Biomass Conversion and Biorefinery
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2024
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IF 3.5
Li Yihui,Zhong Zhaoping,Wang Wei,Ye Qihang,Zheng Xiang,Liu Hengyuan,Yun Zekun
The valorization of cellulose in lignocellulose into high-value products is a crucial step in biorefinery processes. In this study, FeCl 3 ·6H 2 O was impregnated and supported on a carbon-based substrate, followed by carbonization and sulfonation to prepare the composite carbon-based solid acid. The resulting composite carbon-based solid acid was used as the catalyst, while γ-valerolactone, a lactone solvent, served as the reaction medium for producing furfural as the product from cellulose. When using this catalytic system to treat cellulose, under appropriate reaction temperature and residence time, the yield of furfural reached 75.26%, while the conversion rate of cellulose was 99.8%. Characterization techniques including SEM, EDS, XRD, XPS, and Py-FTIR were employed to confirm that the composite carbon-based solid acid possessed Brønsted acid sites, Lewis acid sites, and -Cl active groups, all of which exhibited excellent catalytic activity and selectivity towards furfural production. Furthermore, the synergistic effect between the catalytic activity of the three active groups in the carbon-based solid acid and the inhibitory effect of the nonpolar solvent on side reactions contributed to the outstanding performance of the catalytic system. And this study proposes a possible reaction pathway for the conversion of cellulose to furfural. This research provides an efficient pathway for the valorization of cellulose and holds significance in furfural production and biomass conversion. Graphical abstract
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Aozhou Wang,Kaisheng Yao,Shuaibo Li,Qi Wang,Tianhang Han,Weiwei Lu,Haili Zhao
Furfuryl alcohol (FA) is an important chemical and has extensive applications in varied fields. To realize the highly selective hydrogenation of furfural (FF) to produce FA, the key is the preparation of the catalysts with excellent performance. Herein, a very simple wet chemical method is developed for the one-step preparation of PdAg nanosponges (NSs). Specifically, with Pd(OAc) 2 and AgNO 3 as precursors, and ethylene glycol (EG) as both solvent and reducing agent, PdAg NSs can be grown and assembled at mild temperature of 40 °C. Throughout the reaction, no any surfactants and additional reducing agents are applied. The as-prepared PdAg NSs possess 3D self-supported alloy structures, “clean” surface, abundant pores, high specific surface area and rich defects. In the FF hydrogenation reaction at 60 °C under 1.5 MPa H 2 pressure in the mixed solvent of ethanol and water (1 : 4 in volume ratio), the self-supported PdAg-1 NSs (1 : 1 in Pd/Ag molar ratio) exhibit superior catalytic performance than other PdAg NSs, pure Pd sample and commercial Pd/C (10%). With PdAg-1 NSs as catalyst in the absence of support, 100% FF can be converted and the selectivity toward FA is as high as 97.1% at 36.0 h of reaction. After 4 cycles, PdAg-1 NSs still maintain the high catalytic activity in FF hydrogenation and high selectivity toward FA, which may originate from the 3D self-supported structures, high specific surface area, “clean” surface, rich defects and electronic synergistic effect between Pd and Ag. This simple fabrication of PdAg NSs introduces new ideas for the synthesis of other nanostructured bi- and multi-metallic catalysts for highly selective FF hydrogenation to FA and other advanced applications.
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Journal of Materials Chemistry A
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2024
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IF 10.7
Yuhui Huang,Yehan Tao,Qingqing Wang,Jian Du,Jinwen Hu,Jie Lu,Yanna Lv,Haisong Wang
To develop an industrial zeolite-based catalyst for efficient furfural production, the acidity, pore structure, and electronic properties of H-β zeolite were modulated by synergistic deatomization and atomic implantation treatments. The dealumination effectively decreased the intrinsic aluminum-related Lewis and Brosted acid sites, thus decreasing the occurrence of unwanted side reactions. Meanwhile, the removed skeleton aluminum can create voids for the following atomic implantation of introducing higher valent-state niobium species, which would provide new kinds of catalytic active sites, increase the average pore size by distorting the zeolite skeleton, and enhance the interaction with reactant molecules by acting as more electron deficient centers. In a single-phase water/γ-valerolactone reaction system, the optimum catalyst can efficiently convert both xylan and xylose with a conversion of 100 % at a medium temperature of 130 ℃ within 3 hours. Compared with the furfural yield over untreated H-β (12.7%), the yield over deAlβ/Nb(20%) catalyst was greatly enhanced by 54% with xylose as raw material. The catalyst can be recovered by simple cleaning and thermal regeneration and then reused. The proposed post-treatment strategy could maintain the integrity of the zeolite structure, ensure uniform and stable metal dispersion under harsh conditions, manage the complexity and cost of the preparation process, and most importantly, optimize the catalytic performance. Addressing these issues is essential for improving the efficiency and practical application of industrial zeolite catalysts by this general approach and benefiting industrial furfural production.
