Molecular Catalysis
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2021
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IF 5.062
Weile Li,Mengzhu Li,Huai Liu,Wenlong Jia,Xin Yu,Shuai Wang,Xianhai Zeng,Yong Sun,Junnan Wei,Xing Tang,Lu Lin
The economic and highly efficient synthesis of γ-valerolactone (GVL) is being increasingly focused due to its wide applications in solvent, chemical, and fuel. Herein, a range of SAPO-34 supported zirconium phosphate (ZPS-X) catalysts were prepared for a facile one-pot conversion of furfural (FF) to GVL through a series of cascaded reactions involving transfer hydrogenation, etherification, alcoholysis and esterification. The introduction of zirconium phosphate renders the formation of relatively strong Lewis acid sites, and the amount of Lewis (L) and Brønsted (B) acid sites of ZPS-X catalysts could be modified by adjusting the molar ratio of Zr to P (Zr/P ratio). Specifically, ZPS-1.0 having an appropriate Zr/P ratio with relatively strong L acid sites exhibited superior activity and selectivity for the production of GVL from FF.
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Molecular Catalysis
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2020
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IF 3.687
Yang Zhong,Bo Zhou,Lijun Wang
Fe/FeO x embedded in LDH was prepared by reducing the pre-synthesized [Fe(C 2 O 4 ) 3 ] 3− anions intercalated LDH and used as a multi-functional catalyst for synthesis of C7-C9 compound via transfer hydrogenation between furfural (C5) and short-chain alcohols (C2-C4) and a subsequent aldol reaction of furfural with intermediate short-chain aldehydes in the absence of a homogeneous base with furfuryl alcohol as a byproduct. Screening reaction conditions, evaluation and improvement of the cyclic catalytic performance, and determination of catalytically active components were performed, and the results demonstrated that both high conversion and high selectivity to the C C bond forming product can be obtained under a non-oxidizing atmosphere of Ar or H 2 /Ar mixed gas, a reaction temperature of 140 °C and a reaction time of 4 h; the catalyst was easily deactivated during the cycle experiments, however, its catalytic stability can be effectively improved by depositing Ni with weak reducibility on the surface of Fe nanoparticles at the cost of reducing partial catalytic activity. Fe/FeO x together with LDH as a whole proved to be effective in catalyzing the transfer hydrogenation reaction and the support LDH imparted basic catalytic function to the composite realizing the aldol reaction in the absence of a homogeneous base.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Lei Ye,Yiwen Han,Hui Bai,Xuebin Lu
Bifunctional heterogeneous catalysts (HZ-ZrP) were prepared by using HZSM-5 as the carrier to support a zirconium phosphate (ZrP) active component for the one-pot value-added conversion of biomass-derived furfural (FAL). By changing the loading amount of ZrP, the ratio of Lewis to Brønsted acid (2.7–15.4) and the acid strength of the catalysts can be adjusted. HZ-ZrP-5 and HZ-ZrP-16 were selected for the production of different value-added chemicals, and a total yield of up to 93.8% (i-PL and GVL) and 64.2% (GVL) were obtained using isopropanol as the hydrogen donor under optimized conditions, respectively. Furthermore, stability and recyclability of the catalyst were also tested and showed no significant drop in total yield after recalcination. The catalysts have high activity (Ea = 27.05 ± 3.08 kJ mol–1), but the ring-opening reaction restricted the cascade reaction. In addition, a possible reaction pathway and mechanism for the FAL conversion were proposed.
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APPLIED CATALYSIS A-GENERAL
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2020
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IF 5.006
Xu Yang,Wu Liu,Fenghua Tan,Zhaoxia Zhang,Xindi Chen,Tengda Liang,Chuande Wu
Catalyst deactivation caused by the metal sintering/leaching is still a great challenge confronted by the scientists. Herein, we report a robust strategy to in situ synthesize mesoporous silica supported highly dispersed copper catalyst by homogeneously hybridizing the silica and metal-organic framework (MOF) copper benzene-1,3,5-tricarboxylate (Cu 3 (BTC) 2 ). We find the introducing silica is the key to the formation of homogeneous hybridization by regulating the growth of Cu-BTC crystallite, yielding various metal dispersion and reducibility during calcination; while the added BTC ligands acts as porous initiator, promoting the accessibility of copper centers for reactants. The optimized CuO#SiO 2 – s1 with molar ratio Cu/Si of 0.23, exhibits excellent catalytic performance towards the furfural hydrogenation, showing a high activity as 9.2 mol FF mol Cu −1 h −1 , nearly 100 % furfural alcohol selectivity and minimized activity decline (<5%) after 5 repeated run. This work could open up a new avenue for the synthesis of mesoporous silica supported highly dispersed metal catalyst for hydrogenation.
