CATALYSIS TODAY
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2024
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IF 5.2
Yang Gao,Shilin Fan,Bin Zhu,Soliman I. El-Hout,Jinghui Lyu,Jian Zhang,Chunlin Chen
Biomass energy has gained significant attention due to its renewability and clean, low-carbon characteristics. We prepared a Co@NC-a catalyst using the complexation-carbonation-acid etching method, which can catalyze both thermochemical and electrochemical HMF selective oxidation reactions. In thermocatalysis, it can achieve 100 % HMF conversion and 94.4 % FDCA yield at 65 °C and 0.2 MPa O 2 . In electrocatalysis , 100 % HMF conversion and 73 % FDCA yield were also realized. Significantly, graphitized carbon contributes to the aerobic oxidation of HMF due to its excellent electrical conductivity , which promotes electron transfer during the reaction. Additionally, a comparative study of the activation energy of this catalytic system in electrocatalysis and thermocatalysis showed that electrocatalysis is kinetically more favorable. The energy efficiency calculation also indicates electrocatalysis is more energy efficient than thermocatalysis.
研究领域:
生物质能
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催化化学
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材料科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xinkang Peng,Xulong Song,Wei Cao,Zhenchen Tang,Tingting Wang,Yunxia Wen,Zhinan Wu,Tong Zhou,Han Lin,Xiaohua Lu,Tuo Ji,Jiahua Zhu
2,5-Furandicarboxylic acid (FDCA), an important platform chemical, is often synthesized from hydroxymethylfurfural (HMF), while the energy efficiency of the reaction is limited by the slow hydroxymethyl oxidation, resulting in poor technoeconomy. In this study, a bimetallic Au–Pd microwave-responsive catalyst was designed to achieve high-efficiency synthesis of FDCA by coupling microwave-activated peroxyl radical formation from hydrogen peroxide (H2O2). Pd sites were responsible for dissociating H2O2 into peroxyl radicals (·OOH), and Au sites accepted peroxyl radicals and oxidized HMF into FDCA. The microwave-boosted reaction synergy on the bimetallic Au–Pd dual active centers enabled the reaction to occur at near-room temperature (45 °C) and reached the highest FDCA yield of 88 mol % at 65 °C. Experimental and electric-field DFT studies revealed that microwaves increased the rate constant of H2O2 decomposition by 1.6-fold compared to conventional heating methods, with an ultrahigh H2O2 utilization rate of 90%. This work provides a new platform for highly efficient peroxyl radical formation with microwave energy, which can be extended to a wider range of oxidation reactions with accelerated reaction kinetics and enhanced energy efficiency.
研究领域:
催化化学
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绿色化学
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能源化学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2024
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IF 11.3
Haohan Wu,Bowen Liu,Yi Qi,Xueqing Qiu,Liheng Chen,Yanlin Qin
The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) provides a viable pathway for the efficient utilization of biomass resources. However, designing and regulating the activity and selectivity of the corresponding electrocatalysts remain significant challenge. Spinel compounds show great potential as catalysts due to their adjustable electronic structures and notable catalytic properties, but their intrinsic low conductivity has limited their further application. Herein, a lignin-based carbon fiber (LCF) embedded CuFe2O4 catalyst (CuFe2O4/LCF) is successfully constructed using an electrospinning technique. The catalyst can efficiently and selectively synthesize 2,5-furandicarboxylic acid (FDCA) at a relatively low potential. The experimental results and theoretical simulations demonstrate that the introduction of lignin can significantly optimize the pregraphitic turbine carbon microstructure of the carbon fibers and facilitate rapid electron transfer between CuFe2O4 and the carbon layer. Furthermore, the ATd–O–BOh interactions on the surface of the CuFe2O4 spinel structure significantly enhance the adsorption capacity for the substrates and OH– species, effectively promoting the catalytic reaction. The findings hope to provide a unique perspective to improve the catalytic activity of lignin carbon fiber spinel catalysts and the stability of biomass value-added mechanism.
