Surfaces and Interfaces
·
2025
·
IF 6.3
Yuefeng Jiang,Xiaofei Li,Ruijie Li,Lili Geng,Yongming Zeng,Ley Boon Sim,Binghui Chen
Electrooxidation of 5-hydroxymethylfurfural (HMF) has long been recognized to efficiently produce the bioplastic precursor, 2,5-furandicarboxylic acid (FDCA). Introducing composite components to construct multiphase interfaces has high potential in modulating the electronic structure of catalysts. Therefore, we synthesized Ni 3 S 2 -CeO 2 /NF using a three-dimensional porous foam nickel scaffold, in-situ grown Ni 3 S 2 /NF via hydrothermal sulfidation, and further incorporated CeO 2 . Characterization with XRD, HRTEM, and SAED confirms the phases of Ni 3 S 2 and CeO 2 and their heterojunctions. XPS analysis shows that CeO 2 increases the Ni 3+ /Ni 2+ ratio; in situ Raman spectroscopy confirms that NiOOH (Ni 3+ ) regenerated from Ni 3 S 2 /Ni(OH) 2 (Ni 2+ ) is the active material for HMF oxidation, complementarily demonstrating that CeO 2 facilitates NiOOH production and that the oxidation process follows an indirect mechanism. Electrochemical analysis shows that at 1.504 V (vs. RHE), Ni 3 S 2 -CeO 2 /NF achieves 99.5% conversion (vs. 83.1%) of 30 mL of 10 mM HMF within 120 minutes, with 99.4% (vs. 89.2%) FDCA selectivity at 97.1% (vs. 78.4%) Faraday efficiency, along with excellent stability, compared to Ni 3 S 2 /NF. DFT calculations indicate that the synergistic effect of CeO 2 enhances HMF adsorption on NiOOH and significantly reduces the activation energies of all associated elementary reactions. This study provides thorough analysis into how Ni 3 S 2 -CeO 2 /NF has enhanced HMF oxidation capabilities.
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Zehua Liu,Caiyi Liu,Shenghe Si,Ying-Ao Liu,Xuhui Shao,Dong Liu
Photoelectrochemical (PEC) oxidation provides a promising strategy to convert solar energy into high-value-added products. The oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is of particular interest, but efficient PEC conversion remains challenging due to the limitations of selectivity, stability, and energy conversion efficiency. Although n-type silicon offers the highest theoretical photocurrent, its practical application is hindered by insufficient photovoltage and sluggish interfacial catalysis. Here, we report a NiO x /Ga 2 O 3 /n-Si photoanode integrated with a Ni(OH) 2 cocatalyst for efficient HMF oxidation. The ultrathin Ga 2 O 3 interlayer facilitates the built-in electric field, thus leading to enhanced photovoltage and enabling superior HMF oxidation performance. When coupled with a commercial Pt/C cathode, the system achieves stable, bias-free FDCA production under simulated solar illumination. This work highlights the potential of engineered silicon photoanodes for sustainable light-driven biomass valorization.
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产品关联
DOI
高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
·
2019
·
IF 3.553
Li-Quan Ren,Tian-Tian Chang,Da-Peng Ren,Ying Zhou,Bang-Ce Ye
Acinetobacter sp. strain LMB-5 can produce a kind of esterase degrading phthalate esters. However, low activity of Est3563 esterase limited its large-scale application. In this study, computer-aided simulation mutagenesis was used to improve the esterase activity with a tightened screening library and enlarged success rate. Two positive mutants, P218R and A242R, were obtained with 2.5 and 2.1 folds higher than the WT Est3563 esterase, with 11.96 ± 0.45 U·mg −1 and 9.90 ± 0.52 U·mg −1 , respectively. With the help of bioinformatics analysis and three-dimensional printing technology, it was found that the mutations could increase the 240–280 residues swing distance and make them deviate from the catalytic pocket. The instability and deviation of these residues on the lid-like structure of the esterase could deteriorate the seal of the binding pocket and expose the active site. Thus, the catalytic efficiency of the mutants became higher. This result demonstrates that the instability and deviation of the lid-like structure could expand the binding pocket of the esterase and enhance the esterase activity.