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Polymers
·
2024
·Vol. 16
·期 23
·3421
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IF 4.7
Zhiyin Zhang,Huimin Hu,Jie Yang,Zhengguang He,Guangyue Zhu,Chang Wen
Resource use is crucial for the sustainable growth of energy and green low-carbon applications since the improper handling of biomass waste would have a detrimental effect on the environment. This paper used nano-ZnO and ammonium persulfate ((NH4)2S2O8, APS) as a template agent and heteroatom dopant, respectively. Using a one-step carbonization process in an inert atmosphere, the biomass waste furfural residue (FR) was converted into porous carbon (PC), which was applied to the supercapacitor electrode. The impact of varying APS ratios and carbonization temperatures on the physicochemical properties and electrochemical properties of PC was studied. O, S, and N atoms were evenly distributed in the carbon skeleton, producing abundant heteroatomic functional groups. The sample with the largest specific surface area (SSA, 855.62 m2g−1) was made at 900 °C without the addition of APS. With the increase in adding the ratio of APS, the SSA and pore volume of the sample were reduced, owing to the combination of APS and ZnO to form ZnS during the carbonization process, which inhibited the pore generation and activation effect of ZnO and damaged the pore structure of PC. At 0.5 A g−1current density, PC900-1 (FR: ZnO: APS ratio 1:1:1, prepared at 900 °C) exhibited the maximum specific capacitance of 153.03 F g−1, whereas it had limited capacitance retention at high current density. PC900-0.1 displayed high specific capacitance (141.32 F g−1at 0.5 A g−1), capacitance retention (80.7%), low equivalent series resistance (0.306 Ω), and charge transfer resistance (0.145 Ω) and showed good rate and energy characteristics depending on the synergistic effect of the double layer capacitance and pseudo-capacitance. In conclusion, the prepared FR-derived PC can meet the application of a supercapacitor energy storage field and realize the resource and functional utilization of biomass, which has a good application prospect.
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NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Yun Wang,Jiayang Wang,Zhiyang Zhang,Runsheng Xu,Shuang Wang
The reductive amination of biomass-derived furfural over non-noble metal catalysts represents a promising but challenging strategy for the sustainable synthesis of furfurylamine. Herein, we report mesoporous carbon supported CoZn bimetallic catalysts (CoxZny@MC) via a one-pot solvent evaporation induced self-assembly (EISA) method for high-efficiency reductive amination of furfural to furfurylamine with hydrous hydrazine (N2H4⋅H2O) as a nitrogen source. A complete conversion of furfural with a 97.5% yield of furfurylamine was achieved over bimetallic Co1Zn3@MC catalyst under mild conditions of 100 °C and 1.5 MPa H2 for 3 h. Furthermore, Co1Zn3@MC could be reused for at least five times with only a slight loss in activity. The excellent performance of the Co1Zn3@MC catalyst was mainly attributed to the introduction of moderate Zn species, which led to high dispersion of Co particles on the catalyst surface, as well as the abundant mesopores and high specific surface area of the catalyst. Moreover, a significant electron transfer from Zn species to Co centers occurs, which improves the inherent catalytic activity of the non-noble bimetallic catalyst by enhancing the electron density of Co particles.
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MOLECULES
·
2025
·Vol. 30
·期 2
·225
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IF 4.6
Jieqiong Wang,Jingyi Yang,Zezheng Bing,Yuanyuan Gao,Tao Yang,Qiaoyun Liu,Meng Zhang,Zhongyi Liu
Controllable hydrogenation of carbonyl groups (C=O) is crucial for converting furfural into high-value furfuryl alcohol. Instead of traditional impregnation method, a novel Cu-based catalyst (Cu/SiO2) is prepared using the ammonia evaporation method (AE) for the efficient hydrogenation of furfural to furfuryl alcohol under mild conditions. At the reaction conditions of 90 °C and 1 MPa H2, the 5Cu/SiO2-AE sample showed optimal performance with higher turnover frequency (36.0 h−1) and furfuryl alcohol selectivity (>99.9%). After five cycles, the catalyst recycled still showed a high reaction activity and selectivity for furfuryl alcohol. Characterization results such as XRD, H2-TPR, FT-IR, and XPS showed that the excellent catalytic performance of 5Cu/SiO2-AE catalyst was attributed to the formation of layered copper silicate and the high dispersion of Cu species. Furthermore, the formation of layered copper silicate resulted in a higher ratio of Cu+/(Cu0+Cu+) at a reduction temperature of 250 °C, which was also responsible for the optimum activity. This work showed the importance of controllable synthesis of layered copper silicate in improving the catalytic performance of copper-containing catalyst.
