FUEL
·
2023
·
IF 7.4
Honghui Gong,Juan Zhang,Qi Li,Longxing Wei,Ya Hu,Yifan Rui,Xian-Lei Shi
A series of sulfonic acid functionalized coffee biochar (SFCB-x) with high acid density and strength were prepared by using sulfuric acid as the sulfating agent. The obtained catalysts could be directly used for esterification of levulinic acid (LA) and alcoholysis of furfural alcohol (FA) affording ethyl levulinate (EL). Further activity tests and characterization confirmed the linear correlation between the catalytic activity and -SO 3 H density of the catalyst, SFCB-4 holds the highest -SO 3 H density and thus exhibits the highest catalytic activity towards the production of EL. Under mild conditions, about 97.6% and 81.7% yield of EL could be obtained for LA esterification and alcoholysis of FA, respectively. The catalyst also shows high stability during consecutive catalytic recycles. Furthermore, hot filtration testing suggested that the leaching of the active species was not observed during catalytic recycles, which could be attributed to the covalently linked -SO 3 H groups on SFCB-4 skeleton. The rational design and construction of SFCB-4 will drive the development of solid acid catalyst derived from natural biomass for the production of bio-based chemicals.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinxin Li,Linchuan Cong,Yupeng Wu,Nan Lin,Fangbing Liu,Deyuan Xin,Fuyu Han,Jin Yang,Weitong Chen,Haibo Lin
Electrochemical methods for catalytic furfural conversion have drawn significant interest in both academic and industrial research communities. Paired electrocatalytic conversion has been identified as a promising strategy for reducing energy consumption and promoting carbon neutrality. To optimize product distribution and conversion efficiency, we have developed a divergent paired electrochemical upgrading approach for furfural in acidic environments, with a focus on prioritizing strong gas evolution reactions and product transformations. The high electrocatalytic activity of CuSn/CuF@Cu prepared by electrodeposition can effectively inhibit the hydrogen evolution. The performance of the electrocatalysts and the pathways of electrocatalytic hydrogenation (ECH) of furfural to 2-methylfuran (MF) were investigated by combination of experiments and the density functional theory (DFT) calculations. A stable Ti/PbO 2 electrode with high oxygen evolution overpotential was prepared for anodic electrocatalytic oxidation (ECO) and the product transformation route was described. The conversion of furfural to maleic acid (MA) and MF in acidic environment was successfully achieved. In the paired electrosynthesis system, the electrons generated from anodic ECO of furfural are utilized in valuable and controllable cathodic ECH. It significantly and continuously reduces the power cost associated with renewable energy sources and further promotes the development of biomass electrochemical conversion.
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高影响因子
FUEL
·
2022
·
IF 8.035
Lungang Chen,Yong Liu,Xinghua Zhang,Jianguo Liu,Qi Zhang,Longlong Ma
Catalytic conversion of biomass to liquid fuel is one of critical part to ease dependence on fossil fuel. Herein, a route of transformation of biomass-derived furfural and levulinic acid into long-chain hydrocarbon fuels was developed. A C20 oxygenate with 95 % mol yield was firstly synthesized through condensation-polymerization reactions catalyzed by NaOH. Various techniques were employed to verify the chemical structure of the C20 oxygenate. The condensation mixture was then directly subjected to hydrodeoxygenation reaction to prepare long-chain hydrocarbons with a catalytic system of Pd/C and H 3 PO 4 in aqueous phase. A 57.1 % weight yield of liquid fuel was obtained with main products of C12, C14, and C18 hydrocarbons. The mass percent of carbon and hydrogen in fuel was significant improved to 95.91 %, as well as the high heat value was increased to 47.04 MJ/kg.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 45
·17119-17126
·
IF 8.067
Tian Wang,Jinlian Zhu,Kaiwei Zhang,Jing Wang,Yonggui Liao,Guochuan Yin,Xiaolin Xie
Transformation of bulky biomass into a carbon source for the chemical industry is important as it can provide different monomers for the syntheses of high-performance and/or functional polymers. In this work, Pd-catalyzed carbonylative esterification of methyl 5-bromofuroate, derived from renewable furfural, to dimethyl 2,5-furandicarboxylate (DMFD) has been explored under mild conditions with CO as the reductant source. The prepared DMFD was then used as a bi-functionalized monomer for the synthesis of a photo-responsive liquid crystalline polymer (PAzo-DMFD) through melt polycondensation. This furan-based polyester PAzo-DMFD shows excellent thermal stability and reversible trans–cis photo-isomerization in chloroform solution and in thin films benefitting from the azobenzene unit along the polymeric backbone. Photoisomerization of PAzo-DMFD can be used in the writing and erasing of information under light irradiation, thus providing new opportunities for the syntheses and applications of functional furan-based polymers.
