DALTON TRANSACTIONS
·
2025
·
IF 3.3
Xue-Qing Xu,Shen Yu,Xing-Yu Yue,Zhan Liu,Jia-Min Lyu,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Li-Hua Chen,Bao-Lian Su
Phenol is an important intermediate for high value chemicals. Current phenol production via a three-step cumene process causes severe energy-waste and environmental problems. The conversion of benzene to phenol under mild condition can be achieved by oxidation with Cu-based zeolites. However, conventional microporous zeolite suffers from severe diffusion limitation, especially when bulky molecules are involved, such as benzene. In this work, we used a hierarchically macro-meso-microporous ZSM-5 single crystal (Hier-ZSM-5) as substrate for Cu species (Cu@Hier-ZSM-5). Irregular morphology of opal-like Hier-ZSM-5 exhibits abundant surface Si-OH groups and provides a platform for stabilizing Cu2+ sites. Meanwhile, hierarchical porosity provides significantly improved diffusion ability of bulky molecules. As a result, excellent selective oxidation performance of benzene was obtained with the Cu@Hier-ZSM-5, achieving a conversion of 77% and a phenol selectivity of 73%, which is 1.5 times and 2 times of these obtained with a catalyst based on a microporous ZSM-5, respectively. Species of CuOOH were identified as an important intermediate for benzene oxidation. This hierarchical zeolite system with a synergistic effect of site anchoring and molecular diffusion presents an excellent platform for catalyst design.
研究领域:
催化化学
·
材料科学
·
环境化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science China-Materials
·
2023
·Vol. 67
·期 1
·162-169
·
IF 8.1
Yang Bixia,Zhu Mengyao,Jiang Xingpeng,Shao Wenlei,Wang Zhiqi,Yan Jiawei,Zheng Yanting,Zhuang Zanyong,Yu Yan
The photooxidation of renewable bioderivatives into value-added chemicals is highly significant; however, it typically exhibits low selectivity owing to the challenges in controlling the oxidative species and managing the desirable reaction pathways. In this work, we used the Bi 2 O 2 CO 3 /ZnIn 2 S 4 heterostructure, prepared by a CO 2 -mediated solid–solid phase transition, to catalyze the photooxidation of bioderived 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) with a high selectivity of 98.1% and a yield rate of 882.6 µmol g −1 h −1 . The metal carbonate/oxide heterointerface enables the effective transfer of photoactive electrons and holes, optimizes surface oxygen activation, and facilitates the synergy of ·OOH and holes to selectively convert HMF into DFF. The findings unravel how the tailoring and coupling of the electron–hole pairs and reactive oxygen species on heterostructured materials can promote the usage of renewable feedstocks for sustainable development.
研究领域:
光催化
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环境化学
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材料科学
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绿色化学
·
可再生能源
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2019
·
IF 3.774
Yun-Peng Zhao,Fa-Peng Wu,Qing-Lu Song,Xing Fan,Li-Jun Jin,Rui-Yu Wang,Jing-Pei Cao,Xian-Yong Wei
In this work, a bimetallic catalyst of Pd and Ni supported on HZSM-5 was designed and evaluated in the hydrodeoxygenation of model compounds representing various C–O bonds in lignin. The effects of temperature, holding time, and initial H 2 pressure on the catalytic performance of the Pd–Ni/HZSM-5 catalyst were investigated. The results indicated that the Pd–Ni/HZSM-5 catalyst exhibited superior catalytic activity towards the conversion of the model compounds to alkanes compared to its monometallic counterparts. Direct cleavage of the C–O bond in DPE was achieved under low H 2 pressure, mainly producing benzene and minor amounts of phenol and cyclohexane, while at high H 2 pressure, the reaction pathway was altered towards hydrogenation of the benzene ring , followed by then cleavage of the C–O bond to afford only cyclohexane. Moreover, the Pd–Ni/HZSM-5 catalyst showed high activities when applying other substrates including anisole, veratrole, guaiacol, benzyloxybenzene, phenethyl phenyl ether, and dibenzyl ether.