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ChemCatChem
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2021
·Vol. 13
·期 19
·4164-4181
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IF 5.686
Qiuli Fu,Shibo Yang,Ping Ning,Rongrong Miao,Liang He,Qingqing Guan
Graphical Selective hydrogenation : In rubber seed shell porous biochar supported Cu−Ni bimetals, the formed Cu 1 Ni 3 alloy stabilized the excessive Cu species which were in the lattice on the inner/outer surfaces of the rss AC support. The catalytic activity is retained, ensuring that the catalyst would neither be oxidized nor aggregated severely. The prepared high-efficiency Cu 1 Ni 1 / rss AC catalyst catalyzed the hydrogenation reaction of FAL to produce FOL, THFA and 2-MF. Using cheap Cu-based catalysts for highly selective hydrogenation of furfural (FAL) is of great importance of upgrading this biomass-derived platform molecule but is still challenging for large-scale application due to the low conversion efficiency and the easy aggregation of Cu active sites. To address these issues, a nitrogen-autodoped porous biochar derived from rubber seed shell ( rss AC) was fabricated for anchoring Cu sites on a nanoscale. Moreover, by the co-crystallization strategy of Cu and the second metal (M, M=Ni, Zn, Co, Ce), stable Cu−M nanoalloys were constructed on the surface of the rss AC support. The FAL hydrogenation experiments showed that the type, proportion and loading amount of the second metal had great effect on the catalytic efficiency. Compared with the other metals, Ni-doped Cu/ rss AC catalyst exhibited the best hydrogenation performance due to their extraordinary adsorption and activation capacity for hydrogen. Further, the highest catalytic efficiency was observed using 20 % Cu 1 Ni 1 /rss AC catalyst. The characterization results showed that the key to its success was highly-dispersive anchoring of the CuNi active sites onto the inner/outer surface of the nanopores of rss AC support by the strong interaction between the surface N-containing functional groups and metals. Of note, the formed CuNi alloys with the Cu/Ni atomic ratio of 1 : 3 played an important role in the stabilization of the adjacent nano-dot matrix Cu 0 species. Kinetic test indicated that the formation step of furfuryl alcohol (FOL) from FAL was still the key step and the hydrogenation products can be converted between FOL and tetrahydrofurfuryl alcohol (THFA). The life evaluation test showed that the catalyst still kept high activity and selectivity after being reused five times. The advanced synthesis method co-using N-doped support anchoring and the second metal alloying strategy sheds light on preparing effective catalysts for hydrogenation of biomass-based compounds.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Yuan Zhao,Hao Xu,Kaifeng Lu,Yang Qu,Lingjun Zhu,Shurong Wang
Arabinose, the second most abundant pentose in lignocellulosic biomass, can be dehydrated to produce a well-known platform chemical named furfural. However, the lowest reactivity of arabinose among the aldopentoses in biomass has hindered its application. In this work, a butanone–water mixture as a green solvent system was employed in the production of furfural from arabinose, and a Lewis acidic ionic liquid was chosen as the catalyst. An excellent furfural yield of 60% and corresponding arabinose conversion of 100% was obtained at 140 °C within 30 min. The kinetic analysis indicated that the decreasing furfural yield was mainly due to the condensation reaction between furfural and the intermediate, which came from arabinose dehydration. Self-degradation of furfural played a minor role in the falling yield at prolonged reaction time. Moreover, the butanone–water solvent mixture was beneficial for increasing the activation energy of furfural degradation, and therefore, the formation of byproducts was suppressed.
