ChemSusChem
·
2019
·Vol. 13
·期 2
·394-399
·
IF 7.804
Dengmeng Song,Bo Li,Xin Li,Xuzhuo Sun,Jun Li,Chengbo Li,Tongyu Xu,Yong Zhu,Fei Li,Ning Wang
Graphical Get in or get out : A cobaloxime catalyst and Eosin Y photosensitizer were assembled with macrocyclic cucurbit[7]uril through inclusion and exclusion interactions, respectively. The synchronous self-assembly drove an orthogonal arrangement of the ternary system with significant spatial proximity. The ternary supramolecular system showed better performance for photocatalytic H 2 evolution than multicomponent systems. The fabrication of efficient and convenient photocatalytic H 2 evolution systems is a fascinating research topic in the field of solar energy conversion. A ternary self-assembled photocatalytic H 2 evolution system was fabricated through supramolecular host–guest chemistry. The system consisted of the H 2 evolution catalyst [Co(dmgH) 2 (4-ppy) 2 ]NO 3 ( 1 ; dmgH 2 =dimethylglyoxime, 4-ppy=4-phenylpyridine) and the photosensitizer Eosin Y (EY) assembled with the macrocyclic compound cucurbit[7]uril (CB[7]) to form the 1 @CB[7]/EY complex through inclusion and exclusion interactions, respectively. The synchronous self-assembly drives an orthogonal arrangement of the 1 @CB[7]/EY system. The inclusion complex 1 @CB[7] was successfully characterized by 1 H NMR spectroscopy and single-crystal XRD. The exclusion process of CB[7] with EY was identified by NMR titration and the optimized geometry of the exclusion structure was determined by DFT calculations. The use of CB[7] resulted in a 6-fold increase in turnover number, a 3-fold increase in turnover frequency, and a 3-fold extension of lifetime for photocatalytic H 2 evolution as compared with the system in the absence of CB[7]. The improvement of the light-driven H 2 evolution activity was ascribed to the ability of CB[7] to link the photosensitizer and catalyst.
研究领域:
化学
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材料科学
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可再生能源研究
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2014
·
IF 4.331
Dan Chen,Xiaolong Ma,Jizhi Zhou,Xi Chen,Guangren Qian
We synthesized a novel magnetic composite, Fe 3 O 4 /Cu(Ni)Cr-LDH, as a heterogeneous catalyst for the degradation of organic dyes in the solution using sulfate radical-based advanced oxidation processes. The physicochemical properties of the composite synthesized via two-step microwave hydrothermal method were characterized by several techniques, such as X-ray diffraction (XRD), inductively coupled plasma (ICP), transmission electron microscopy (TEM) and vibrating sample magnetometer (VSM). The degradation tests were performed at 25 °C with Acid Orange 7 (AO7) initial concentration of 25 mg/L and AO7/peroxymonosulfate (PMS) molar ratio of 1:10, which showed that the complete degradation by Fe 3 O 4 /Cu 1.5 Ni 0.5 Cr-LDH could be achieved and the mineralization rate could reach 46%. PMS was activated by Cu (II) and Fe (II/III) of Fe 3 O 4 /Cu(Ni)Cr-LDH to generate sulfate radicals (SO 4 − ). Subsequently, the organic functional groups of AO7 molecules were destroyed by sulfate radicals (SO 4 − ), inducing the degradation of AO7. Moreover, the catalytic behavior of the catalysts could be reused five times. Therefore, our work suggested that the Fe 3 O 4 /Cu(Ni)Cr-LDH composite could be applied widely for the treatment of organic dyes in wastewater.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Chenkai Zhou,Daohui Lin,Kun Yang
Nonlinear sorption and isotherm nonlinearity of organic compounds by widely used porous resins such as XAD-7 are commonly interpreted as adsorption due to their large surface area. However, through displacement experiments using saturated 4-nitrophenol as the displacer, we observed that the nonlinear sorption and isotherm nonlinearity of selected organic compounds (i.e., naphthalene , nitrobenzenes , phenols and anilines) by XAD-7 was captured by a nonlinear partition mechanism rather than the adsorption mechanism. Nonlinear sorption of organic compounds by XAD-7 includes a nonlinear/displaced fraction and a linear/non-displaced fraction. A dual-mode (DM) model, including a nonlinear Dubinin-Ashtakhov (DA) model component and a linear model component, was developed to describe the nonlinear/displaced fraction and the linear/non-displaced fraction, respectively. The capacity of these two fractions are dependent on their solubility in water or octanol with positively linear relationships but not their molecular size, supporting the nonlinear partitioning mechanism. Besides van-der-waals force, hydrogen-bonding is primarily responsible for the nonlinear partitioning of phenols and anilines into XAD-7, while π-π interaction is responsible for the nonlinear partitioning of naphthalene and nitrobenzenes. The explored nonlinear partitioning mechanism for XAD-7 implies that the nonlinear sorption of organic compounds by porous resins should be recognized for their recovery and applications as sorbents .
