INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2021
·
IF 6.953
Xiaoqi Wang,Mo Qiu,Yiwei Tang,Jirui Yang,Feng Shen,Xinhua Qi,Yingliang Yu
Sulfonated lignin-derived ordered mesoporous carbon (OMC-SO 3 H) solid acid was synthesized through solvent evaporation induced self-assembly (EISA) method followed by sulfonation , using lignin as carbon precursor and glyoxal as cross-linking agent during the preparation process. The as-synthesized OMC-SO 3 H exhibited a typical 2D hexagonal meso-structure (space group p6mm ) and showed a good catalytic performance for the catalytic conversion of hemicellulose-derived xylose to furfural. A highest furfural yield of 76.7% with 100% xylose conversion was achieved at 200 °C for 45 min in γ-valerolactone (GVL)-water (85:15 v /v%) mixture. The lignin-derived OMC-SO 3 H solid acid catalyst showed superior stability and reusability, and was also applicable to the catalytic production of furfural from xylan . This work provides a promising strategy for the synthesis of ordered mesoporous carbon solid acid from green and sustainable lignin biomass resource, which has wide range of applications in the utilization of cellulose and hemicellulose .
研究领域:
生物质化学
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催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Xiaoyi Xu,Zhimin He,Hui Tang,Yidong Sun,Shuyuan Zhang,Dezhi Shi,Fangying Ji
In this study, using furfuryl alcohol as the precursor carbon and mesoporous silica as the template, and furfuryl alcohol-derived mesoporous carbon (FMC) was prepared. The specific surface area of FMC was 1022.61 m 2 /g, the pore volume was 1.71 cm 3 /g, and the mesoporous volume was 98.8%. Based on the adsorption kinetics of pharmaceuticals onto the FMC in synthetic urine, equilibrium adsorption was reached in 120 min, and it followed a pseudo-second-order model. The adsorption isotherms were well-fitted by the Sips isotherm model, and the saturated adsorption capacities of diclofenac and oxytetracycline in fresh urine were 411.8 mg/g and 465.9 mg/g, respectively. Batch experiment results showed that pharmaceutical removal was strongly influenced by urine components such as sodium chloride, urea, and ammonium hydroxide. The adsorption of diclofenac and oxytetracycline was influenced by many factors including π-π interactions, hydrogen bonds , and electrostatic forces. FMC exhibited excellent reusability and retained urine nutrients during pharmaceutical adsorption.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
He Wei,He Yu-Cai,Ye Jianren
The objective of this work was to develop an efficient approach for chemoenzymatically transforming biomass to furfurylamine by bridging chemocatalysis and biocatalysis in a deep eutectic solvent of EaCl:Gly–water. Using hydroxyapatite (HAP) as support, heterogeneous catalyst SO42−/SnO2–HAP was synthesized for transforming lignocellulosic biomass into furfural using organic acid as a co-catalyst. The turnover frequency (TOF) was correlated with the pKa value of the used organic acid. Corncob was transformed by oxalic acid (pKa = 1.25) (0.4 wt%) plus SO42−/SnO2–HAP (2.0 wt%) to produce furfural with a yield of 48.2% and a TOF of 6.33 h-1 in water. In deep eutectic solvent EaCl:Gly–water (1:2, v/v), co-catalysis with SO42−/SnO2–HAP and oxalic acid was utilized to transform corncob, rice straw, reed leaf, and sugarcane bagasse for the production of furfural with the yield of 42.4%–59.3% (based on the xylan content) at 180°C after 10 min. The formed furfural could be efficiently aminated to furfurylamine with E. coli CCZU-XLS160 cells in the presence of NH4Cl (as an amine donor). As a result of the biological amination of furfural derived from corncob, rice straw, reed leaf, and sugarcane bagasse for 24 h, the yields of furfurylamine reached >99%, with a productivity of 0.31–0.43 g furfurylamine per g xylan. In EaCl:Gly–water, an efficient chemoenzymatic catalysis strategy was employed to valorize lignocellulosic biomass into valuable furan chemicals.