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DOI
PubMed
高影响因子
ACS Catalysis
·
2018
·
IF 11.384
Yuchao Chai,Sihang Liu,Zhi-Jian Zhao,Jinlong Gong,Weili Dai,Guangjun Wu,Naijia Guan,Landong Li
Metal nanoparticles encapsulated in zeolite have been recently developed as a special type of catalyst that shows significant advantages in activity, shape-selectivity, and stability over conventional supported catalysts. The selectivity modulation of encapsulated nanoparticle catalysis by the zeolite microenvironment is theoretically possible but not addressed yet. Here, we report the in situ encapsulation of sub-nanometric palladium species within MFI-type zeolites, which exhibit high activity and good stability in the hydroconversion of furfural as a model reaction of biomass upgrading. Remarkably, different products, e.g., furan, furfural alcohol, and 1,5-pentanediol, from furfural hydroconversion can be obtained when silicalite-1, Na-ZSM-5, and H-ZSM-5 are employed as hosts of palladium nanoparticles, respectively. Density functional theory calculations and spectroscopy investigations reveal that both the adsorption of furfural and the activation of hydrogen are significantly affected by the zeolite microenvironment, leading to different reaction pathways. Our work presents an elegant example of catalytic selectivity modulation of encapsulated metal nanoparticles by tuning the zeolite microenvironment.
研究领域:
催化
·
材料科学
·
化学工程
·
纳米技术
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DOI
高影响因子
ANALYST
·
2021
·Vol. 146
·期 8
·2506-2519
·
IF 4.616
Yue-Ming Yu,Yuan-Yuan Niu,Ling-Yang Wang,Yan-Tuan Li,Zhi-Yong Wu,Cui-Wei Yan
For highlighting the predominance of phenolic acid nutraceutical ferulic acid (FR) in regulating the in vivo/vitro performances of anticancer drug 5-fluorouracil (Flu) and strengthening their cooperativity in antitumor effect, thus achieving a major breakthrough in the development of drug-nutraceutical cocrystal with synergistic antitumor action, a cocrystallization strategy of dual optimization is created, in which both the in vivo and vitro natures of Flu are improved by exploiting the FR's excellent physicochemical property. Moreover, Flu's anticancer effects were promoted by exerting the assistant antitumor peculiarity of FR. Such dual optimization of FR for Flu in physicochemical properties and anticancer activities is beneficial for realizing synergistic augmentation effect by taking the benefit of the cooperativeness of Flu and FR in the anticancer ability. Based on this idea, a novel cocrystal of Flu and FR, namely, Flu-FR-H2O, is successfully assembled as the first 5-fluorouracil-nutraceutical cocrystal with synergistic antitumor effect and its explicit structure is resolved. The single-crystal X-ray diffraction demonstrates that Flu and FR have a ratio of 1 : 1 with one equivalent of solvent water in the cocrystal, where one-dimensional hydrogen-bonding helices and FR-Flu hydrogen-bonding pairs, together construct a three-dimensional supramolecular network. By combining experimental evaluation with theoretical analysis, in vitro/vivo pharmaceutical properties are scientifically investigated. Results show that the permeability and aqueous solubility of Flu are respectively elevated by 5.08 and 1.64 folds, which has brought about ameliorated pharmacokinetics, thus providing prolonged retention time and increased oral bioavailability. More interestingly, the cocrystal shows synergistic inhibition ability of Flu and FR against tested tumor cell strains, hence laying the groundwork for reducing the dosage and even the toxic side effects of Flu. As a result of this, the present research not only provides a new strategy for Flu to optimize its physicochemical properties and antitumor activities simultaneously but also offers some opinions for the development of synergistic antitumor pharmaceutical cocrystals.
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DOI
PubMed
高影响因子
FUEL
·
2012
·
IF 3.248
Tao He,Yuxin Wang,Pengjie Miao,Jianqing Li,Jinhu Wu,Yunming Fang
Deep hydrogenation of aromatics is an important reaction in modern oil refinery. The key of an aromatic hydrogenation unit is high active, sulfur resistant hydrogenation catalyst. In this paper, the catalytic performance of a newly developed hydrogenation catalyst, platinum supported on mesoporous ZSM-5 (Pt/MZ-5), was tested in naphthalene (model compound of light cycle oil) hydrogenation. Pt/ZSM-5 and Pt/Alumina were used as reference. In some experiments, dibenzothiophene (DBT) was added to test the sulfur tolerance of catalysts. In the absence of DBT, Pt/MZ-5 and Pt/Alumina showed much higher hydrogenation activities and decalin selectivity than Pt/ZSM-5. The selectivity to decalin exceeds 97% over Pt/MZ-5 at temperature range between 523 and 573 K. Furthermore, Pt/MZ-5 shows better sulfur resistance than that of Pt/Alumina. In the presence of 3000 ppm dibenzothiophene, the selectivity of decalin over Pt/MZ-5 was only slightly dropped to 89.4% at 573 K, which is much higher than that of Pt/Al 2 O 3 (51.4%). The excellent catalytic performance and sulfur tolerance of Pt/MZ-5 were attributed to the combination of high acidity and mesoporous structure in MZ-5.