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Reaction Chemistry & Engineering
·
2022
·Vol. 8
·期 2
·377-388
·
IF 5.2
Tiefu Li,Jiaming Liu,Zipeng Li,Peng Zhang,Yunlong Yao,Zhichao Sun,Yao Wang,Ying-Ya Liu,Anjie Wang
A monolith reactor was fabricated by growing carbonaceous fibers in a copper tube (i.d. 2 mm) via copper-catalyzed acetylene polymerization. The fibers were oxidized with air to convert CC bonds to CO bonds and to improve hydrophilicity. –SO3H groups were anchored on the surface by amination. Cu species were introduced by deposition and subsequent reduction. The resultant Cu/CF-SO3H monolith reactor was used to continuously and selectively convert furfural to furfuryl alcohol. At 180 °C, the monolith catalytic reactor performed significantly and stably in a 500 h run, maintaining a 100% conversion with a >99% selectivity. Additionally, the monolith reactor also performed well in continuous transfer hydrogenation of other α,β-unsaturated compounds, including 5-hydroxymethyl-2-furaldehyde, benzaldehyde, and cyclohexanone.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Ravi Balaga,Peifang Yan,Kishore Ramineni,Hong Du,Zhi Xia,Mahender Reddy Marri,Zongchao Conrad Zhang
Furfural is an important bio-based platform chemical in the production of valuable products such as biofuel intermediates and polymeric materials. In this work, isolated Zr on mesoporous silica catalysts at varied Zr loading were prepared and evaluated for aldol condensation of furfural with acetone to 4-(2-furyl)− 3-buten-2-one(FAc) and 1,5-bis-(2-furanyl)− 1,4-pentadien-3-one(F 2 Ac). A remarkable effect of the Zr loading on the catalyst performance is revealed. The catalysts are characterized by XRD, BET, NH 3 -TPD, Py-FTIR, XPS, UV–visible, and TGA. The connectivity of Zr was characterized by XPS and UV–visible spectroscopy. For the 25 wt% Zr loading, Zr is present predominantly as isolated monomeric species on mesoporous SiO 2 . The types and densities of different acid sites of the catalysts are measured with Py-FTIR analysis. The results show that isolated Zr on mesoporous SiO 2 enhanced Lewis acid site densities and exhibited superior catalytic activity for aldol condensation between furfural and acetone to produce FAc and F 2 Ac.
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Materials Advances
·
2022
·Vol. 3
·期 9
·3885-3896
·
IF 0
Xing-Long Li,Rui Zhu
Developing an economic catalyst to upgrade furfural to cyclopentanol is highly significant for fine chemical synthesis and biomass utilization. In this manuscript, an efficient and economical multi-functional porous Co-400 catalyst was developed. This catalyst obtained porosity, magnetism, Lewis acidity and hydrogenation activity via simple reduction of purchased Co3O4. Various factors were investigated in detail, and 87% yield of CPL could be obtained when Co-400 was used as the catalyst. The active sites of the catalyst were identified according to XRD, IR, XPS, SEM and Raman analysis. Moreover, the keys to the high activity and chemoselectivity of the Co-400 catalyst were mainly attributed to highly dispersed Co0 species and amorphous porous Co3O4 species, which were precisely controlled by the reduction temperature. The catalyst can be easily separated by magnetism. Furthermore, a possible reaction mechanism was proposed based on a series of controlled experiments and catalyst characterizations.
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Biomass Conversion and Biorefinery
·
2022
·
IF 4.05
Chen Dong,Chen Shanshuai,He Liang,Guan Qingqing,Miao Rongrong
Porous biochar was prepared from agricultural and forestry wastes to remove Cr(VI) in sewage, which solved the problem of water pollution and realized the reuse of wastes. Herein, in this work, the bagasse pith residues after alkali pre-extraction have been used as the raw material for preparing porous biochars ( BPR -BC), which could be further used for efficiently purifying the simulated Cr(VI) wastewater. The results showed that the as-prepared biochars had an ultra-high specific surface area of 2745.7 m 3 /g and Cr(VI) removal capacity of 185.07 mg/g. The kinetic and isotherms studies were best described by pseudo-second-order model and Langmuir adsorption isotherm model, respectively. The thermodynamic studies showed that the adsorption process was endothermic and spontaneous. Furthermore, based on the concept of “waste to waste,” the Cr-contained waste adsorbent by doping Cu has been converted into a bagasse pith residues biochar supported Copper-Chromium catalyst (Cu-CrOx/ BPR -BC) for further hydrogenation of furfural. The catalytic experimental result showed that the furfural 1 can be selectively converted into furfuryl alcohol (FOL) and difurfuryl ether (DEF) catalyzed by the prepared Cu-CrOx/ BPR -BC catalyst, provided a new idea for the further utilization of Cr(VI) containing adsorbents.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Yaru Xu,Zhaoyang Xu,Zhidong An,Junmou Zhou,Jiang Li
Catalytic transfer hydrogenation (CTH) recently attracts significant attention in biorefinery due to the free of using high-pressure fossil-derived H 2 that potentially reduce the equipment cost. Herein, up to 20 kinds of metal oxide-nitrogen-doped carbon (MO x -N-C) hybrid catalysts are prepared via a hydrothermal method followed by heat treatment under argon, and the successful preparation of such hybrid catalyst is confirmed by various means. Al is found to be the best element to construct such hybrid catalyst towards CTH, giving 96.6% yield of furfuryl alcohol at 99.3% furfural conversion at 120 o C for 6 h. By combining various characterization techniques, the deactivation and regeneration of AlOx-N-C catalyst is attributed to the change in specific surface area, pore volume, and the number of oxygen vacancies. The excellent catalytic performance of AlO x -N-C catalysts provides a broader prospect for its utilization in other biomass conversions as catalysts or active supports.