研究领域:
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Yu-Feng Qi,Kai-Yao Wang,Yan Sun,Jie Wang,Cheng Wang
The utilization of biomass resources is essential for constructing a carbon neutral society. Electrochemical conversion of biomass-derived platform molecule 5-hydroxymethylfurfural (HMF) to 5-furandicarboxylic acid (FDCA) is a highly promising alternative pathway for the production of valuable biobased oxygenated chemicals, which primarily takes advantage of the on-going development of efficient, robust, and inexpensive catalysts. In the present work, a carbon paper-supported nickel-iron layered double hydroxide (LDH) nanosheet array implanted with abundant cationic vacancies (d-NiFe LDH/CP) is employed as a self-standing electrode for oxidation of HMF to FDCA. A 97.35% conversion of HMF and a 96.8% yield of FDCA could be achieved at 1.48 V, with a faradaic efficiency as high as 84.47% in 1 M KOH electrolyte. More importantly, it also exhibits excellent stability for 10 cycles. The successful introduction of M2+ vacancies was proved by electron paramagnetic resonance spectroscopy. X-ray photoelectron spectroscopy results confirmed that the implanted cationic vacancies would effectively raise the electron density of d-NiFe LDH and tailor the electronic structures of metal sites. This results in a significantly increased active site number and lowered charge transfer resistance that facilitate the electrocatalytic performance improvement. Postreaction characterization indicates that the in situ generated metal (oxy)hydroxides are the active species, and the HMF would be oxidized through both chemical and electrochemical pathways. These interesting findings shed light on the innovation of defect-rich catalysts and their promising application in electrochemical biomass derivative upgrading.
研究领域:
材料科学
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催化化学
·
生物质化学
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DOI
高影响因子
MONATSHEFTE FUR CHEMIE
·
2014
·Vol. 146
·期 3
·441-447
·
IF 1.347
Li Longfei,Chen Lin,Liu Weifeng,Yang Yongzhen,Liu Xuguang,Chen Yongkang
5-Fluorouracil surface-imprinted thermosensitive magnetic microspheres were prepared by using Fe 3 O 4 -encapsulating carbon microspheres as cores, N -isopropylacrylamide as thermosentitive monomer, ammonium persulfate as initiator, N , N ′-methylenebisacrylamide as crosslinker, and 5-fluorouracil as template molecule. The formation of these hybrid microspheres was verified by field emission scanning electron microscopy, transmission electron microscopy, Fourier transformation infrared spectroscopy, thermogravimetry, and dynamic light scattering. The results of the latter measurements show that the as-synthesized microspheres have a hydrodynamic diameter of 326 nm with the lower critical solution temperature of around 43 °C. The obtained microspheres are magnetic and show good potential for controlled loading and release of 5-fluorouracil. Graphical abstract
研究领域:
药剂学
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纳米医学
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肿瘤治疗
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高分子材料科学
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靶向给药系统
✓ 已验证
DOI
高影响因子
JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
·
2025
·
IF 4.9
Ahmed M. Omer,Eman M. Abd El-Monaem,Heba S. Hassan,Mahmoud A. Elmeligy,Angela Kleinová,Abdelazeem S. Eltaweil,Abolfazl Heydari
pH-sensitive carriers have emerged as an optimal choice for the oral administration of anticancer drugs, exhibiting the desired release performance. This study aims to develop biocomposite beads for the sustained release of the anticancer drug 5-fluorouracil (5-FU). Here, 5-FU was encapsulated within a ZIF-8 metal-organic framework (MOF), which was subsequently impregnated into amino-chitosan beads. The resulting Am-CS@ZIF-8 biocomposite beads were characterized for their chemical structure, surface morphology, elemental composition, crystallinity, surface charges, and mechanical properties utilizing Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), zeta potential analysis, and a texture analyzer, respectively. The developed beads exhibited a textured surface, denser composition, and a positively charged surface with a maximum zeta potential of +12.4 at pH 7.4. In comparison to Am-CS beads, the Am-CS@ZIF-8 biocomposite beads demonstrated superior mechanical properties, achieving a maximum stress value of 5.668 MPa compared to the 1.874 MPa recorded for pure Am-CS beads. pH sensitivity was assessed through the investigation of water uptake behavior at pH 1.2 and pH 7.4. The Am-CS@ZIF-8 biocomposite beads demonstrated a high encapsulation efficiency of approximately 81.6 % for 5-FU. They exhibited pH-responsive release behavior, with only 17 % of the drug released at pH 1.2 after 2 h and a sustained release of 52 % at pH 7.4 over 24 h. The release mechanism was predominantly governed by Fickian diffusion, as closely fitted by the Peppas-Sahlin kinetic model. The formulated carrier confirmed its biodegradability under enzymatic physiological conditions, suggesting its potential applicability as an effective system for the oral delivery of anticancer drugs.