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ENERGY & FUELS
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2018
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IF 3.024
Lincai Peng,Xueying Gao,Xin Yu,Hui Li,Junhua Zhang,Liang He
An integrated multistep catalytic process in a one-pot cascade model to realize conversion is preferred in terms of process economics and energy efficiency. Here, we present the noble-metal-free but highly effective catalytic transfer hydrogenation and acid-catalyzed conversion of biomass-derived furfural for direct production of biofuel alkyl levulinate using alcohols as the hydrogen donor and reaction medium. With optimization of the process variables, a high yield of alkyl levulinate at up to 85.3% could be captured under mild conditions in isopropanol medium with the combination of Zr-MCM-41 and Amberlyst-15 catalysts. The reaction proceeds via the catalytic transfer hydrogenation of furfural to furfuryl alcohol over Zr-MCM-41, which is then converted to alkyl levulinate by an Amberlyst-15 acid catalyst. The spent hybrid catalysts could be effectively recovered from the resulting reaction mixture and reused 5 times with little deactivation after plain regeneration treatment.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2025
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IF 2.4
Vinh Thanh Chau Doan,Nhung Tuyet Thi Nguyen,Thinh An Tan Le,Phuong Hoang Tran
BACKGROUND Furfural is an important platform compound obtained through the dehydration of xylose, a key component of lignocellulosic biomass. Carbonaceous catalysts for this conversion have received rising interest due to low-cost price and easy modification. Rice husk is an abundant agricultural waste that could be employed as a carbon source for the preparation of many carbon materials, especially through green methods. RESULTS A carbonaceous catalyst (RH-SO₃H) derived from rice husk through microwave (MW)-assisted carbonization and sulfonation was employed as the catalyst for the conversion of xylose to furfural in dimethyl sulfoxide (DMSO). Fourier transform infrared (FT-IR) spectroscopy results indicated that RH-SO 3 H had typical signals of Brønsted acid groups while other characteristics were examined through other techniques, namely X-ray diffraction (XRD), energy-dispersive X-ray (EDX) spectroscopy, Raman spectroscopy, scanning electron microscopy (SEM), and elemental mapping. Through many investigations, the furfural yields were impacted by the nature of solvents, substrate concentrations, catalyst dosages, reaction temperatures, and reaction time. A furfural yield of 60.3% was obtained at 160 °C for 8 h. The catalyst recyclability and the scalability ability of the procedure were examined, and a mechanism was also proposed. CONCLUSION Rice husk could be used as a starting source to prepare a carbon material via a MW-irradiated protocol. The conversion of xylose to furfural under the catalysis of RH-SO 3 H was easily operated, and the desired product was obtained in good yield. The crucial advantages of the current process are environmentally friendly, inexpensive, simple, and highly large-scale application. The findings pave the way for eco-friendly industrial applications, promoting circular economy principles and reducing reliance on non-renewable resources in platform chemical production. © 2025 Society of Chemical Industry (SCI).
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jicheng Wang,Yanhong Quan,Linjie Li,Shunan Yin,Xinxin Ding,Jun Ren
A series of Cu/SBA-15 catalysts with different Cu loadings are prepared by the ammonia evaporation method for the liquid-phase hydrogenation of furfural (FF) to furfuryl alcohol (FA). The results show that the supported Cu loading influences the structure and catalytic activity during FF hydrogenation. The 20Cu/SBA-15 catalyst shows the optimum performance with 99.3 % FF conversion, 99.0 % selectivity to FA, nearly pure FA product, and a turnover frequency reaching up to 81.7h −1 . The effect of Cu loading can be related to Cu dispersion and the interaction between the metal and support, which further promotes the surface Cu + /Cu 0 ratio. Additionally, the correlation of FF conversion with Cu + /Cu 0 ratio confirms that the excellent performance of 20Cu/SBA-15 is mainly derived from the synergy of Cu + and Cu 0 species, although the range of performance is not large. Finally, the optimal reaction conditions are screened using a reaction temperature of 150 °C, a reaction pressure of 4 MPa, a catalyst dosage of 0.1 g, and a reaction time of 60 min. The present study confirms that the Cu loading has a significant effect on the structure of Cu/SBA-15 and nearly pure objective FF product can be feasibly obtained with an appropriate Cu support in the synthesis of FA from FF hydrogenation.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ye Tian,Wenlong Xie,Zihao Yang,Zhendong Yu,Renjie Huang,Lin Luo,Miao Zuo,Zheng Li,Lu Lin,Xianhai Zeng
Selective ring-opening hydrogenolysis of furfural (FF) to 1,5 pentanediol (1,5-PeD) is crucial for biomass valorization. However, achieving accurate bond-breaking is challenging. Herein, we report a facile method to synthesize layered double hydroxide nanoflake (ZnCo-LDH) mediated via Co 2+ etching ZIF-8 with NaBH 4 in water at ambient temperature. The structure, morphology, and chemical properties of synthesis catalysts with different concentrations of Co 2+ were characterized. The results indicated a partial ZIF-8 structure in ZnCo-LDH, with increased Co 2+ concentrations leading to catalyst agglomeration. Furthermore, the constitutive relationships between the catalyst’s properties and 1.5-PeD yields were established. Moreover, Co introduction altered the catalyst surface’s Brønsted and Lewis acids content. Density functional theory (DFT) indicated enhanced H 2 adsorption and dissociation due to electro-transfer between Co and Zn species, with a tilted configuration favoring ring opening. Finally, a possible reaction mechanism was proposed. This work provides valuable insights for preparing ultrathin nanoflake ZnCo-LDH catalysts for biomass-derived furfur compound upgrading.