研究领域:
催化化学
·
石油炼制工程
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DOI
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 8
·期 17
·4338-4348
·
IF 5.365
Xiaoli Yang,Xiong Su,Binglian Liang,Yaru Zhang,Hongmin Duan,Junguo Ma,Yanqiang Huang,Tao Zhang
The oxide–zeolite process has been attracting widespread attention due to its promising performance in syngas conversion to hydrocarbons with high selectivity and stability. Here, a composite catalyst containing Zn–Cr oxide and ZSM-5 zeolite provides a competitive option in the one-step conversion of syngas into C5+ hydrocarbons. In order to figure out the influence of the pore structure and acidity of zeolite on the oxide–zeolite process, alkali treatments on ZSM-5 are carried out. The treated ZSM-5 shows increased selectivity for gasoline fractions. With a set of structural and morphological characterization techniques, the formation of a hierarchical porous structure is demonstrated, which is favorable for the diffusion of heavy products. Furthermore, an increase in the number of Lewis acid sites, acting as the main active sites for the polymerization, cyclization and aromatization reactions, also contributes to the promotion of C5+ hydrocarbon production. It must be noted, however, that a certain amount of Brønsted acid sites is necessary for the tandem transformation of CH3OCH3 intermediates, which may further affect the CO conversion.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
NUCLEAR MEDICINE AND BIOLOGY
·
2024
·
IF 3.6
Yuli Sun,Guangwen Li,Haiyan Hong,Lin Zhu,Hank F. Kung,Yan Zhang,Jinxia Zhu
Objective Diabetes mellitus (DM) is one of the major diseases in the world. Nuclear medicine imaging may be able to detect functional status of pancreatic β cells in vivo , which might elucidate the pathological mechanisms of diabetes and develop individualized treatment plans. In this study, we evaluated the ability of [ 125 I]ADAM, a serotonin transporter (SERT) imaging agent, as a probe for detecting pancreatic β-cell mass (BCM). Methods In vitro cell studies were evaluated in INS-1 cells (rat islet β cell line). Biodistribution studies were performed in male normal Sprague-Dawley rats and alloxan-induced type 1 diabetes mellitus (T1DM) rats. Distribution and expression of SERT protein in pancreas of rats were also measured by immunofluorescence staining and Western blot. Results In vitro cell studies showed that the concentration of [ 125 I]ADAM associated with the INS-1 cells was increased gradually with incubation time, and the SERT specific inhibitor, escitalopram, exhibited the inhibitory effect on this interaction. Biodistribution studies also showed that the uptake of [ 125 I]ADAM in the pancreas of normal rats was decreased in the presence of escitalopram. However, in the T1DM rat model with a significant β cells reduction, the uptake of pancreas was increased when compared with the control. Through immunofluorescence staining and Western blot, it was found that both the endocrine and exocrine cells of the normal pancreas expressed SERT protein, and the level of SERT protein in the exocrine cells was higher than islets. In the diabetic state, the expression of SERT in the exocrine cells was further increased. Conclusions The SERT imaging agent, [ 125 I]ADAM, at the present form will not be suitable for imaging β cells, specifically because there were extraordinarily high non-specific signals contributing from the exocrine cells of pancreas. In addition, we noticed that the level of SERT expression was abnormally elevated in the diabetic state, which might provide an unexpected target for studying the pathological mechanisms of diabetes.
研究领域:
医学影像学
·
内分泌学
·
糖尿病研究
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Zhe Hong,Lihua Deng,Fanglin Wang,Fangyu Zhu,Yingsen Fang,Li Song,Lei Li,Zhirong Zhu
ZSM-5 zeolites with accessible micropore architecture and tunable acid–base sites are important shape-selective catalysts. However, the presence of exposed straight channels and the external acid–base sites of conventional ZSM-5 has a negative impact on shape selectivity. Herein, we report on the direct synthesis of an intergrowth ZSM-5 zeolite mimicking the mortise–tenon joints. It can be revealed by various methods that the mortise–tenon ZSM-5 shows an inverse Al gradient from the surface to the core of the zeolite. More importantly, the sinusoidal channels predominantly opened to their external surfaces are constructed. The shape-selective capability of the ZSM-5 zeolite has been fully exploited due to the intrinsic inert external surface and unique sinusoidal channel features, thereby resulting in high styrene selectivity (>90%) and good catalytic stability (>100 h) in the toluene side-chain alkylation reaction. In addition, in situ DRIFTS confirms that this intergrowth ZSM-5 contributes to the formation of more active intermediates of HCOO* and H3CO*, which is another reason responsible for the superior performance.
