryl alcohol at 30 °C and pH 7.5. In the established chemoenzymatic cascade process, corncob was efficiently transformed to furfuryl alcohol with a productivity of 0.304 g furfuryl alcohol/(g xylan in corncob). In general, biomass could be efficiently valorized into valuable furan-based chemicals in this tandem reaction with the chemocatalyst (bio-based UST-Sn-RH) and the biocatalyst (KPADH cell) in an aqueous system, which has potential application.Keywords:furfural;furfuryl alcohol;heterogeneous catalyst;chemoenzymatic strategy
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Baoyu Wang,Mingrui Li,Songdang Zhang,Hongguo Wu,Yuhe Liao,Hu Li
Finite size effect is closely correlated with heterogeneous catalytic activity and selectivity as reducing the metal to a few nanometers, but may suffer from deficient active sites for cascade reactions. Here, a type of dual-size heterogeneous N-doped cobalt catalysts (Co SAs-NPs /NC(n)) with the coexistence of Co single-atoms (Co-SAs) and Co nanoparticles (Co-NPs) were prepared for efficient synthesis of benzimidazoles (up to 91% yield) from 2-nitroanilines and bio-based alcohols via cascade hydrogen transfer-dehydrogenative cyclization. Experimental results and density functional theory calculations suggested that the bio-alcohol dehydrogenation mainly occurs at Co-SAs sites, while Co-NPs sites remarkably facilitate the subsequent reduction of nitro species, indicating the synergistic effect between Co-SAs and Co-NPs in the coupled hydrogen transfer process. The Co SAs-NPs /NC(0.25) catalyst can be recycled and applied to a wide range of substrates (28 examples). This catalytic approach based on the metal size effect opens a new route for the direct upgrading of biomass feedstocks involving multiple reactions.
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Frontiers in Bioengineering and Biotechnology
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2023
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IF 5.7
Huang Lizhen,Bian Zelun,Li Dalin,Cheng Xin,Luo Xiaolin,Shuai Li,Liu Jing
Biobased furfural is a sustainable alternative to petrochemical intermediates for bulk chemicals and fuel production. However, existing methods for the conversion of xylose or lignocelluloses in mono-/bi-phasic systems to furfural involve non-selective sugar isolation or lignin condensation, limiting the valorisation of lignocelluloses. Herein, we used diformylxylose (DFX), a xylose derivative that is formed during the lignocellulosic fractionation process with formaldehyde protection, as a substitute for xylose to produce furfural in biphasic systems. Under kinetically optimized conditions, over 76 mol% of DFX could be converted to furfural in water-methyl isobutyl ketone system at a high reaction temperature with a short reaction time. Finally, isolation of xylan in eucalyptus wood as DFX with formaldehyde protection followed by converting DFX in a biphasic system gave a final furfural yield of 52 mol% (on the basis of xylan in wood), which was more than two times of that without formaldehyde. Combined with the value-added utilization of formaldehyde-protected lignin, this study would enable the full and efficient utilization of lignocellulosic biomass components and further improve the economics of the formaldehyde protection fractionation process.
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CARBON
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2023
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IF 10.9
Xiang Li,Jindong Hu,Meng Wu,Chaochao Guo,Long Bai,Jinming Li,Yuwei Li,Dehao Luo,Jiamin Duan,Xiaoli Li,Zhiguo Li
Promoting and enhancing the transport rate of multivalent electrolyte ions in the pores of electrode is central for constructing high-performance electrochemical devices . Herein, waxberry-like porous carbon with nanosheets packaged by spherical carbon particles is produced by adjusting separation of hydrophilic and hydrophobic parts of carbon source precursors. The carbon particles maintain their original morphology after KOH activation at high temperature, forming tunable pores (pore volume: 0.9386 cm 3 g −1 ) on the surface of stacked nanosheet layers. Benefiting from the synergistic effect of structural features, an interfacial transport of aqueous zinc ions within the carbon electrodes is achieved, endowing the assembled zinc-ion hybrid supercapacitors (ZHSCs) with excellent energy storage performances, including high capacity (122.3 mAh g −1 at 0.1 A g −1 ), high energy density (97.78 Wh kg −1 ), large power density (8000 W kg −1 ), and cycling stability up to 10,000 cycles with capacity retention of 98%. Moreover, the ZHSCs show superior low-temperature performance and operability (78.27 mAh g −1 at −30 °C and three-time cycling stability between −20 and 20 °C without performance degradation). This work presents a new prospect on design and development of aqueous rechargeable zinc-ion energy storage devices that are available for a range of environmental conditions.
