GREEN CHEMISTRY
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2026
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IF 9.2
Ting Xiang,Njud S. Alharbi,Xijun Wang,Changlun Chen
The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) coupled with hydrogen evolution offers a sustainable approach for producing value-added chemicals and green hydrogen. Achieving both high current densities and long-term operational stability remains a significant challenge. A metal–organic framework (MOF)-structured Co–Ni(TCNQ)2·2H2O nanorod-array catalyst demonstrates exceptional activity and durability for HMF electrooxidation. This bimetallic framework achieves high current density up to 1000 mA cm−2, requiring only 1.72 V in 1.0 M KOH with 200 mM HMF, which significantly outperforms Ni(TCNQ)2·2H2O and highlights the strong promoting effect of cobalt incorporation. Nearly complete HMF conversion and high selectivity for 2,5-furandicarboxylic acid (FDCA) are observed, along with excellent recyclability under concentrated substrate conditions. Operando and ex situ analyses indicate that cobalt doping mitigates over-oxidation and the associated irreversible structural transformation of the nickel sites stabilizes a dynamic Ni2+/Ni3+ redox cycle, and enhances charge delocalization through the TCNQ ligand. These effects collectively prevent over-oxidation and ensure sustained catalytic turnover. Density functional theory calculations confirm that cobalt strengthens HMF adsorption and facilitates FDCA desorption, thereby coupling efficient substrate activation with effective product release. This dual thermodynamic modulation explains the reduced onset potential and increased current density. Thus, Co–Ni(TCNQ)2·2H2O serves as a robust, selective, and scalable electrocatalyst, linking mechanistic understanding to industrial-scale biomass upgrading and simultaneous hydrogen generation.
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CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 13.2
Hao-Yue Ma,Jun-Fei Gu,Xing-Chuan Li,Zhan Chen,Qi-Yu Fu,Francis Verpoort,Wen-Jie Mo,Zheng Liu,Cheng Chen,Soon Hyeok Hong,Zongkui Kou
The transition from petroleum-derived chemicals to sustainable alternatives has intensified interest in 2,5-furandicarboxylic acid (FDCA), a biomass-derived monomer for green polyester production. However, many non-noble metal catalysts for converting 5-hydroxymethylfurfural (HMF) to FDCA still require multistep syntheses and/or harsh oxidation conditions. Here, we report a straightforward molten-salt strategy to prepare nitrogen-doped porous carbon–supported cobalt catalysts (Co@N-C-x). Under ambient air at 90 °C in water, the optimized [email protected] catalyst affords complete HMF conversion and > 99 % FDCA yield, with a productivity of ~1.17 mol FDCA mol Co −1 h −1 , and retains 96.5 % yield in an initial 400-fold scale-up test. Mechanistic and kinetic analyses support a sequential pathway of HMF → HMFCA → FFCA → FDCA, with the FFCA-to-FDCA step being kinetically most demanding under the present conditions. Structure–activity analysis, together with atmosphere-dependent experiments, indicates that Co–Nₓ sites serve as the primary catalytic centers, while adjacent defect-rich surface sites (denoted as O₂-activation sites) promote dioxygen activation and facilitate stepwise oxidation. Density functional theory calculations further show that FDCA binds more strongly to the catalyst surface than the intermediates, which can hinder product desorption and contribute to the observed loss of activity upon recycling.
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Energy Technology
·
2015
·Vol. 4
·期 5
·600-609
·
IF 2.824
Yating Shen,Yunlei Zhang,Yao Chen,Yongsheng Yan,Jianming Pan,Meng Liu,Weidong Shi
Stable oil-in-water high internal phase emulsions (HIPEs) with an internal phase volume fraction of 85 % were stabilized using Tween 85. The prepared poly(HIPEs) were first investigated as adsorbents to treat water polluted with Cr III , and then the catalysts with Lewis acidic sites was synthesized. The catalysts with Brønsted acidic sites were obtained by ion-exchanging. The as-prepared HIPEs–Cr III (PEs–Cr III ) and HIPEs–SO 3 H (PEs–SO 3 H) possess open-cell structure, interconnecting pores, and strong acidity, they are utilized as highly efficient catalysts for the conversion of biomass to 5-hydroxymethylfurfural (HMF). These results showed maximum production yields for cellulose, glucose, and fructose of 37.0 %, 58.0 %, and 80.8 %, respectively. PEs–Cr III and PEs–SO 3 H can be very easily recycled at least four times without significant loss of activity. Herein, a new method is presented to transform cellulose by using two catalysts in a one-pot process for meeting the varying demands involved at different reaction stages.