研究领域:
材料科学
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化学工程
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催化
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电化学
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可持续化学
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产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 11
·2645-2652
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IF 5.6
Rulu Huang,Yuan Cheng,Huai Liu,Lincai Peng,Junhua Zhang
It is incredibly challenging to design a catalyst with high activity for catalytic transfer hydrogenation (CTH) of levulinic acid (LvA) into gamma-valerolactone (GVL). In our previous work, we have designed a mesoporous acid-base bifunctional hybrid (Zr-FDCA) with high contents of Lewis acid (LA) and Lewis base (LB) sites from zirconium and 2,5-furandicarboxylic acid (FDCA) by using acetic acid as the modulator, which exhibited an outstanding performance in CTH of furfural into furfuryl alcohol. However, the catalytic performance was not satisfactory in CTH of LvA into GVL. Herein, we modified a Zr-FDCA hybrid with the introduction of phosphotungstic acid (HPWO). Comprehensive characterization revealed that HPWO could significantly affect the acidity, which afforded acid catalytic activity and introduced a Brønsted acid (BA) site. The synergistic effect between LA and BA sites resulted in the outstanding catalytic activity in CTH of LvA into GVL; a GVL yield of 95.4% with a high formation rate of GVL (12.72 mmol g−1 h−1) was obtained over Zr-FDCA-HPWO. Simultaneously, it also showed an ideal cycle stability and could be used for at least five consecutive runs with no significant loss in the catalytic activity.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 45
·21285-21292
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IF 3.591
Tianci Wang,Yu Song,Wanna Zhao,Chunmei Zhou,Yuguang Jin,Xiaoyue Wan,Yihu Dai,Yanhui Yang
The oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is one of the most attractive reactions to establish a sustainable chemical process based on biomass resources. In this work, a CNT-supported ruthenium–manganese oxide nano-catalyst (RuO2/MnO2/CNT) was employed for the electro-catalytic oxidation of HMF in base-free aqueous solution. The activity test showed that α-MnO2 can effectively promote the activity of RuO2 in the oxidation of HMF. In comparison with RuO2/CNT, RuO2/MnO2/CNT possessed a lower activation energy and more than twice the FDCA formation rate. Under the optimized reaction conditions, the RuO2/MnO2/CNT catalyst afforded a FDCA yield of 72.1% in a 0.1 M K2SO4 aqueous solution at a 0.9 V (vs. Ag/AgCl) applied potential. To our knowledge, this is the first demonstration of FDCA formation as the primary product with high yield in an initially neutral electrolyte. The product FDCA can be easily separated after cooling the reaction solution to room temperature.
研究领域:
催化
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化学工程
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可持续化学
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生物质转化
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
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2021
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IF 7.92
Wen Guan,Yunlei Zhang,Yao Chen,Jianchun Wu,Yu Cao,Yanan Wei,Pengwei Huo
Efficient nanoreactors for the catalytic oxidation of the key platform compound HMF to the high value-added chemical FDCA are highly desirable in the field of biomass transformation. Herein, hierarchical porous bowl-like nitrogen-doped carbon supported AuPd bimetallic (AuPd/pBN x C) nanoreactors were synthesized by the following steps: precipitation polymerization, carbonization, SiO 2 sphere removal, and sol curing. By changing the amount of nitrogen doping and removing the template, AuPd/pBN x C nanoreactors with a hierarchical porous structure and adjustable basicity were prepared. The alkaline sites of N x C carriers provided anchoring sites for metals and had a certain adsorption affinity for HMF and its intermediates. Theoretical calculations and adsorption experiments indicated that the doped nitrogen significantly enhanced the combining capacity between the HMF molecule and nanoreactors. The nanoreactor was used for the tandem oxidation of HMF to FDCA in water, and the highest FDCA yield of 97.6% could be obtained under optimum reaction conditions. The reaction process was evaluated by kinetics calculations, and the oxidation of FFCA to FDCA was confirmed as the rate-determining step. The regeneration experiments showed that the AuPd/pBN x C nanoreactors could be recycled and reused at least five times without an obvious loss in catalytic activity.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
RSC Advances
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2025
·Vol. 15
·期 36
