ACS Catalysis
·
2024
·
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
·
化学工程
·
催化
·
电化学
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED POWDER TECHNOLOGY
·
2020
·
IF 4.217
Yekun Zhu,Yun Zhang,Lili Cheng,Mohammed Ismael,Zhiyuan Feng,Ying Wu
The g-C 3 N 4 /NaNbO 3 photocatalyst was synthesized by simply calcining the mixture of NaNbO 3 and melamine. The synthesized composite exhibits high photocatalytic performance in the selective oxidation of 5-Hydroxymethylfurfural (HMF) to 5-formyl-2-furancarboxylic acid (FFCA) when using water as solvent. The structure and composition of g-C 3 N 4 /NaNbO 3 photocatalysts were characterized by TG, XRD, SEM, UV–Vis, FT-IR, and XPS methods, and the optical and electrochemical properties were investigated by EIS, PC, and PL techniques. O 2 − was inferred to be the primary active species in this process based on the active species trapping experiment. Heterostructure formation of g-C 3 N 4 /NaNbO 3 composites efficiently promoted the separation of photo-generated electron-hole pairs and accelerated the electron transfer rate, thus reduced the formation of OH, and sequentially improved the selectivity of FFCA. The highest HMF conversion of 35.8% with FFCA selectivity of 87.4% was achieved on C/N-59.6 photocatalyst under the irradiation of visible light. The possible mechanism and reaction route were also proposed.
研究领域:
化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Physics
·
2023
·
IF 11.5
Zhenfei Yang,Xinnian Xia,Ming Fang,Longlu wang,Shuaijun Pan,Yang guo
Efficient spatial separation of photogenerated carriers is the key to achieving photocatalytic oxidation reduction synergistic reactions, and the built-in electric field generated by piezoelectric effects can provide a strong driving force for charge separation. A novel Pt/ZnIn 2 S 4 /BaTiO 3 (PBZIS) piezo-photocatalyst with spatial charge separation was successfully constructed through two-step hydrothermal and photodeposition methods. Due to the special 1D/2D core/shell structure, the inner BaTiO 3 can served as hole-storage layer, while the outer Pt nanoparticles can acted as electron capture center, thus greatly improving the separation of photo generated charge carriers and achieving spatial separation of redox sites. Under the ultrasound, the polarized electric field induced by the piezoelectric effect can further improve the extraction rate of photo generated holes by BaTiO 3 and accelerate surface catalytic reactions . Therefore, the synergism of electron/hole co-extraction and piezoelectric effect construct a directional transmission channel and target active sites for photogenerated electron-holes over PBZIS heterojunctions , reuslting in the highest performance for photocatalytic cooperative H 2 evolution (1335.3 μmol g −1 h −1 ) and HMF oxidation (1070.8 μmol g −1 h −1 ). This work would inspire the development of high-performance piezo-photocatalysts for the cooperative biomass oxidation coupling with high efficient hydrogen evolution .
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2013
·Vol. 4
·期 1
·59-66
·
IF 0
Li Hu,Zhang Qiuyun,Liu Jian,Liu Xiaofang,Chang Fei,Liu Yancai,Xue Wei,Yang Song
ZrMo mixed oxides modified by a series of low-cost monofunctional carboxylic acids including stearic acid, palmitic acid, myristic acid, and lauric acid were prepared and were characterized using TG analysis, XRD, FT-IR, NH 3 -TPD, and SEM techniques. These strong solid acids were evaluated as heterogeneous catalysts with porous property for the conversion of carbohydrates to 5-hydroxymethylfurfural (HMF) by oil heating rather than using microwave heating, in the aim of facilitating the industrial feasibility of this catalytic process and discussing the relation between surface acidity and reactivity in carbohydrates to HMF conversion. Under the optimal reaction conditions, moderate yields of HMF could be achieved from fructose, glucose, sucrose, and cellulose, and the strong solid catalysts can be recycled for seven times with no significant loss of activity.