研究领域:
化学工程
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生物质能
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催化科学
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高影响因子
FUEL
·
2022
·
IF 8.035
Shuai Wang,Thomas L. Eberhardt,Hui Pan
A lignin-derived mesoporous carbon solid acid catalyst (LDMCC) was prepared using alkali lignin as a carbon source and KCl as a salt template to generate a carbon support that was carboxylated with acrylic acid. The prepared LDMCCs were characterized by various spectroscopies (FTIR, XPS, XRD, Raman), porosity determinations (BET), microscopies (SEM, TEM), thermogravimetric analysis, and acid-base titration. The LDMCC produced at the highest carbonization temperature (900 °C) possesses a rich porous structure, high specific surface area (1197.1 m 2 ·g −1 ), large pore volume (0.63 cm 3 ·g −1 ), and abundant –COOH groups (2.4 mmol·g −1 ). This weakly acidic catalyst exhibits excellent synergistic catalytic performance with DMSO in the catalytic dehydration of fructose to prepare 5-hydroxymethylfurfural (5-HMF); the yield of 5-HMF was 96.0% using dimethyl sulfoxide as the solvent, reaction conditions of 180 °C for 2.0 h, and a catalyst loading of 0.1 mg·mg −1 . In addition, the prepared LDMCC exhibits excellent reusability over five cycles of use without significant loss in its catalytic activity. This study provides a novel green route for the preparation of a weakly acidic catalyst which may be useful for a variety of biomass conversion processes.
研究领域:
生物质化学
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催化化学
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Journal of Central South University
·
2020
·Vol. 26
·期 11
·2974-2986
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IF 1.249
Xu Si-quan,Pan Dong-hui,Xiao Guo-min
With the aim of achieving a high 5-hydroxymethylfurfural (HMF) yield from glucose with H-ZSM-5 catalyst at low cost, three inexpensive biphasic reaction systems, H 2 O—tetrahydrofuran (THF), H 2 O—2-methyltetrahydrofuran (MeTHF) and H 2 O’2-butanol, were discovered and proved to be particularly effective in promoting the formation of HMF from glucose over H-ZSM-5 zeolite. In order to determine the optimal process conditions, the effects of various experimental variables, such as reaction temperature, reaction time, catalyst dosage, volume of organic solvent, as well as inorganic salt type on glucose conversion to HMF in three systems were investigated in detail. It was found that under optimal reaction conditions, H 2 O—THF, H 2 O—2-butanol and H 2 O—MeTHF allowed the glucose dehydration process to achieve HMF yields of up to 61%, 59%, and 50%, respectively. Moreover, in the three biphasic systems, the H-ZSM-5 catalyst was also demonstrated to maintain excellent stability. Thus, the catalytic approach proposed in this paper can be believed to have potential prospects for industrially efficient and low-cost production of HMF.
研究领域:
化学工程
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生物质转化
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催化科学
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FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Shiyun Mu,Kai Liu,Hong Li,Zhenyu Zhao,Xiaoqi Lyu,Yilai Jiao,Xingang Li,Xin Gao,Xiaolei Fan
This work presents an efficient method of supporting zirconia (ZrO 2 ) on COOH functionalized multi-walled carbon nanotubes (ZrO 2 /MWCNTs(C)) via a microwave (MW)-assisted method, which can be used as an efficient catalyst for converting fructose to 5-HMF. The developed composite by the MW-assisted route shows highly dispersed ZrO 2 with small sizes of 4–5 nm on the carbon support, which could not be achieved the conventional hydrothermal synthesis. Characterization shows a unique zirconia amorphous structure which was ascribed to the special interaction between the carbon support and MW irradiation. Specifically, MWCNTs were heated selectively due to their strong MW-absorbing ability, which led to the formation of microscopic “hot spots”, enabling rapid synthesis (8 min) of highly dispersed ZrO 2 with smaller sizes on the hot surface of MWCNTs. Conversely, under conventional heating, the nucleation rate of ZrO 2 was slow and prone to form agglomerated particles on the carbon support. The amorphous ZrO 2 contributed to the excellent activity of ZrO 2 /MWCNTs(C) in fructose conversion to 5-HMF. In detail, fructose conversion and 5-HMF yield were achieved at ~72.8% and ~62.9%, respectively, for the catalyst prepared by the MW method, whilst they are only about 24.7% and 15.7% over the catalyst prepared by the conventional hydrothermal synthesis.
