LANGMUIR
·
2024
·
IF 3.7
Yongzhi Xiong,Jianchun Jiang,Yajun Liu,Xialin Ji,Changzhou Chen,Kui Wang
The electrooxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) demonstrated its unique superiority, not only in reducing overpotential and improving energy conversion efficiency for green hydrogen production but also in utilizing abundant biomass resources and producing high-value-added chemicals. However, designing highly efficient electrocatalysts for HMF electrooxidation (HMF-EOR) with low cost and high performance for large-scale production remained a huge challenge. Herein, we introduced an easy one-step activation process to produce P-doped porous biochar loaded with multiple crystal surfaces exposed to CoP2O6 catalysts (CoP2O6@PC), which exhibited outstanding electrooxidation performance. To achieve a current density of 50 mA cm–2, only a low overpotential of 200 mV was needed for the electrooxidation of HMF in 1.0 M KOH + 10 mM HMF. This performance far surpassed that of other similar materials. CoP2O6@PC exhibited outstanding HMF-EOR performance with high conversion (nearly 100%), selectivity (97.1%), faradaic efficiency (95.3%), and robust stability. This work represents a promising strategy to fabricate macroscale and low-cost HMF-EOR electrocatalysts and achieve potential industrial applications of HMF-EOR.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xuan Gao,Zhihui Li,Shuxing Zhang,Dongsheng Zhang,Xinqiang Zhao,Baoquan Zhang,Yanji Wang
Developing cost-effective and inherently safe methods for accelerating the sustainable production of value-added chemicals from biomass presents a promising solution to the current energy crisis. This study introduces heterogeneous copper species anchored on a γ-Al 2 O 3 catalyst (Cu/γ-Al 2 O 3 ) with high dispersibility and small Cu particle size, synthesized via a straightforward incipient-wetness impregnation method. This method facilitates the selective anaerobic dehydrogenation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) in the absence of any oxidant or hydrogen acceptor. An HMF conversion of 69.8 % and a DFF yield of 44.9 % were attained at 130 °C over a 12-h period. Extensive characterizations were conducted to elucidate the correlation between the catalyst’s structure and its dehydrogenation activity. The findings indicated that strong L-acid sites, elevated Cu dispersions, small Cu particle size and an increased number of Cu + active sites were conducive to enhanced dehydrogenation reactivity. The Cu/γ-Al 2 O 3 catalyst demonstrated superior catalytic efficiency and stability. A possible reaction mechanism is suggested, integrating DFT calculations with experimental observations. This research offers valuable insights into the selective conversion of HMF to DFF and encourages further exploration into the dehydrogenation of biomass alcohols into high-value chemicals under oxidant-free conditions.
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ELECTROANALYSIS
·
2012
·Vol. 24
·期 2
·286-292
·
IF 2.872
Chengxiang Ruan,Li Xu,Xiuzhen Wang,Jin Lou,Weimin Gao,Wei Sun
In this paper a molecular wire modified carbon paste electrode (MW-CPE) was firstly prepared by mixing graphite powder with diphenylacetylene (DPA). Then a graphene (GR) and chitosan (CTS) composite film was further modified on the surface of MW-CPE to receive the graphene functionalized electrode (CTS-GR/MW-CPE), which was used for the sensitive electrochemical detection of adenosine-5′-triphosphate (ATP). The CTS-GR/MW-CPE exhibited excellent electrochemical performance and the electrochemical behavior of ATP on the CTS-GR/MW-CPE was carefully studied by cyclic voltammetry with an irreversible oxidation peak appearing at 1.369 V (vs. SCE). The electrochemical parameters such as charge transfer coefficient ( α ) and electrode reaction standard rate constant ( k s ) were calculated with the results of 0.53 and 5.28×10 −6 s −1 , respectively. By using differential pulse voltammetry (DPV) as detection technique, the oxidation peak current showed good linear relationship with ATP concentration in the range from 1.0 nM to 700.0 µM with a detection limit of 0.342 nM (3 σ ). The common coexisting substances, such as uric acid, ascorbic acid and guanosine-5′-triphosphate (GTP), showed no interferences and the modified electrode was successfully applied to injection sample detection.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Tianyun Jing,Shaokang Yang,Tingting Li,Yangyang Wan,Huimin Jia,Yonghai Feng,Yunpeng Zuo,Dewei Rao
Atomic scaling of cobalt-based catalysts is the feasible and sustainable approach for selective oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to produce bio-plastic monomer of 2,5-furandicarboxylic acid (FDCA) under mild conditions. Here, a high-efficiency dual single-atomic Co/Cu supported on nitrogen-doped carbon (a-Co/Cu-NC) is constructed. Leveraging exceptional oxygen activation ability, the Co/Cu dual-atomic-sites can accelerate the HMF oxidation, suppressing by-product formation mediated by reactive oxygen species (ROS) in low-oxygen environments. This leads to enhanced FDCA selectivity with a yield of 98% and a production rate of 298.8 mmol FDCA g metal −1 h −1 under ambient conditions. Comprehensive experiments and density functional theory (DFT) calculations demonstrate that long-range interactions between Co and Cu sites optimize reactant adsorption and lower energy barriers for •O 2 − and HMFCA formation.