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ACS Catalysis
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2024
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IF 11.3
Weijie Geng,Di Zhang,Ni Zhen,Jianxin Du,Jing Dong,Chengpeng Liu,Shi-Lu Chen,Yingnan Chi,Changwen Hu
The electrochemical coupling of biomass platform molecules to biofuels provides a promising method for addressing energy crises and environmental issues. However, achieving high yields of C–C coupling products under ambient conditions remains a challenge. Herein, we present a highly efficient electrocatalyst, [Cu(pz)]3[PW12O40] (Cu-PW12), fabricated by combining a Cu-pz complex (pz = pyrazine), a redox catalytic center, with Keggin-type PW12O40, and an electron sponge. Cu-PW12 exhibits remarkable catalytic activity for the electroreductive C–C coupling of furfural (FF), a bulk and low-cost biomass platform chemical, to produce a jet fuel precursor, hydrofuroin (HDF). Under neutral and ambient conditions, over 99% of FF is converted and the selectivity of HDF reaches 91.2%. Furthermore, experimental and theoretical studies, including control experiments, kinetic isotope studies, electrochemical and spectral analyses, and DFT calculations, reveal a synergistic catalysis effect between Cu center and PW12. The introduction of PW12 not only facilitates electron transfer, improving FF conversion, but also changes the rate-determining step, favoring the formation of HDF. Under turnover conditions, the Cu-PW12 catalyst is initially reduced and then FF is reduced by the Cu center to ketyl radical after protonation on the electrode surface. Finally, the self-coupling of two ketyl radicals in solution leads to the generation of HDF.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2020
·Vol. 95
·期 9
·2537-2548
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IF 2.75
Liquan Zhang,Can Wang,Hairong Zhang,Haijun Guo,Lian Xiong,Hailong Li,Xuefang Chen,Xinde Chen
BACKGROUND Levulinic acid (LA) and furfural are important biomass-based platform compounds. During the preparation of LA and furfural from lignocellulosic biomass, other organic chemicals including sugars, formic acid, acetic acid, and acid-soluble lignin (ASL) will be produced simultaneously. Thus, the purification of LA and furfural is an important process. In this work, a series of glycidyl methacrylate (GMA) modified hyper-cross-linked resins were synthesized and the mechanism of pore formation of the resins was studied. Furthermore, the effect of their textural properties on adsorption performance towards LA and furfural was investigated. RESULTS The hyper-cross-linked resin modified with 50 wt% GMA (PC-4) achieved the best adsorption performance. The adsorption capacities of LA and furfural onto PC-4 were 100.81 and 40.22 mg g −1 , respectively, which were 2423.76% and 249.24% higher than the un-modified resin HQ-8, and 31.0% and 22.7% higher than its precursor PR-4. During desorption process, the average desorption ratio of LA and furfural were 94.96% and 97.86%, respectively. Moreover, PC-4 also showed a good adsorption performance towards formic acid, acetic acid, and ASL, while sugar loss rate was about 5%. CONCLUSION This study not only reported a potential adsorbent, PC-4, for the comprehensive utilization of sugarcane bagasse hydrolysate, but it also studied the relationship between synthesis conditions, resin structures, and its adsorption performance of GMA modified hyper-cross-linked resins, which provides a guidance for new adsorbent design. © 2020 Society of Chemical Industry
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