研究领域:
化学工程
·
催化
·
材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mufan Wang,Shiying Fan,Shaomin Liu,Xinyong Li
5-Hydroxymethylfurfural (HMF) serves as a key platform molecule for producing high-value chemicals via green and efficient photocatalytic oxidation. Transition metal oxides, particularly spinel substances, are promising heterogeneous catalysts due to their ability to promote interfacial electron transfer. However, the impact of interfacial electron transfer in HMF photocatalytic oxidation on spinel catalysts remains largely unexplored. In this study, we engineered Mn 4+ -O V -Co 2+ active sites in cobalt-based spinel by in-situ (MCO 4-δ -1) and post-doping (MCO 4-δ -2) strategies to investigate their impact on photocatalytic HMF oxidation. The microstructure morphology, chemical valence states, and band structure of prepared catalysts were systematically characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and UV–vis diffuse reflectance spectra (DRS) techniques. The results revealed that the post-doping catalyst (MCO 4-δ -2) exhibited a higher density of surface oxygen vacancy (Ov), significantly enhancing charge transfer and HMF photocatalytic conversion activity. Specifically, MCO 4-δ -2 achieved an outstanding HMF oxidation product yield of 356.55 μmol g −1 under visible light over 4 h. Furthermore, density functional theory (DFT) calculations provided mechanistic insights, revealing that the oxygen in the aldehyde group of HMF preferentially occupies surface Ov sites at Mn 4+ -Ov-Co 2+ interfaces, thereby facilitating selective HMF oxidation pathways. This study not only expand the application scope of cobalt-based spinel photocatalysts in biomass valorization but also provides an insight on the effects of doping-induced interfacial electronic effects in photocatalytic oxidation reactions.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2021
·
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
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 45
·21285-21292
·
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
·
化学工程
·
可持续化学
·
生物质转化
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wei-Yao Yang,Meng Wen,Hong-Da Zhang,Ya-Qiao Tian,Shi-Chao Su,Yu Lang,Zhi-Ping Zhao,Le Sang
In this work, ACB 18 -SO 3 H-Cl with dual structure Brønsted sites was prepared via chemical grafting method, and promoted the efficient production of HMF from batch to continuous reactors. The optimal catalyst was obtained by adjusting the acid etching time and the grafting amount of acidic functional groups. Through BET and NH 3 -TPD, it was found that the specific surface area of the 0.3 mm spherical activated carbon support reached 1179 m 2 /g, and the acid concentration of prepared ACB 18 -SO 3 H-Cl catalyst reached 7.86 mmol/g. The fructose conversion of 99.2 % and HMF yield of 96.2 % were achieved in stirred tank reactors (STRs) within 2 h, and 90.6 % HMF yield was obtained in micropacked bed reactors (μPBRs) within 86.4 s. Meanwhile, Py-IR and selective poisoning experiments confirmed that the Brønsted acid site is the catalytic active center, and there is a synergistic catalytic effect between the two structural Brønsted sites. The space–time yield (STY) of HMF in μPBRs can reach 2.96 kg/L/h/g, which is at least one order of magnitude larger than reported values in batch and continuous reactors. Moreover, based on the synergistic strengthening effect of μPBRs and ACB 18 -SO 3 H-Cl, the apparent activation energy for synthesizing HMF in μPBRs is lower than that of STRs.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 10
·3363-3371
·
IF 6.177
Gang Xu,Chenyu Chen,Mengxia Li,Xinyi Ren,Lianggao Hu,Chengrong Wu,Yu Zhuang,Fanan Wang
The electrocatalytic HMF oxidation reaction (HMFOR) is one of the promising technologies for the valorization of biomass derivatives and potential replacements for the energy-consuming oxygen evolution reaction (OER). For the most investigated Ni-based electrode, the in situ reconstruction from Ni(OH)2 to NiOOH is hardly avoidable during the electro-oxidation reaction, which is also a highly indispensable prerequisite towards HMFOR. Herein, we developed an efficient strategy of sacrificing W to investigate the effect of surface defects on the self-reconstruction of Ni for promoting HMFOR. It was rationalized that the selective and rapid exsolution of the W species from the as-prepared NiW layer created a porous structure and induced lattice defects on the surface, which facilitated the ion and electron transportation, and further promoted the in situ reconstruction for the formation of higher oxidated Ni with superior activity for HMFOR. This work offers a novel and low-cost means to enrich the active sites for the electrocatalytic upgrading of HMF and other bio-derived platforms.