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Separations
·
2024
·Vol. 11
·期 2
·39
·
IF 2.5
Zhenhua Sun,Qingxiang Shu,Qikun Zhang,Shaopeng Li,Ganyu Zhu,Chenye Wang,Jianbo Zhang,Huiquan Li,Zhaohui Huang
ZSM-5 zeolite is a kind of high-value-added porous aluminosilicate zeolite. The use of the coal gasification slag utilization process by-product desilication liquid as a silicon raw material to replace the current raw materials such as water glass will help reduce production costs and achieve high-value utilization of solid waste. ZSM-5 zeolites for volatile organic compounds (VOCs) adsorption were prepared by a one-step hydrothermal method using the desilication solution prepared from coal gasification slag as the main silicon source and sodium source. The effects of crystallization reaction time, the crystallization temperature, the Na2O/SiO2molar ratio, and the SiO2/Al2O3molar ratio on the relative crystallinity and the specific surface area of the ZSM-5 zeolite were investigated and optimized. The optical reaction conditions were as follows: a crystallization time of 12 h, a crystallization temperature of 170 °C, a Na2O/SiO2molar ratio of 0.2, and a SiO2/Al2O3molar ratio of 200. The optimal ZSM-5 zeolite synthesized is hexagonal, with regular grains, a relative crystallinity of 101.48%, a specific surface area of 337.48 m2·g−1, and a pore volume of 0.190 cm3·g−1. And the optimal ZSM-5 zeolite was composed of SiO2content of 97.52 wt%, Al2O3content of 1.58 wt%, Na2O content of 0.33 wt%, and SiO2/Al2O3molar ratio of 104.93. Na2O/SiO2molar ratio is 0.0033. The results of static adsorption experiments show that the static adsorption capacities of ZSM-5 zeolite forp-xylene, benzene, toluene, and butyl acetate were 118.85, 69.98, 68.74, and 95.85 mg·g−1, respectively, which can effectively adsorb VOCs. The synthetic process of the ZSM-5 zeolite is a simple preparation process and short in synthesis time. The results of this study not only help to realize the high-value utilization of silicon components in solid waste, but also provide an economical and effective way to synthesize VOCs adsorption materials.