研究领域:
生物化学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Xu Wu,Heqin Guo,Litao Jia,Yong Xiao,Bo Hou,Yongxiang Gao,Debao Li
δ-MnO 2 exhibits excellent activity for furfural oxidation to furoic acid under base-free conditions. However, its poor C H bond breaking capacity leads to lower conversion efficiency per unit mass catalyst than noble metal. Thus, a series of Ru-modified δ-MnO 2 (Ru x /δ-MnO 2 ) have been made to enhance its C H bond breaking ability. The result showed that the furfural conversion was greatly enhanced on Ru x /δ-MnO 2 due to the enhanced capability for breaking the C H bond. Especially for Ru0.25/δ-MnO 2 , whose conversion rate per unit mass was 18 times higher than δ-MnO 2 . The characterization results showed that the Ru species mainly existed as single atoms or clusters on Ru0.25/δ-MnO 2 and Ru0.5/δ-MnO 2 , while started to aggregate to RuO 2 nanoparticles on Ru1/δ-MnO 2 and Ru2/δ-MnO 2 . With the increase of Ru particles, the Ru's average oxidation state (AOS) decreased from +6 on Ru0.25/δ-MnO 2 to +4.74 on Ru2/δ-MnO 2. The Ru's TOF (intrinsic activity per Ru) was positively linearly related to the Ru's AOS. The electron-deficient Ru in Ru0.25/δ-MnO 2 can strongly adsorb the H atom of the C H of geminal diol intermediate and accelerate the breakage of its C H bond. As a result, Ru in the Ru0.25/δ-MnO 2 exhibited the highest TOF, which can even reach 29.85 mmol FF /mmol Ru /h.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2019
·
IF 2.584
Xiaofang Liu,Hu Pan,Heng Zhang,Hu Li,Song Yang
Enlarging the dispersed micropores of metal-organic frameworks to the well-ordered mesostructure can enhance the accessibility of acidic sites for reactants resulting in the improvement of selectivity. With the regulation of cetyltrimethylammonium bromide/Cr3+ and ClSO3H sulfonation, a series of mesoporous MIL-101(Cr)-SO3H (MMSs) with multiple pore sizes and acidic properties were synthesized and explored to further facilitate the furfuryl alcohol (FA) ethanolization to ethyl levulinate (EL) for the first time. The optimal catalytic activity of 83.8% EL yield at full FA conversion demonstrated that the appropriate mesopore size, acidic density, and accessible −SO3H sites contributed to the superior performance of the MMS(0.3)-0.15. The turnover frequency value (14.8 h–1) obtained with MMS(0.3)-0.15 was comparable to the commercial Nafion NR50 (18.3 h–1) and much higher than the classical Amberlyst-15 (1.9 h–1), confirming the predominant catalytic performance. Furthermore, two coexistent reaction paths with 2-ethoxymethylfuran and 4,5,5-triethoxy-pentan-2-one as intermediates indicated the possibility of producing EL from FA.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 4
·1956-1965
·
IF 3.119
Weiqi Xie,Shiwen Huang,Donglin Tang,Shumei Liu,Jianqing Zhao
A furfural-based DOPO-containing flame retardant, 6,6′-(((methylenebis(4,1-phenylene))bis(azanediyl))bis(furan-2-ylmethylene))bis(dibenzo[c,e][1,2]oxaphosphinine 6-oxide) (MBF-DOPO), was synthesized and utilized as a co-curing agent of 4,4′-diaminodiphenyl methane (DDM) for fire-safe epoxy thermosets. For the cured epoxy resin containing 4.0% MBF-DOPO, the limiting oxygen index (LOI) reached 32.9% (with the V-0 rating in UL-94 test), and the peak heat release rate and total smoke production values were respectively decreased by 29.3% and 33.6%, compared to pure epoxy resin. Scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR) results confirmed that the furfural-based flame retardant MBF-DOPO promoted the charring formation of the epoxy matrix, which effectively isolated the gas and heat transfer during combustion and thus enhanced the fire-safety performance of the epoxy thermosets. This work provides an effective route for synthesizing a furfural-based flame retardant, which possesses great potential for application in fire-safe epoxy thermosets.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Yilin Wei,Zhiwei Sun,Qingqing Li,Dan Wu,Jianshe Wang,Yuexing Zhang,Chunbao Charles Xu,Renfeng Nie
Cost-effective and environmentally friendly production of biomass-derived amines under mild conditions is highly desirable but challenging. Herein, bifunctional Co@CoO x catalysts comprised of Co and CoO x were prepared by controllable precipitation-reduction and adopted for furfural (FAL) reductive amination with N 2 H 4 . The structure of Co species can be regulated gradually via tuning reduction temperature, resulting in a significant influence on reductive amination. The optimal CoO x -250 can achieve 96.4 % furfurylamine (FFA) yield at 60 °C, and even 95.8 % at 30 °C. The control experiments and DFT calculations suggest that the metal Co is responsible for H 2 dissociation and C N reduction, while the oxygen-vacant CoO x favors the hydrogen spillover and the C N bond activation, thus resulting in a collaborative effort for FAL reductive amination. The catalyst is stable and versatile for various aldehydes/ketones with amine yields around 95–99 %, showing great potential for industrial application.