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ACS Catalysis
·
2025
·
IF 13.1
Yuanjing Zhang,Guanyi Zhang,Quandong Hou,Shiquan Zhao,Si Wang,Enze Xu,Lei Wang,Xin Zhang,Feng Li,Yusen Yang,Min Wei
Aqueous-phase tandem reactions, as a fundamental aspect of green chemistry, hold a crucial position in the contemporary synthesis of fine chemicals, wherein the advancement of high-performance heterogeneous catalysts remains a formidable challenge. Herein, we report a Pt1Con single-atom alloy (SAA) catalyst in which Pt single atoms are immobilized onto the surface of Co nanoparticles through Pt–Co coordination. The Pt1Con SAA catalyst exhibits a high chemoselectivity for the aqueous-phase hydrogenation–rearrangement reaction of furfural (FAL) to cyclopentanol (CPL) (yield: >93%, considering the carbon loss), with a TOF value of 2257 h–1 (based on Pt). A joint investigation based on reaction dynamics, isotope-label tracing experiments, EPR, and in situ FT-IR verifies a five-step consecutive tandem reaction pathway for the formation of CPL. Notably, during the reaction, the rapid exchange of hydrogen atoms would occur between activated hydrogen species and the water solvent. Furthermore, the water molecule does not serve as a H-donor but is involved in the rearrangement reaction in the side chain of the furan ring. Kinetic studies combined with DFT calculations substantiate that the Pt–Co interface sites effectively lower the energy barrier of the cyclopentanone (CPO) hydrogenation step via facilitating activation adsorption of the carbonyl group, accounting for the largely enhanced catalytic behavior. This study sheds light on the advancement of a highly efficient and stable heterogeneous catalyst for a biomass upgrading reaction in the aqueous phase.
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Materials Today Chemistry
·
2025
·
IF 6.7
Tianwei Wang,Hua Lin,Zhicheng Tang,Rongwen Lu,Shufen Zhang
The hydrogenation of furfural (FFA) to tetrahydrofurfuryl alcohol (THFOL) is of immense commercial significance. This transformation, however, remains challenging and often requires high temperature and pressure to achieve high selectivity, or more importantly, the design and development of novel catalysts. Herein, we develop the rattle-typ (Pd@HASs) nanoreactors for selective hydrogenation of FFA to tetrahydrofurfuryl alcohol at mild condition via a regulatable metal-doped vesicles method, which was assembled from the double hydrophobic anionic surfactant AOT (sodium dioctyl sulfosuccinate). The structure and growth process of the Pd@HASs were analyzed by HRTEM, SEM, XPS and DLS. Through the regulation means which modulated the metal coordination or anionic environment, the metal-doped vesicles with tunable size and distribution of metal nanoparticles could convert to a series of Pd@HASs with different cavity sizes from 32 nm to 144 nm. The Pd@HASs exhibited great selectivity in FFA hydrogenation, with a tetrahydrofurfuryl alcohol yield of >99 % within an hour at 120 °C, 10 bar H 2 pressure. Among the nanoreactors with different cavity sizes, Pd@HASs with a 50 nm cavity has the best performance. This work provides a new way for the design and synthesis of hollow alumina nanospheres encapsulated metal nanoparticles nanoreactors, and the selective hydrogenation of FFA at mild condition.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yakai Chen,Xinya Feng,Xiaohan Yu,Xingliang Xu,Jing Xu
Catalytic aldol condensation of biomass-derived furfural (FAL) with acetone (AC) into the single-condensation product 4-(2-furyl)-3-buten-2-one (FAC) is a potential and promising strategy for biomass improvement process and still challenging. Metal oxides exposed different crystal facets can regulate their surface structure and adsorption activation ability, which can provide an opportunity to enhance aldol condensation performance. Here, nanoparticles-CeO 2 (P-CeO 2 ), nanorods-CeO 2 (R-CeO 2 ) and nanocubes-CeO 2 (C-CeO 2 ) with (111), (110) and (100) plane predominant exposure was prepared to explore their catalytic performance for the aldol condensation of FAL with AC to obtain FAC. The serial detailed characterizations, experimental results and density functional theory calculation revealed that R-CeO 2 with a dominant (110) facet possesses appropriate surface adsorption energy, abundant oxygen vacancy (Ov) and excellent acid-base properties, which can effectively boost the adsorption and activation of FAL and AC and reduce the barrier of aldol condensation reaction based on the acid-base catalysis mechanism. The work would reveal the influence of CeO 2 crystal facet on the aldol condensation and provide a broad potential for the rational design of metal oxide catalysts for other acid-base catalytic reactions.