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BIOMASS & BIOENERGY
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2022
·
IF 5.774
Gang Liu,Yujiao Xie,Chunjie Wei,Chang Liu,Feng Song,Xiuyu Sun,Yuan Zhang,Hongyou Cui
The one-pot approach was developed by using molten salt hydrate consisting of ZnCl 2 ·4H 2 O and LiCl·3H 2 O to produce 5-hydroxymethylfurfural (5-HMF) from cellulose . Cellulose was dissolved and regenerated to study the interaction of cellulose and molten salt hydrate. The effects of ZnCl 2 ·4H 2 O concentration, reaction time, and temperature on the conversion of cellulose to 5-HMF were investigated. 5-HMF yield increased when ZnCl 2 ·4H 2 O was mixed with LiCl·3H 2 O, and the maximum value (44.1%) was reached at 160 °C and 90 min when ZnCl 2 ·4H 2 O concentration was 64.9 mol%. The species of ZnCl 2 ·4H 2 O–LiCl·3H 2 O were analyzed, and the function of species concentration was correlated with the 5-HMF yield from the conversion of glucose and fructose. It was found that the synergistic catalysis of ZnCl 3 − , Zn 2+ , Zn(OH) + , H + as well as Li + promoted the efficiently cellulose conversion to 5-HMF.
研究领域:
化学工程
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催化
·
生物化工
·
可再生能源
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CELLULOSE
·
2022
·Vol. 29
·期 8
·4525-4537
·
IF 6.123
Wang Huiqiang,Fang Shengqiong,Zuo Miao,Li Zheng,Yu Xin,Tang Xing,Sun Yong,Yang Shuliang,Zeng Xianhai,Lin Lu
Removal of copper ions (Cu(II)) efficiently from water is crucial for water environment security. We use sustainable, low-cost, renewable cellulose derivatives (carboxymethylcellulose sodium (CMC-Na)) and polyvinyl alcohol (PVA) as the matrix, and cellulose nanocrystals (CNCs) as the functional addition. The CNC/CMC-Na/PVA hydrogel was prepared by the physical cross-linking method. Static adsorption experiments proved that CNC/CMC-Na/PVA hydrogel has a greater adsorption potential (108 mg/g) towards Cu(II). At the same time, the adsorption of Cu(II) on CNC/CMC-Na/PVA hydrogels is spontaneous and endothermic, and obeys the pseudo-second-order model with intra-particle diffusion. Furthermore, the primary adsorption mechanisms had been electrostatic attraction and surface complexation. Importantly, CNC/CMC-Na/PVA hydrogel has efficient absorbability and preferable reusability in actual water samples. Furthermore, the copper nanoparticles (Cu NPs) adsorbed on the surface of CNC/CMC-Na/PVA hydrogels were reduced with NaBH 4 in situ to realize the secondary utilization in CNC/CMC-Na/PVA hydrogels supported by Cu NPs. It is found that the material can be used as a catalyst to efficiently catalyze the conversion of HMF to BHMF (99%). Consequently, we provide insights into the hydrogel preparation that would possibly be promising novel adsorbents for the elimination of heavy-ion from sustainable water purification. Graphical abstract
研究领域:
环境科学
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材料科学
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化学工程
·
水处理
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BIOMASS & BIOENERGY
·
2026
·
IF 7
Chenxin Jin,Yajun Liu,Lingfeng Li,Yihan Wang,Changzhou Chen,Jianchun Jiang
This study investigated the electrocatalytic oxidative process of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) using Co/N-doped carbon catalysts derived from lignin subjected to different pretreatment methods, including enzymatic hydrolysis lignin (EHL), alkali lignin (AL), and kraft lignin (KL). The EHL-derived catalyst exhibited superior activity, achieving a current density of 110 mA cm −2 at 1.5 V vs. RHE along with 98% HMF conversion, 99.02% FDCA selectivity, and 98.4% Faradaic efficiency (FE). Structural characterizations and theoretical calculations revealed that the preserved aromatic framework of EHL promoted the formation of atomically dispersed Co–N x active sites and facilitated efficient HMF adsorption. The computational results further demonstrated that the optimized electronic structure of the Co-N x sites reduced the activation energy for the rate-determining step. This work demonstrated a direct correlation between the pretreatment history of lignin and its electrocatalytic performance, offering a precursor-based design strategy for efficient HMF electrooxidation.