研究领域:
催化化学
·
生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Yongxin Zhang,He Li,Zhongliang Shi,Miao Guo,Yanming Hu,Guangyuan Zhou
Total hydrogenation of furfural (FAL) is an efficient way to produce the industrially important tetrahydrofurfuryl alcohol (THFOL). However, it is a challenge to obtain highly selective catalysts for this transformation especially under mild reaction conditions. Herein, we report that the β-ketoenamine-linked covalent organic framework (TpBD COF) supported ultrafine Pd nanoparticles exhibit significantly enhanced selectivity for THFOL compared to Pd/C (95% vs. 82 %) at almost full FAL conversion. This heightened selectivity is attributed to the increased electronic density on the Pd surface, resulting from the electron-donating effect of pendant groups in the TpBD COF. Moreover, kinetic investigations reveal that the activity of total FAL hydrogenation on Pd surface is linked to the rate-determining step in its first C = O hydrogenation process. Additionally, Pd/TpBD COF could catalyse various other bio-based furanic compounds to the corresponding furan ring saturated products in high yields. This work provides guidance for the rational design catalysts to improve its tandem hydrogenation efficiency.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Wenli Zhang,Yijie Zhou,Zhenzhen Wu,Cheng Pan,Qunpeng Cheng,Guozhi Fan
A porous sulfonic acid-functionalized zirconium-based metal–organic framework possessing both Lewis acid and Brønsted acid sites (UiO-66-SO 3 H) was synthesized and tested for the selective conversion of furfural (FUR) to isopropyl levulinate (IPL) through one-pot cascade reaction. UiO-66-SO 3 H exhibited excellent catalytic performance, and the conversion of FUR as well as the yield and selectivity of IPL reached 96.4 %, 86.0 %, and 89.2 %, respectively. UiO-66-SO 3 H could be simply recovered and reused, but the catalytic performance was significantly decreased. The FUR conversion and IPL yield dropped to 73.8 % and 65.1 %, respectively, after 1 cycle, and the reason for the decrease in the catalyst activity were also investigated. It was found that the decrease was mainly caused by the loss of some −SO 3 H groups, and the cyclic performance of UiO-66-SO 3 H could be restored by supplementing a small amount of BDC-SO 3 Na. A plausible mechanism for the selective synthesis of IPL from FUR was proposed, wherein both Lewis acid and Brønsted acid sites played important roles. This work provides guidance for the selective conversion of FUR into IPL, and the high-valued utilization of biomass and its derivatives.