研究领域:
化学工程
·
电催化
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2024
·Vol. 99
·期 4
·978-988
·
IF 2.8
Likai Dai,Zheng Fang,Anxian Peng,Yunhong Chen,Yitong Liu,Huimei Chen,Rongjun Yan,Rencheng Zhou,Mingming Du
BACKGROUND Photothermal catalytic oxidation technology for synthesis of high value-added chemicals has become a hot topic of research at home and abroad. As a special structure, titania (TiO 2 ) nanotubes (Ti-NTs) possess larger specific surface area and adsorption capacity, which have shown great application prospects in photothermal catalytic oxidation. RESULTS In this work, high-performance palladium (Pd-Ti-NTs catalyst were prepared and applied to the photothermal catalytic oxidation of 5-hydroxymethyl (HMF) and benzyl alcohol. The photothermal dependence on catalytic activity and selectivity of HMF and benzyl alcohol oxidation was studied in detail. The results revealed that compared with thermal catalytic oxidation, the catalysts showed significantly higher conversions of both benzyl alcohol and HMF under light. in particular, HMF conversion increase from 55.6% to 99.7%. Aldehyde oxidation is inhibited by alcohol and can be dramatically promoted by light radiation. This is probably because alcohol can inhibit the adsorption of aldehyde, and this inhibiting effect is weakened through light radiation, thus promoting the oxidation of aldehydes. Therefore, the selectivity of the final products 2,5-furandicarboxylic acid (FDCA) and benzoic acid were dramatically increased in both systems under light radiation, and the selectivity for FDCA was obviously increased from 5.8% to 61.3%, and the yield reached 61.0%, which is higher than that of most of the reported Pd-TiO 2 -based catalysts for FDCA. CONCLUSIONS In this paper, we verify that Pd-Ti-NTs could preferentially promote the conversion of aldehydes to acids in the presence of light, and obtained catalysts with high catalytic performance and high stability for benzyl alcohol and HMF oxidation. © 2024 Society of Chemical Industry (SCI).
研究领域:
催化
·
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zongxi Zhang,Xiaoying Guo,Hui Cao,Jiancheng Zhao,Yingxiong Wang,Shuai Chen,Yan Qiao
The key issue in electricity-drive 5-Hydroxymethylfurfural oxidation reaction (HMFOR) is to accelerate the electrochemical protons deintercalation process of catalyst for reducing the reaction potential and improving the reaction activity. Herein, we developed a novel ionic liquid (IL) modification strategy to construct 1-butyl-3-methylimidazolium trifluoroacetate modified Co 2 Ni( OH ) x ([BMIm][TFA]-Co 2 Ni( OH ) x /NF) catalyst. The introduction of IL provides assistance in the morphological structural and electronic configuration modulation, thereby enhancing mass transfer efficiency and the generation of high-valent active species (TFA-M 2+ -OH ⇌ TFA-M 3+ -O). Benefit from the above favorable regulatory strategies, the resulting [BMIm][TFA]-Co 2 Ni( OH ) x /NF exhibits remarkable low onset potential (1.13 V vs. RHE), high current density (97 mA/cm 2 at 1.40 V vs. RHE), and excellent FDCA yield (98%) with high Faradaic efficiency (98%) across a wide potential range (1.44–1.50 V vs. RHE). In addition, the experimental results reveal that IL modification strategy impedes overcover of *OH and hereby effectively suppressed OER process, thus maintaining excellent HMFOR reactivity over a wide voltage range. This route provides a novel and green ligand modification scheme for enhancing the synergistic effect of Ni/Co sites in CoNi hydroxides and rapidly formation of active species for HMFOR.
研究领域:
电化学
·
催化
·
材料科学
·
绿色化学
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 36
·29692-29702
·
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
·
纳米技术
·
酶工程
·
绿色化学
·
可持续生物制造
·
生物基材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）