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ChemCatChem
·
2026
·Vol. 18
·期 5
·e70637
·
IF 4.1
Yintao Song,Hang Zheng,Mengyuan Huang,Quanwei Deng,Luhui Lin,Yaqi Shi,Jiacheng Li,Chenting Yang,Lu Lin,Changlong Wang,Xing Tang
We have developed a highly efficient and stable non-noble metal-based heterogeneous catalyst for the selective oxidation of HMF to DFF. Mixed oxide catalysts with different Mn/Ni molar ratios were synthesized using the urea precipitation method. The Mn 6.6 NiO X catalyst exhibited a 95.33% HMF conversion rate and a 99.39% DFF selectivity under the conditions of 110°C, 2 h, 1 MPa O 2 , and N,N -dimethylformamide. Experimental results indicate that the introduction of NiO can effectively regulate the crystal structure of MnO 2 , forming an amorphous Mn─O─Ni interface, which significantly increases the specific surface area (SSA) of the catalyst while reducing the binding energy of surface lattice oxygen (O L ), promoting the generation of oxygen vacancies (O V ), and thereby enhancing the adsorption and activation capabilities of O 2 . Combined adsorption experiments and kinetic analysis revealed that Ni species preferentially anchor the hydroxymethyl group in HMF molecules, enhancing reaction selectivity. Further experiments demonstrated that the Mn 6.6 NiO x catalyst, under certain conditions, could achieve an HMF conversion rate of 87.52% and a DFF selectivity of 85.81% even at a high substrate concentration of 10 wt% HMF.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiahui Liu,Hongchen Liu,Fan Yang,Junpu An,Siyuan Sun,Yang Sun,Kexin Wei,Xinyang Sun,Junwei Yuan,Meitong Zhao,Haojia Zhong,Kuobo Wang,Jintian Ren,Zhenxing Li,Yongfen Li
The electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) represents a promising pathway to synthesize the critical polymer monomer 2,5-furandicarboxylic acid (FDCA). However, the restricted adsorption of both HMF and OH − to the catalyst surface results in low activity and selectivity. To address this issue, this study introduced an electrochemically assisted strategy to synthesize Ni aerogel with Cu heteroatom doping (Ni 0.94 Cu 0.06 /NF), demonstrating excellent performance for HMF to FDCA conversion in alkaline media. The catalyst achieves 10 mA cm −2 at 1.307 V vs. RHE, with outstanding Hydrogen evolution reaction (HER) activity (10 mA cm −2 @11 mV). Notably, the conversion rate of HMF, the selectivity of FDCA and the Faraday efficiency can reach 99.5 %, 99 % and 97 %, respectively. Scanning Electron Microscope (SEM) and transmission electron microscopy (TEM) demonstrated that the aerogel's self-supported 3D framework with interwoven nanowire structure enables efficient exposure of catalytic sites. X-ray photoelectron spectroscopy (XPS) analysis further showed the modification with Cu forms unique Ni O Cu linkage within the catalyst's surface region, which effectively adjusts the electronic configuration of Ni sites and increases lattice oxygen content, thereby enhancing HMF adsorption. Density functional theory (DFT) revealed that the synergistic interplay between Ni and Cu markedly boosts the uptake capacity for both HMF and OH − , improves the rate-determining step (RDS) thermodynamics by reducing its barrier, and consequently accelerates the HMF oxidation reaction (HMFOR). Our findings elucidate fresh perspectives into the structure-performance relationship of nickel-based catalysts and offer a novel approach for designing advanced electrocatalysts for biomass upgrading.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Weizhen Xie,Yue Tang,Jiacheng Li,Yaqi Shi,Shigang Su,Yong Sun,Lu Lin,Xing Tang
The aqueous-phase hydrogenation of concentrated 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) is a crucial transformation for sustainable chemical production. However, this process is often limited by sluggish H 2 activation at low temperatures and poor selectivity arising from over-hydrogenation. Here, we develop a Pt catalyst supported on oxygen-deficient manganese oxide (Pt/MnO x –O v ), featuring finely dispersed Pt/PtO 2 domains in conjunction with abundant Pt–O–Mn interfacial ensembles. Under mild aqueous conditions (30–60 °C), the catalyst efficiently converts HMF at concentrations up to 40 wt%, delivering a BHMF yield of 90.9 %. In addition, continuous-flow operation at 30 °C sustains BHMF yields above 90 % over a cumulative operation time of 80 h, thereby demonstrating promising potential for industrial application. Mechanistic studies suggest that hydrogen is initially activated on Pt nanoparticles and subsequently undergoes in situ spillover, migrating across the Pt/PtO 2 heterostructure toward adjacent Pt–O–Mn interfacial sites. At these interfacial regions, the asymmetric electronic distribution, induced by nearby oxygen vacancies, facilitates the formation of polarized H δ+ –H δ- species. These reactive hydrogen species, together with the preferential adsorption of the carbonyl group, enable selective hydrogenation while suppressing undesired side reactions. This study demonstrates that tailoring interfacial structures is an effective strategy for improving catalytic performance in biomass upgrading.
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