研究领域:
药剂学
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生物材料学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Tao Jiang,Fumin Wang,Xubin Zhang,Yi Zhai,Guojun Lv,Yu Shen,Yuzhou Wu
Mesocrystal zeolite with well-defined morphology owns mesoporous channels and single crystal characteristics, which could promote diffusion efficiency, stability and catalytic activity. Thus, we performed the controllable synthesis of ZSM-5 mesocrystal without special additives and complex methods. Selected area electron diffraction (SAED) and fast Fourier transform (FFT) showed diffraction spots regardless of crystallization time, which indicated the well oriented feature of synthesized ZSM-5 zeolites. The crystallization process was further investigated. The oriented particle attachment (OPA) effectively guided the synthesis process of mesocrystals, which followed the nonclassical crystallization mechanism. The crystallinity curve exhibited valley-like shape, which manifested that the crystallization pathway went through three stages: fast precipitation, deconstruction and reorganization. The plausible formation mechanism was proposed, which might be useful for the fabrication of ZSM-5 mesocrystal. The prepared zeolites showed superior catalytic performance in aldol condensation reaction between benzaldehyde and 2-hydroxyacetophenone, obtaining 93% of the conversion.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Shiyou Xing,Pengmei Lv,Che Zhao,Ming Li,Lingmei Yang,Zhongming Wang,Yong Chen,Shijun Liu
Non-H 2 and solvent-free catalytic conversion of waste lipids to liquid hydrocarbons is of great interest because of the associated low-cost, full-safety, and easy-operability. In this work, a solvent-free catalytic process for deoxygenating oleic acid was performed in H 2 and non-H 2 (N 2 , CH 4 , and CO 2 ) media over nano-Ni/HZSM-5. 8-Heptadecene, a primary product obtained at 320 °C in four media, was derived from the straightforward decarboxylation of oleic acid. In non-H 2 medium at 360 °C, the formation of C 8 –C 15 alkanes was enhanced, with yields of ca. 65.05 mol%, 70.71 mol%, and 73.09 mol% for N 2 , CH 4 , and CO 2 , respectively. A low yield of 49.67 mol% C 8 –C 15 alkanes in H 2 medium suggested that the H 2 medium reduced catalytic cracking . This was due to the preferential formation of stable heptadecane from 8-heptadecene in the presence of abundant H 2 . The absence of H 2 favored the cracking of 8-heptadecene. These cracked products were further converted to C 8 –C 15 alkanes, for which a mass supply of hydrogen was mandatory. Gas-phase reactions including methanation , Fisher-Tropsch (F-T) synthesis, and water-gas shift (WGS) reactions between deoxygenated gas products and reaction media provided significant pathways for the hydrogen required for the formation of alkanes. The CH 4 medium also acted as a hydrogen source due to its decomposition, catalyzed by nano-Ni/HZSM-5. Coke was substantially formed in all the four media. It was highlighted that the medium of H 2 favored the formation of aliphatic cokes, whereas the non-H 2 media, particularly the CO 2 medium, facilitated aromatic coke species on account of its weak oxidizability. Additionally, there was a severe loss of loaded Ni nanoparticles under H 2 medium but a slight Ni loss in CO 2 medium, which was proposed to the reason of aromatic cokes formation at the catalyst surface , acting as a trap for the loaded Ni nanoparticles.
研究领域:
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
npj Science of Food
·
2025
·Vol. 9
·期 1
·1-10
·
IF 7.8
Sun Zhi,Wang Fangfang,Zhou Peipei,Chen Di,Zuo Lihua
5-Hydroxymethylfurfural (HMF), a product of the Maillard reaction and caramelization in honey, serves as a crucial marker of food quality and thermal processing, underscoring the importance of regulatory surveillance for consumer safety. This study introduces a method for rapid, high throughput and eco-friendly detection of HMF, using derivatization in matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS). 5,10,15,20-Tetrakis-(4-aminophenyl)-porphyrin was employed for in-situ derivatization of aldehydes after extraction by ethyl acetate, enhancing detection sensitivity by shifting low-molecular-weight aldehydes to higher regions. The calibration curves for HMF determination exhibited outstanding linearity. The detection limit reached 0.347 mg/kg with good accuracy and precision. Variations in the content of HMF in honey during heating were also assessed, revealing the increased formation of HMF under high temperature and prolonged heating. The method’s proficiency was evidenced through the detection of various aldehydes. This method represents an advance in rapid analysis for food safety, aligning with green chemistry principles.