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Journal of Energy Chemistry
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2022
·
IF 13.599
Hui Yang,Hao Chen,Wenhua Zhou,Haoan Fan,Chao Chen,Yixuan Sun,Jiaji Zhang,Sifan Wang,Teng Guo,Jie Fu
Hydrodeoxygenation of furfural (FF) into 2-methylfuran (MF) is a significant biomass utilization route. However, designing efficient and stable non-noble metal catalyst is still a huge challenge. Herein, we reported the N, O co-doped carbon anchored with Co nanoparticles (Co-SFB) synthesized by employing the organic ligands with the target heteroatoms. Raman, electron paramagnetic resonance (EPR), electrochemical impedance spectroscopy (EIS), and X-ray photoelectron spectroscopy (XPS) characterizations showed that the co-doping of N and O heteroatoms in the carbon support endows Co-SFB with enriched lone pair electrons, fast electron transfer ability, and strong metal-support interaction. These electronic properties resulted in strong FF adsorption as well as lower apparent reaction activation energy. At last, the obtained N, O co-doped Co/C catalyst showed excellent catalytic activity (nearly 100 mol% FF conversion and 94.6 mol% MF yield) and stability for in-situ dehydrogenation of FF into MF. This N, O co-doping strategy for the synthesis of highly efficient catalytic materials with controllable electronic state will provide an excellent opportunity to better understand the structure–function relationship.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Zhengliang Zhang,Zhiwei Zhang,Xubin Zhang,Fumin Wang,Zheng Wang,Yongwang Li,Xingtao Wang,Rosine Ahishakiye,Xu Zhang
Exploring low-cost green catalysts to achieve green organic chemicals and fuels from biomass is one of the crucial ways to solve the energy crisis. The 20 wt% Co-CoO x /AC catalysts were prepared to achieve the one-pot conversion of furfural to 2-methylfuran under milder reaction conditions (120 °C, 2.5 MPa H 2 ), shorter reaction time (5 h) and less catalyst dosage by regulating the ratio of metal to oxide species. The yield of 2-methylfuran reached 87.4 % is achieved under 20 wt% Co-CoO x /AC catalyst conditions, and there was no significant degradation of all catalyst properties after five cycles. Characterization results showed that the active components in the catalyst were present as Co 0 species with CoO x species. The reaction mechanism was explained by combining the characterization results, experimental data and DFT calculations. The formyl group of the furfural side chain is first adsorbed on the Co 0 species, and furfuryl alcohol is produced in the presence of the Co 0 species. Subsequently, the CoO x species adsorbs the C O bond on the side chain, which is broken in the presence of the CoO x species to form 2-methylfuran. The excellent catalytic activity of the 20 wt% Co-CoO x /AC catalyst provide a promising application for preparing 2-methylfuran by hydrodeoxygenation of furfural.
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Molecular Catalysis
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2022
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IF 5.089
Peng Zhang,Mingwei Ma,Pan Hou,Jingjie Cao,Qi Guo,Huijuan Yue,Ge Tian,Shouhua Feng
A series of ultrathin metal intercalated montmorillonite (Mont) nanosheet materials were prepared and characterized for the one-pot cascade conversion of furfural (FAL) to obtain γ-valerolactone (γ-GVL). The coordination of the intercalated metal ions and the hydroxyl groups between the montmorillonite layers leads to an increase in the specific surface area and pore volume of the material, which coupled with the acidity of the metal ions themselves improves the catalytic performance of the material. Thus Zr-Mont-0.1 exhibited optimal catalytic performance with 100% conversion of FAL and 50.4% yield of GVL under mild conditions, and more importantly, the catalyst maintained its good catalytic performance after the fourth use. Meanwhile the number of Lewis and Brønsted acid sites in the Zr-Mont catalyst can be varied by adjusting the zirconium ion concentration. The proposed reaction mechanism provides initial insights into the role of metal-functionalized montmorillonite in catalyzing the reaction. In addition, the ten-fold magnification reaction confirmed the potential industrial application of the catalyst.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yongfang Zhou,Thomas J.A. Slater,Xuanli Luo,Yi Shen
Single atom electrocatalysts (SAECs) exhibit intriguing catalytic performance due to their utmost atom-utilization efficiency and unique electronic structure. However, the application of SAECs is limited on simple reactions such as the hydrogen/oxygen evolution reactions, and oxygen/nitrogen reduction reactions. Herein, single copper atoms supported on nitrogen doped carbon nanosheets (Cu/NCNSs) were demonstrated as a versatile SAEC for biomass upgrade. The activity of Cu/NCNSs was benchmarked against commercial Cu nanoparticles . Twelve basic platform compounds including 5-hydroxymethylfurfural (HMF), furfural , glucose, formaldehyde, methanol, ethanol, isopropanol, ethylene glycol , glycerol, benzyl alcohol, formic acid , and oxalic acid were employed as substrates. The products of electro-oxidation of these substrates were analyzed by high performance liquid chromatography. The reaction pathways and mechanisms of substrate oxidation on Cu/NCNSs and Cu NPs were explored by in-situ electrochemical Raman spectra. HMF oxidation on Cu NPs followed the 5-diformylfuran (DFF) path at lower potentials, while it turned to 5-hydroxymethyl-2-furancarboxylic acid path at applied potentials over 1.67 V. For Cu/NCNSs, HMF oxidation followed the alcohol hydroxyl oxidation pathway, that is, the direction of generating DFF. The active sites for substrate oxidation on Cu/NCNSs are different from those on Cu NPs. This work broadened the application of SAECs in the field of biomass upgrade, and paved a new route to fabricate advanced electrocatalysts for biomass valorization.