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Reaction Kinetics Mechanisms and Catalysis
·
2025
·
IF 1.7
Yu Peng,Zhang Rui
Solid acid catalysts containing both Brønsted acidic and Lewis acidic sites were hydrothermally prepared in this work to convert glucose into 5-hydroxymethylfurfural (5-HMF). A series of catalysts was synthesized by combining metal salts (CuSO 4 , ZrOCl 2 , Al 2 (SO 4 ) 3 , Co (NO 3 ) 2 ) with 2,4,6-trimethylbenzene-1,3,5-trimethylphosphonic acid (H 6 L) as a ligand in a hydrothermal reaction. Additionally, either 2,2-bipyridyl or 4,4-bipyridyl was added as an auxiliary ligand to adjust the internal structure and enhance the Brønsted acid strength of the catalyst, resulting in solid acid catalysts with varying Lewis acid site content. Catalyst characterization demonstrated that 4,4-bipyridine was more effective in enhancing Brønsted acid strength compared to 2,2-bipyridine. Glucose dehydration was performed to synthesize 5-HMF in a two-phase reaction solvent composed of saturated brine, sec-butanol, and methyl isobutyl ketone (1:1.6:4 ratio) at 463 K. The experiments results indicated that the CoL4 catalyst achieved a conversion yield of 89.1% and exhibited excellent thermal stability. The present study emphasizes the comparison and selection of bipotent acid solid catalysts containing different metal active sites for light use in the dehydration of glucose to 5-HMF.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Ruixue Zhang,Weiyao Yang,Hongda Zhang,Le Sang,Zhiping Zhao
This work presents the efficient, safe, and continuous production of 5-hydroxymethylfurfural (HMF) and levulinic acid (LA) from inulin in micropacked bed reactors (μPBRs) over HND-580. Through optimization reaction conditions, the highly selective production of fructose and LA from aqueous inulin and HMF from an inulin DMSO-water mixed solution can be achieved with respect to other reactor technologies. The highest yields of 89% for fructose, 81% for HMF, and 84% for LA can be obtained within a reaction time of 7.26 min. Polysaccharide inulin is used as the reaction substrate, and the space-time yield (STY) of HMF and LA in μPBRs is at least an order higher than that in conventional batch reactors. Subsequently, an intrinsic kinetic model for inulin conversion is established. The most predicted values show good agreement with the experimental results with a relative error of ±20%.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jiaming Guo,Jing Li,Shanhao Ze,Fei Li,Junchao Wang,Qing Liu,Zhe Hua,Liu Yang,Fei Liu,Baodan Liu
In this study, we introduce a novel perspective that the formation of the atomically ultrathin oxide layer on the surface of liquid alloys is primarily governed by thermodynamic laws and is additionally influenced by the surface tension of the liquid alloys. In this case, we control the competition of Gibbs free energy and surface tension to effectively address the severe segregation problem of Ga 2 O 3 and realize the precise doping of Ga 2 O 3 in the preparation process of two dimensional IGO film through the liquid InGa alloy printing approach. Importantly, the Ga 2 O 3 content in the IGO films can be tailored in the full range and a sub-5 nm ultrathin IGO film transistor is innovatively fabricated. The oxidation law, band gap, Fermi level, field-effect mobility, subthreshold swing, and other properties of IGO films in sub-5 nm scale are systemically investigated in detail. It has been demonstrated that the incorporation of Ga 2 O 3 in the doping process dramatically reduced the device's turn-off current and enhanced its ability to resist ultraviolet interference. This novel doping process opens up a significant opportunity for future developments of atomically ultrathin transparent conducting film.
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Catalysis Science & Technology
·
2025
·
IF 4.2
Peixin Wang,Ruilong Zhang,Ifunanya Rejoice Akaniro,Puranjan Mishra,Reeti Kumar,Jun Zhao
Catalytic dehydration of fructose to 5-hydroxymethylfurfural (HMF) is a key reaction in biomass valorization and sustainable chemistry. The development of solid acid catalysts with high selectivity for HMF remains challenging due to the formation of undesired by-products, such as levulinic acid and formic acid in the reaction. In this study, SrNb2O6 catalysts with various morphologies were prepared by a facile one-step hydrothermal method, triggering synergetic catalysis for selective transformation of fructose to HMF. Among the Nb-based mixed oxides synthesized under varying conditions, including different pH environments and Nb concentrations, SrNb2O6 nanorods (denoted as SNO-NR, with pH = 13 and Sr/Nb ratio of 1:2) demonstrated the highest catalytic performance. Specifically, it achieved a 74.9% HMF yield and a selectivity of 78.5% in DMSO at 120°C for 1 hour. Comprehensive characterization analyses collectively indicated that an optimal acid capacity and a balanced Brønsted/Lewis acid ratio, which facilitate synergistic effects, are critical for achieving a highly selective conversion of fructose to HMF. Furthermore, it is also noteworthy that this SNO-NR catalyst was recyclable and stable for up to six runs with a minor reduction in its activity, confirming its remarkable robustness.