·29692-29702
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IF 4.6
Lei Yang,Anbang Duan,Yuan Ding,Xiquan Song,Qianli Ma,Zhanyin Liu,Tingying Wei,Zhixing Wang,Chunzhao Liu
The growing demand for sustainable biomanufacturing has driven significant interest in 2,5-furandicarboxylic acid (FDCA), a bio-based platform chemical for producing renewable polymers. The eco-friendly oxidoreductase laccase exhibits promising FDCA biosynthesis capacity yet is hampered by pH-dependent activity decay and susceptibility to proteolytic degradation. Herein, we developed a bio-enabled synthesis approach to fabricate three-dimensional laccase-integrated copper hybrid nanoflowers (Lac-NFs) through enzyme–metal coordination-driven self-assembly. The engineered Lac-NFs displayed high enzyme encapsulation efficiency (89.28%) and enhanced environmental robustness compared to free laccase. Furthermore, the Lac-NFs maintained prolonged storage stability with well-preserved activity relative to the native enzyme. Elevated catalytic efficiency and refined enzymatic kinetics were achieved via copper-mediated electron transfer networks within the hybrid matrix. Remarkably, Lac-NFs demonstrate exceptional catalytic efficiency and selectivity in the conversion of HMF to FDCA, achieving complete substrate conversion under precisely controlled operational parameters. This nano–biohybrid design establishes a robust and efficient biocatalytic platform for biomass valorization into high-value-added chemicals, exhibiting promising scalability prospects for industrial implementation.
研究领域:
生物催化
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纳米技术
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酶工程
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绿色化学
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可持续生物制造
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生物基材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Tianyu Gao,Yongxuan Yin,Guanghui Zhu,Qiue Cao,Wenhao Fang
Oxidative transformations of HMF are key routes toward a wide variety of chemicals and biofuels through an environmental friendly process. Co 3 O 4 NPs decorated Mn-Co-O solid solution, donated as Co 3 O 4 /Mn X Co, was prepared by co-precipitation method and used as non-precious metal catalyst for base-free oxidation of HMF to FDCA in the presence of O 2 and water. Comprehensive characterizations such as XRD, H 2 -TPR, O 2 -TPD, XPS, NH 3 /CO 2 -TPD and TEM were used to study materials properties especially the oxygen mobility and acidity-basicity. The effect of Mn/Co molar ratio in catalyst and the reaction conditions were investigated and optimized. In addition, the kinetics of the reaction was monitored to reveal the reaction route and rate-determining step. The variation of Mn/Co molar ratio was found to affect not only HMF conversion but also distribution of products. When the Mn/Co ratio was of 0.2, the Co 3 O 4 /Mn 0.2 Co catalyst showed the optimal catalytic performance (i.e., >99% yield of FDCA obtained under 1 bar O 2 at 140 °C after 24 h) due to the highest content of both Lewis and Brønsted acid sites on the surface, leading to the strongest ability of HMF adsorption and COOH group formation, as well as the enhanced oxygen mobility. This catalyst was shown stable after a minor deactivation (≤8%) during six recycling uses and its activity can be entirely regenerated by calcination in air.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Zhiyan Hou,Yufeng Wu,Weijin Cao,Changlong Wang
Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) is a promising carbon-less and sustainable approach to 2,5-furandicarboxylic acid (FDCA) using renewable electricity. However, the performance of this process suffers from low profitability, low efficiency and selectivity if further industrial FDCA electrosynthesis would be applicable. Here we first use techno-economic analysis (TEA) to look at the technological challenges by taking the feeding of the substrates and downstream purification of FDCA into account, and to provide baseline for achievable profitability based on the crucial performance parameters: the faradaic efficiency and current density. Subsequently we designed a NiCu electrocatalyst comprising hetero-structured Cu(OH) 2 and α-Ni(OH) 2 , enabling the rapid transformation of Ni 3 + /Ni 2+ sites for electrooxidation of HMF to FDCA via 5-hydroxymethyl-2-furan-carboxylic acid pathway at ampere-level current density. Moreover, such a NiCu catalyzed electrooxidation HMF-to-FDCA process can be carried out in a continuous fashion with one pass FDCA faradaic efficiency up to 92 % for over 500 h, allowing scale-up for bulk production of FDCA with high profitability ($417.5/ton FDCA ). This work thus showcases the systematic design including the process and highly efficient electrocatalyst for potential industrial FDCA electro-synthesis.