研究领域:
材料科学
·
催化化学
·
无机合成
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2018
·
IF 3.849
Shuangshuang Jing,Xuefei Cao,Linxin Zhong,Xinwen Peng,Runcang Sun,Jinchao Liu
Efficient valorization of cellulose is a sustainable route yet a challenging topic to solve the crisis of fossil resources. Although heterogeneous catalysts such as metal oxides have various advantages, the low surface contact area between metal oxides and cellulose is unfavourable for the hydrolysis of cellulose and thus restricts the application of metal oxides in direct conversion of cellulose to 5-hydroxymethylfurfural (HMF). This work presented the utilization of in-situ carbonic acid from CO 2 as a green acid to enhance the conversion of cellulose to HMF in the presence of ZrO 2 and TiO 2 . Combination of in-situ carbonic acid, ZrO 2 and TiO 2 exhibited a distinctive catalysis on the hydrolysis of cellulose and monosaccharide , isomerization of glucose and monosaccharide conversion in tetrahydrofuran (THF)/H 2 O/NaCl system. Especially, in-situ carbonic acid played a significant role in cellulose degradation and accelerated transforming insoluble polysaccharide into soluble oligosaccharide or monosaccharide, and thus promoted the cellulose conversion catalyzed by metal oxides. A high yield of HMF from cellulose (48.4%) was achieved by physically mixing commercial TiO 2 , ZrO 2 , and CO 2 . Due to the significant effects on cellulose degradation and HMF selectivity improvement, in-situ carbonic acid offers a green, low-cost and environmentally friendly co-catalyst for highly effective converting cellulose into HMF.
研究领域:
化学工程
·
可再生能源
·
催化科学
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DOI
高影响因子
Journal of Materiomics
·
2023
·
IF 9.4
Chongsheng Wu,Kui Liu,Honglan Lai,Fang Xu
Herein, the sintering behavior and dielectric properties of Ta 5+ -doped Li 3 Mg 4 NbO 8 ceramics were investigated by solid-phase reactions in combination with first-principles calculations. In particular, Li 3 Mg 4 Nb 0.96 Ta 0.04 O 8 illustrates the best dielectric properties after sintering at 1,175 °C with ε r = 13.71 ± 0.20, Q × f = (132,112 ± 2,391) GHz (increased by 25%) and τ f = (25.07 ± 1.36) × 10 −6 °C −1 . The non-intrinsic factors reflect that a small amount of Ta 5+ doping produces a secondary phase, increased densification, and grain size, all of which optimize the dielectric properties. The dominant intrinsic factors indicate that the increase in bond ionicity, the greater polarization of Ta 5+ , and the blueshift of the Raman characteristic peak all lead to an increase in ε r . The increase in lattice energy and the decrease in the damping behavior of the Nb/Ta-O bond vibrations lead to an increase in Q × f . The weakening of the Nb/TaO 6 octahedral distortion leads to an optimization of τ f . The modified Li 3 Mg 4 Nb 0.96 Ta 0.04 O 8 ceramics have promising applications in microwave communications.
研究领域:
材料科学
·
陶瓷
·
介电材料
·
微波工程
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DOI
高影响因子
Molbank
·
2015
·Vol. 2015
·期 4
·M871
·
IF 0
Shuitao Yu,Xiaohu Feng,Weiyou Zhou,Zhengjun Xia,Mingguang Zhang,Yang Chen,Zaixin Chen
A new tetrahalogenated benzoic acid 4-chloro-2,3,5-trifluorobenzoic acid was synthesized from methyl 2,3,4,5-tetrafluorobenzoate via three steps. The structure of the newly synthesized compound was established by FTIR, NMR, MS and elemental analysis.Keywords:4-chloro-2,3,5-trifluorobenzoic acid;synthesis;amination;Sandmeyer reaction
研究领域:
有机化学
·
药物化学
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DOI
危险品化学品经营许可证（带存储）