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 8
·1-12
·
IF 2.4
Ma Xueqin,Shen Liuwei,Shi Gaolei,Zhang Xingguang
The selective oxidation of 5-hydroxymethylfurfural (HMF) to value-added products plays an important role in biomass catalytic transformation, which essentially depends upon design of highly efficient and selective catalysts. This study aims to identify contributions of silanols (Si-OH groups) on Ag/USY catalysts to regulating catalytic performances in selective oxidation of HMF to HMFCA (5-hydroxymethyl-2-furancarboxylic acid), by means of aluminium tri-sec-butoxide (AlBO) modification to suppress Si-OH groups of USY and 2,6-di-tert-butylpyridine (2,6-DTBPy) selective poison to shield Brønsted acid sites in the reaction system. The catalysts are characterized by XRD, BET, TEM, XPS and FT-IR to examine the crystal structures, surface areas, porosity, morphology, Ag distribution, chemical states, and surface adsorptive properties. The HMF conversion (44-49.2%) slightly changes with increasing AlBO content, whereas the HMFCA selectivity gradually goes down from 56.2 to around 22.1% and the levulinic acid (LA) selectivity minorly raises from 5.6 to 12.8%. The production of LA originates from enhanced Brönsted acid sites after AlBO modification, and the decline of HMFCA selectivity is principally attributed to the suppression of Si-OH groups that weakens the interaction between HMF reactants and catalysts. This work provides new insights into the role of surface modification in tailoring metal and zeolite-based catalysts for organic conversions. Graphical
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NMR IN BIOMEDICINE
·
2025
·Vol. 38
·期 8
·e70093
·
IF 2.7
Zhongyichen Huang,Qiting Wu,Jing Zhang,Hao Tang,Gang Wu,Yao Zhang,Yi Wang,Dong Liang,Xiaoming Li,Yin Wu
Diabetes mellitus (DM) causes skeletal muscle damage. Energy metabolism alterations in diabetic muscles remain to be elucidated. Chemical exchange saturation transfer (CEST) MRI is increasingly adopted in imaging muscle energy metabolism. This study aimed to investigate energy metabolism alterations in diabetic muscles using CEST MRI. Six adult New Zealand rabbits with alloxan-induced DM were scanned on a 5 T MR imager before and 2, 4, 6, and 8 weeks after the DM model induction, with six normal rabbits as controls. T 2 -weighted imaging, B 1 field mapping, and CEST imaging under four B 1 amplitudes of 0.75, 1.0, 1.25, and 1.5 μT were performed, respectively. Blood glucose level was measured before each MRI experiment. Inverse magnetization transfer ratio analysis was adopted to quantify CEST effects of two energy metabolites of creatine (Cr) and phosphocreatine (PCr), from which their ratio was calculated. B 1 inhomogeneity was corrected using a smoothing spline interpolation algorithm. pH-sensitive CrCEST ratiometric was measured by dividing CrCEST under B 1 of 1.25 μT with that under 0.75 μT. Paired student's t -test and one-way ANOVA were conducted with p < 0.05 considered statistically significant. Blood glucose level measurements confirmed the successfully induced DM model. The controls showed no significant changes in Cr- and PCr-weighted CEST signals throughout the study. In contrast, a significant increase of Cr-weighted CEST signals started in 2 weeks ( p = 0.049) and became more pronounced in Week 6 ( p = 0.045) and Week 8 ( p = 0.002) after the DM model induction, whereas PCr-weighted CEST signals remained constant among multiple time points, leading to significantly reduced PCr/Cr in Week 6 ( p = 0.047) and Week 8 ( p = 0.011). Meanwhile, CrCEST ratio did not show significant alterations ( p > 0.05). The significantly increased Cr-weighted CEST and reduced PCr/Cr with time implied disrupted energy metabolism in diabetic muscles, providing supplementary information for better understanding of DM-related muscle impairments from the metabolic level.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Xin Li,Yue Ma,Xuning Wang,Jianguo Wu,Dong Cao,Daojian Cheng
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd 0 /Pd 2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C 3 N 4 –300 catalyst with a Pd 0 /Pd 2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd 0 and Pd 2+ in Pd/g–C 3 N 4 –300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
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