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FUEL
·
2022
·
IF 8.035
Xing Gao,Yingying Ding,Lilin Peng,Dan Yang,Xiaoyue Wan,Chunmei Zhou,Wen Liu,Yihu Dai,Yanhui Yang
Aqueous phase hydrogenative rearrangement of furfural (FAL) to cyclopentanone (CPO) via furfuryl alcohol (FOL) has been studied over Pd catalysts supported on H–ZSM–5 zeolites. Pd states, zeolite properties and reaction condition parameters were optimized, affording 98% selectivity and 120 h −1 specific reaction rate over 2% Pd/H–ZSM–5(25) catalyst at 160 °C and 3 MPa H 2 . For hydrogenation of FAL–to–FOL, the activity was related to the Si/Al ratio and acid property of zeolite supports. For hydrogenative rearrangement of FOL–to–CPO, pure H–ZSM–5 zeolite could catalyze single–step conversion with relatively low reaction rate, whereas the presence of Pd sites could achieve multi–step transformation with remarkably increased rate, highlighting Pd–zeolite acid sites synergy. Proton and furanylmethoxy–relevant intermediates were captured with spin trapping electron paramagnetic resonance experiments, and 4–hydroxy–2–cyclopentenone and 2–cyclopentenone were also identified as key intermediates in tandem reaction pathway to produce CPO.
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ENERGY & FUELS
·
2021
·
IF 3.605
Yao Liu,Rulu Huang,Junhua Zhang,Liang He,Lincai Peng
Hydrogenation reduction of furfural (FAL) to furfuryl alcohol (FOL) confirms the requirement of sustainable development of society. The key to realize this transformation is to design a cost-effective and environmental catalyst with both Lewis acid and Lewis base sites. Here, we report the preparation of a multifunctional zirconium-based hybrid (Zr@PS-MSA) using Pennisetum sinese (PS), an annual natural lignocellulose, as a natural organic ligand. The prepared hybrid was used as an efficient catalyst for catalytic transfer hydrogenation (CTH) of FAL to FOL in isopropanol, and a high yield of up to 99.6% was accomplished by manipulating exposed versatile acid–base sites. Further studies indicated that Zr@PS-MSA possessed remarkable cycle stability and could be consecutively run at least 6 times without significant change in the catalytic activity. Mechanistic studies for CTH of FAL to FOL through isotopically labeled 2-propanol-d8 experiments evidently demonstrate FAL reduction via intermolecular hydrogen transfer. More gratifyingly, Zr@PS-MSA can also efficiently catalyze the various biomass-derived carboxides to corresponding alcohols, with yields of up to 92.4%.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yujia He,Rui Zhang,Weipeng Song,Huai Liu,Junhua Zhang,Wenlong Jia,Lincai Peng
The simultaneous valorization of biomass-based C5 and C6 sugars to furfural, a versatile intermediate, is of great significance to fully utilize biomass components. Inability to effectively transform C6 sugars remains a major barrier toward this challenging goal. We herein report the 1,4-dioxane-mediated solvent system with Hβ zeolite catalyst for the transformation of glucose giving high yield to furfural (57%). The maintenance of intrinsic balanced Lewis and Brønsted acid sites from Hβ zeolite that is credited to the positive solvent effect of 1,4-dioxane is highly conductive to the selective C-C bond cleavage of glucose. Also importantly, the introduction of proper amount of H 2 O into the reaction system results in a high formation rate and an improved selectivity toward furfural due to the induction of highly reactive acyclic glucose. Glucose-to-furfural through 3-deoxyglucose should be more favorable than that via fructose. Impressively, the developed protocol can also be adapted to C5 sugars dehydration, and the one-pot conversion of glucose and xylose mixtures gains a furfural yield as high as 63%. The activation energy barrier for furfural production is higher from glucose compared to xylose. This work not only develops a promising protocol for furfural production simultaneously from C5 and C6 sugars but also provides insights into the mechanistic role of the solvent 1,4-dioxane to availably manipulate the acid-catalyzed conversion of C6 sugars.
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