研究领域:
电化学
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催化
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可再生能源
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Wen Guan,Yunlei Zhang,Yanan Wei,Bing Li,Yonghai Feng,Changhao Yan,Pengwei Huo,Yongsheng Yan
As an important renewable alternative to the production of petroleum-derived terephthalic acid, selective aerobic oxidation of biomass derivative 5-hydroxymethylfurfural (HMF) into high value-added 2,5-furandicarboxylic acid (FDCA) is attracting increasing attention. Herein, a novel hierarchical porous nitrogen-doped carbon (NC) supported bimetallic AuPd catalyst was synthesized by Pickering high internal phase emulsions (Pickering HIPEs) templating method, subsequent carbonization and the sol-curing technique. By varying Pickering HIPEs parameter, nitrogen-doped content and the loaded AuPd nanoparticles, Au x Pd y /NC catalysts with adjustable porous structure and basicity were obtained. Benefiting from the synergistic effects of the high basicity of NC support and efficient bimetallic AuPd catalyst, tandem oxidation of HMF to FDCA reactions can be carried out under base-free condition in water, which makes the biomass transformation process environmental friendliness and economic. And the highest yield of FDCA at 96.7% was achieved under the optimal reaction conditions. Regeneration test revealed the obtained Au x Pd y /NC catalyst was recovered and reused at least five times without significant loss of catalytic activity. The present work offers a versatile strategy for developing nitrogen-doped carbon supported highly efficient bimetallic catalysts with hierarchical porous structure and adjusting basicity for a wide range of base-free catalytic oxidation in water.
研究领域:
催化化学
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材料科学
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Chemistry and Pharmacy
·
2024
·
IF 5.5
Zhi-Gang Zhang,Yan Yi,Jia-Chun Lin,Dong Chen,Xiao-Jun Ji
2, 5-furandicarboxylic acid (FDCA) is a versatile bio-based building block that can be used for the synthesis of degradable polymers. Recently, developing green and sustainable catalytic processes for producing FDCA from renewable platform chemical molecules has attracted continuing attention. In this study, we proposed a green and sustainable one-pot, two-step biocatalytic process for the sequential oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to form FDCA with good yield and excellent selectivity. The initial step involves the oxidation of HMF to 2, 5-diformylfuran (DFF) and 5-formyl-2-furancarboxylic acid (FFCA) catalyzed by recombinant E. coli cells expressing a 5-hydroxymethylfurfural oxidase . The second step is to convert DFF and FFCA into FDCA final product via aldehyde oxidation reaction catalyzed by Deinococcus wulumuqiensis R12 whole cells . Combining the two different whole-cell biocatalysts , 180 mM of HMF could be easily converted into FDCA with a yield of 99% under optimized reaction conditions. This study offers an efficient and sustainable approach for the valorization of biomass-based HMF to form value-added FDCA.
研究领域:
生物技术
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化学工程
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Qiang Fang,Lu Hao,Tao Zhao,Jiahui Li,Genyan Hao,Guang Liu,Dazhong Zhong,Jinping Li,Qiang Zhao
The electrocatalytic production of 2,5-furandicarboxylic acid (FDCA) via the 5-hydroxymethylfurfural oxidation reaction (HMFOR) is an effective and more suitable alternative to the oxygen evolution reaction (OER) in electrocatalytic water splitting. High-valence Ni(III) is critical for the HMFOR, but the formation is greatly limited by the difficult in situ self-oxidation. In this study, the pre-oxidization-derived amorphous NiO x H y nanosheet presents more accessible Ni(III) for efficient HMFOR. In addition, NiO x H y /NF exhibits a low onset potential of 1.35 V, a high FDCA yield of 98.5 %, and a high Faradaic efficiency of 98.3 % for the HMFOR in 0.1 M KOH with 10 mM HMF. In situ Raman spectroscopy results indicate that Ni(III)OOH is an active intermediate in the electrochemical HMFOR. This work provides a strategy for promoting the formation of high-valence Ni(III) and boosting biomass oxidation.
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）