研究领域:
化学工程
·
催化科学
·
可再生资源利用
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2024
·
IF 3.8
Libin Liu,Yuxi Si,Wenjie Zhao,Qingqin Zhu,Zhaoran Yang,Jing He,Yangqiang Huang,Youwei Cheng
Cyclopentanone (CPO) and cyclopentanol (CPL), derived from renewable biomass resource hemicellulose, are considered sustainable chemicals that can substitute fossil-based products, which could be obtained through the hydrogenation-rearrangement reaction of furfural (FFA). However, the inevitable condensation reactions of FFA and furfuryl alcohol (FA) in aqueous solutions generate humins and result in carbon loss, limiting the industrial application of this process. Herein, a series of Cu-based catalysts were synthesized using the reverse co-precipitation method with various metal promoters and applied in the FFA hydrogenation-rearrangement reaction. The highest yield of 97.1% CPO/CPL achieved in a typical reaction condition at 200 °C, 4 MPa, in 20 wt% isopropanol-water mixed solvent over CuZnZr catalyst and the recyclability test confirmed that the catalyst had excellent stability. Experimental studies and characterizations showed that the enhanced performance could be attributed to the adequate Lewis acid sites, regulated through the synergistic interaction between Cu, Zn, and Zr compounds. The simultaneous introduction of Zn and Zr promotes the Cu reduction, and results in more dispersed Cu0 and Cu+, providing an ample and reliable active site. This study outlines a viable method for the catalyst designing and valorizing biomass into high-value-added products.
研究领域:
催化化学
·
可再生资源化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Yu Zhao,Jun Xu,Jing Wang,Jinglan Wu,Meizhen Gao,Bin Zheng,Hong Xu,Qi Shi,Jinxiang Dong
The objective of this work is to study the adsorptive separation of the biomass-derived furfural (Fur) and 5-hydroxymethylfurfural (5-HMF). Because Fur and 5-HMF have similar ellipsoidal shapes, the diffusion of the larger 5-HMF may be blocked by the elliptical window of adsorbents. Thus, two zeolitic imidazolate framework (ZIF) materials with the identical chemical composition, MAF-6 and MAF-5, were used as spherical and ellipsoidal pore adsorbents, respectively. In the dynamic column adsorption of a binary-component system (Fur/5-HMF, 5/5 wt %) in an aqueous solution, the adsorption amounts of Fur on MAF-6 display a 13% decrease compared with the single-component system, whereas the adsorption amounts of Fur on MAF-5 are identical to those obtained in the single-component system and the amounts of adsorbed 5-HMF are almost negligible. Thus, the Fur/5-HMF selectivity is only 6.4 for MAF-6, whereas the selectivity reached 115.8 for MAF-5. The results show that the narrow elliptical window/ellipsoidal tile of MAF-5 enhanced separation selectivity compared with the larger circular window/spherical cage of MAF-6. In addition, the general rate model and density functional theory calculations further verify that the elliptical window of MAF-5 exhibits a strong mass-transfer barrier that must be overcome for the diffusion of the larger 5-HMF molecules.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2021
·Vol. 14
·期 11
·2341-2351
·
IF 8.928
Bo Zhou,Fan Song,Xinyue Ma,Lijun Wang
Graphical The batch is back : A scalable green catalyst system based on a TiO 2 nanoparticle–exfoliated montmorillonite composite catalyst with hard Lewis acid sites and abundant accessible Brønsted acid sites is developed for the rapid preparation of furfural acetals, which are a promising biofuel with high octane value, high calorific value, and high oxidation resistance. Furfural acetals with high octane value, high calorific value and high oxidation resistance are considered promising biofuels or fuel precursors with huge potential demand. However, there are few studies on efficient scalable catalyst systems, including continuous-flow catalyst systems, for their preparation. In this work, TiO 2 nanoparticles supported on exfoliated montmorillonite, with strong Lewis acid sites and abundant accessible Brønsted acid sites, is used to catalyze the acetalization reactions of biomass-derived furfural and alcohols. Low dosage of the catalyst made the reaction reach equilibrium in a very short time (TOF=690–1305 min −1 ) at room temperature with the acetal as the only product. In continuous-flow reactions, the catalyst showed a stable product output with conversion close to that for the batch reaction with a short catalyst-reactant contact time of 150 s. Contrast experiments revealed that both Lewis and Brønsted acid sites on the catalyst were indispensable for maximizing the catalytic performance, and simultaneously activating both furfural and alcohol on the adjacent Lewis and Brønsted acid sites was proposed to be responsible for the high catalytic performance.
研究领域:
化学工程
·
催化科学
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）