研究领域:
食品科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2025
·
IF 4.9
Yang Chen,Cai Peng
Metal-organic frameworks (MOFs), consisting of both organic linkers and metallic ions, are expected to be excellent drug delivery agents for the treatment of cancer. However, the stability of MOF in the gastrointestinal tract remains to be resolved. In this study, we synthesized a MOF, namely Zr-NDC. Next, a thiolated chitosan (TCS) surface-modified Zr-NDC was developed, providing a strong impetus for oral 5-FU delivery. The most favorable interaction sites between 5-FU and Zr-NDC were explored by computer simulation. Then, the physicochemical properties of TCS-MOF, such as particle size, size distribution, and morphology, were evaluated. Through a series of experiments, including in vitro drug release experiments, MTT analysis, and in situ single small intestinal perfusion (SPIP), the results showed that under the protection of TCS-MOF, the release rate (2.3%) of 5-FU in an acidic environment was far lower than in artificial intestinal juice (60%). The coating of TCS on the surface of Zr-NDC has the effect of controlling drug release. TCS coating can enhance the acid resistance limit of MOF and further increase the adhesion and permeability of 5-FU to the intestinal mucosa. It is expected that TCS-MOF@5-FU can serve as a potential drug delivery system for oral 5-FU.
研究领域:
药剂学
·
肿瘤学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER BULLETIN
·
2018
·Vol. 76
·期 3
·1167-1182
·
IF 1.589
Wu Chengyi,Li Cong,Zhang Xu,Cheng Chao,Wang Jinshou
A novel pH-sensitive and macroporous NaAlg-based hydrogels were prepared, the monomers of which were N -methylolacrylamide (NMAAm) and acrylic acid, using N , N -methylene-bis-acrylamide (MBA) as a cross-linker, 2,2-dimethoxy-2-phenylacetophenone as a photoinitiator via ultraviolet irradiation. The morphology, thermal property and structure of hydrogel were characterized by Fourier transform infrared spectroscopy, scanning electron microscope, X-ray diffractometer and thermogravimetric analysis. The swelling ratios (SRs) of hydrogel were investigated in water, salt and pH solutions. The SR of hydrogel in water increased from 8.1 to 19.4 g/g with increase in weight of NaAlg from 0.2 to 1.0. The result indicated that hydrogel displayed favorable pH- and salt-sensitive. 5-fluorouracil (5-FU) as a model drug was loaded on hydrogel, the drug encapsulation efficiency of products reached to 85.2%, and the cumulative release rate of drug was 78.4 and 37% in the intestinal and gastric fluid, respectively. In addition, the dynamic data of drug release were evaluated by different mathematical models, and the experimental results revealed that it was more fitted to Ritger–Peppas and Higuchi equation models, correlation coefficients ( R 2 ) of which were up to 0.99.
研究领域:
材料科学
·
药学
·
生物医学工程
✓ 已验证
DOI
高影响因子
MACROMOLECULAR RAPID COMMUNICATIONS
·
2021
·Vol. 42
·期 21
·2100431
·
IF 5.734
Hanling Guo,Shengdu Yang,Long Cao,Lixia Chen,Ruihan Gao,Ying Huang,Bai Xue,Zhu Tao
The hydrogels composed of decamethylcucurbit[5]uril (Me 10 Q[5]) and para -phenylenediamine ( p -PDA) are first reported herein. They are the first Q[5]-based supramolecular hydrogels, the formation of which is driven by portal exclusion between Me 10 Q[5] and p -PDA. The composition, structure, and properties of the Me 10 Q[5]/ p -PDA-based hydrogels are investigated by various techniques. Since the 1D supramolecular chain forms via portal exclusion between Me 10 Q[5] and p -PDA is the key to the formation of the hydrogels, any competitive species, such as metal ions, organic molecules, and amino acids, which can affect the portal exclusion, can change the behavior of the Me 10 Q[5]/ p -PDA-based hydrogels. Hence, the hydrogels can be used for various applications. Importantly, the results may provide a new research direction for the preparation of Q[n]-based hydrogels via portal exclusion of Q[n]s with guests.
研究领域:
化学
·
材料科学
·
超分子化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）