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INDUSTRIAL CROPS AND PRODUCTS
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2023
·
IF 5.9
Banglun Xiong,Sen Ma,Binglin Chen,Yunchao Feng,Zhiqing Peng,Xing Tang,Shuliang Yang,Yong Sun,Lu Lin,Xianhai Zeng,Yong Chen
A large number of bamboo waste is produced from bamboo processing industries. Bamboo waste, with high biomass yield and rich in xylan and glucan , is a promising material for the coproduction of xylo-oligosaccharides and glucose. In this work, a formic acid-facilitated hydrothermal pretreatment of bamboo was investegated to increase the yield of xylo-oligosaccharides by controlling the severity factor (SF) and formic acid concentration. The maximum xylo-oligosaccharides yield was 68.04 % (of initial xylan) and the concentrations of X 2 , X 3 , X 4 , and X 5 were 4.56, 3.08, 2.30 and 2.58 g/L, respectively. The highest enzymatic hydrolysis yield reached 93.05 % at 45 FPU/g cellulase dosage. Additionally, lignin isolated after formic acid pretreatment (FA-lignin), and lignin from alkali extraction (AE-lignin) had better thermal stability than milling wood lignin (MWL), which could be used in fire-retardant material applications. The techno-economic analysis predicts a revenue of 118.86 USD by processing 100 kg of waste bamboo combined with enzyme cost analysis. To conclude, xylo-oligosaccharides (12.56 kg), xylose (4.81 kg), glucose (22.37 kg) and lignin (13.28 kg) were produced from bamboo (100 kg, 18.37 % xylan, 44.29 % glucan, 27.23 % lignin). The results can give insights into establishing an efficient acid pretreatment of bamboo waste to produce xylo-oligosaccharides, glucose and lignin.
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BIOMASS & BIOENERGY
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2023
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IF 6
Jirui Yang,Yanwei Zhang,Feng Shen,Xinhua Qi
Meerwein-Ponndorf-Verley (MPV) reaction has been widely acknowledged to be a mild catalytic transfer hydrogenation method for selective reduction of biomass-derived furfural to furfuryl alcohol . Herein zirconium-containing mesoporous composite catalyst was developed through the combination of sol-gel process and soft templating method, in which naturally abundant glucose and F127 triblock copolymer were used as the ligand and pore-forming agent, respectively. The hydroxyl groups in glucose molecules were demonstrated to be coordinated with zirconium ion during hydrolysis-condensation of zirconium precursor, leading to the even dispersion of zirconia nanoparticles in the composite catalyst. The composite catalyst was proven to be highly efficient for catalyzing MPV reduction of furfural with the maximum furfuryl alcohol yield of 93.4% at 180 °C within 180 min in 2-propanol, which served as both solvent and reductant . The composite also showed a good reusability . After five consecutive reaction cycles, furfuryl alcohol yield was slightly reduced from 93.4% to 77.7%, but it could be recovered to 92.8% after the reused composite was regenerated with dilute alkali solution. Batch experiments and systematic characterizations demonstrated that the excellent catalytic performance of composite catalyst was determined by multiple factors mainly including the stronger Lewis acidity, a considerable amount of basic site and the rich mesoporous structure. This study provides a facile strategy to prepare multifunctional composite catalysts using naturally abundant carbohydrates as the feedstocks for lignocellulosic biorefinery .
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2023
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IF 6.1
Tong Zhou,Xue Xia,Heping Cui,Yun Zhai,Foxin Zhang,Khizar Hayat,Xiaoming Zhang,Chi-Tang Ho
The influence of pH was studied on volatile flavor formation during thermal treatment of an Amadori rearrangement product (ARP) with or without the addition of cysteine (Cys). The formation of thiols and sulfides or 2-acetylthiazole and pyrazines induced by Cys during thermal degradation of ARP was pH-dependent. At low pH levels, the hydrolysis of Cys to hydrogen sulfide (H2S) was promoted, giving rise to the increase of thiols and sulfides with an obvious meaty aroma. However, alkaline conditions were beneficial for enhancing the cyclization or transformation of imine to the enol structure, which strengthened the formation of 2-acetylthiazole and pyrazines with a roasted and nutty aroma. The imine was derived from the nucleophilic addition of Cys and methylglyoxal (MGO) and subsequent decarboxylation. At pH 8, Cys-induced variation of the flavor profile was weakened during thermal degradation of ARP. Accordingly, the combinational effect of pH and added Cys could be beneficial for achieving the desirable flavors during thermal processing of ARP.
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