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FUEL
·
2024
·
IF 6.7
Ying Qiu,Huiyu Liu,Rui Shan,Wei Zhao,Junhua Zhang,Jun Zhang,Haoran Yuan
In the present study, the ultra-large specific surface area Zr-decorated hyper-cross-linked polymers (HP) were firstly developed for the catalytic production of furfuryl alcohol (FOL) from furfural (FAL) using isopropanol as both the hydrogen source and solvent. Comprehensive characterizations were performed to uncover the basic physicochemical properties. The as-prepared Zr/HP showed large specific surface area of ∼1000 m 2 /g, good dispersion of Zr species, plentiful acidity and basicity. 2.5Zr/HP presented the highest activity in the FAL-to-FOL transformation, wherein 97.4 % FAL conversion and 92.9 % FOL yield were achieved within 2 h at 160 °C. The recycling experiments revealed that the as-fabricated Zr-decorated hyper-cross-linked polymers presented good recyclability without significant loss of reactivity even after two consecutive cycles, owing to the strong interaction between hyper-cross-linked polymers and grafted Zr species. Kinetical analysis verified that the activation energy for transfer hydrogenation of FAL could be lowered to a certain degree, especially in the case of lower Zr loadings. More gratifyingly, the Zr-decorated hyper-cross-linked polymers were capable of catalyzing other unsaturated compounds with high conversion rates. In addition, the plausible pathway for the FAL-to-FOL transformation over Zr-decorated hyper-cross-linked polymers was proposed.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Xiongqin Liu,Xuanrui Liu,Jun Zhao,Mingruo Ban,Shutao Wu,Fei Liu
The electrochemical reduction of furfural (FF) offers a sustainable approach for producing value-added furfural alcohol (FA). Nevertheless, the limited adsorbed hydrogen (*H) generation capacity on Cu cathode restricts the reaction performance. Because the competitive adsorption of FF and *H decreases *H coverage and induces severe dimerization, most prior studies employed low FF concentrations (typically 20 mM) under constant potential conditions. In this work, carbon-supported Cu nanoparticles grown on Cu nanowire arrays (defined as Cu@Cu/C) were combined with constant current electrolysis for high-concentration FF reduction. A high Faradaic efficiency (72.9 %) and production rate (0.14 mmol cm −2 h −1 ) of FA were realized at −10 mA cm −2 , with a conversion of 98.1 %. Both the Faradaic efficiency and production rate can be sustained with gradual increases in current density or adjustments of FF concentration within a certain range, showing substantial enhancement relative to Cu-nano. Compared with pure Cu-nano, the favorable interaction between Cu nanoparticles and carbon support was certified to regulate the adsorption configuration and strength of FF, and enhance the *H generation performance, which optimizes the *H coverage at cathodic surface and promotes FF hydrogenation with *H via an electrocatalytic hydrogenation (ECH) mechanism. Overall, this work provides a simple and feasible strategy to promote interfacial *H, thus enhancing higher concentration hydrogenation of FF to FA by constant current electrolysis over Cu-based cathode.
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TALANTA
·
2025
·
IF 6.1
Zhanjun Li,Yunwei Liu,Mingru Kong,Yibin Xu,Kunlun Wang,Ke Ma,Qingfen Zhang
This study focused on the valorization of Pinus koraiensis seed scale residues for furfural production from regenerated hemicellulose via solid acid catalysis. The optimized process included solid acid catalysis, ultrasonic pretreatment, and microwave-assisted processing, and the optimal conditions were 50% ethanol (30:1 mL/g), 80 W of ultrasonic power (10 min, 40°C), 3% solid acid, and 385 W of microwave power (20 min), resulting in a theoretical furfural yield of 10.50 mg/g and an actual yield of 10.36 mg/g (conversion rate of 31.49%). The recovered solid acid exhibited similar catalytic performance to the fresh solid acid (yield of 10.23 mg/g and conversion rate of 31.11%). Kinetic analysis revealed that reaction equilibrium was reached within 10 min, with activation energies of 11.96 kJ/mol at 30–40°C and 25.24 kJ/mol at 40–50°C, indicating inhibition at higher temperatures. Characterization confirmed the acidity, high thermal stability and excellent reusability of the acid despite slight deactivation after recovery. Future research will focus on optimizing the efficiency and reusability of solid acid catalysts and exploring the use of regenerated hemicellulose derivatives in biobased chemical and sustainable material applications. As renewable and biodegradable resources with tunable structures, hemicellulose derivatives offer great potential for producing biobased chemicals, ecofriendly materials, and catalysts, advancing the biobased economy while reducing fossil fuel dependence and environmental impacts.
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