研究领域:
环境科学
·
化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yeqiang Lu,Shiyang Li,Fuyou Chen,Hui Ma,Congjie Gao,Lixin Xue
Development of efficient absorbent materials for oil spillage clean-up and environmental pollution remediation is highly desired but remains a challenge. In this work, superhydrophobic/superoleophilic polysulfone based ZIF-7 composite (SPZ) foams were fabricated via chemical modification of polysulfone and integrating with hydrophobic coin-shaped ZIF-7 particles. The synergistic approaches provided the SPZ foams with high porosity, low density and superhydrophobic/superoleophilic features ( θ water =162.3°, θ oil =0°) and outstanding self-cleaning property. The as-prepared SPZ foams exhibited highly selective absorption capacity (up to 3800 wt%) for various kinds of oils and organic solvents. Furthermore, the SPZ foams still maintained 95.2% of its pristine absorption capacity and the θ water remained at 143.6° after ten absorption/distillation cycles. The SPZ foam showed outstanding separation ability towards different types of emulsions with separation efficiency all above 97%. The high oil/water separation efficiency and robust reusability made the SPZ foams promising absorbent in dealing with practical oil spills.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Jun Gao,Danyang Fan,Qinghua Chu,Haixia Lyu,Zenghong Xie
In this study, a novel surface molecularly imprinted polymer (MIP) based on zeolitic imidazolate framework (MIP@ZIF-7) was prepared using dibutyl phthalate (DBP) as template via “one-pot” method, which was used for extraction and determination four phthalates (PAEs) in food samples coupled with high performance liquid chromatography (HPLC). The obtained MIP@ZIF-7 was characterized by fourier transform infrared spectrometer (FT-IR), energy dispersive spectrum (EDS), scanning electron microscopy (SEM), nitrogen adsorption–desorption and contact angle tester. The adsorption performance of the prepared ZIF-7, MIP and MIP@ZIF-7 was compared and the results showed that MIP@ZIF-7 exhibited higher adsorption capacity and selectivity for PAEs owing to combining the high specific surface area and excellent stability of ZIF and the specific recognition of MIP. Subsequently, several requisite synthesis and extraction parameters were investigated. Under the optimal conditions, the linear range of the method was 1–100 μg L −1 and the detection limits were in a range of 0.1–0.8 μg L −1 . The spiked recovery rate of PAEs from drinking water, carbonated beverages and fruit juices ranged from 77.1 ± 1.5% to 100.7 ± 3.4%, with relative standard deviation of 1.65–4.87% (n = 3). The results indicated that MIP@ZIF-7 could be effectively employed for extraction and determination trace PAEs in food.
研究领域:
食品科学
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分析化学
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产品关联
DOI
高影响因子
JOURNAL OF CONTROLLED RELEASE
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2024
·
IF 10.5
Xuerong Zhao,Zhuoya Wang,Guanlin Wu,Lianhong Yin,Lina Xu,Ning Wang,Jinyong Peng
Intestinal ischemia reperfusion injury (II/R injury) is a common and intractable pathophysiological process in critical patients, for which exploring new treatments and mechanisms is of great importance to improve treatment outcomes. Apigenin-7-O-Glucoside (AGL) is a sugar derivative of apigenin natural product with various pharmacological activities to protect against intestinal diseases . In this study, we synthesized two amphiphilic molecules, namely DTPA-N10–10 and mPEG-TK-DA, which can scavenge free radicals and reactive oxygen species (ROS). They were successfully encapsulated AGL through self-assembly, resulting in the formation of multi-site ROS scavenging nanoparticles called PDN@AGL. In vitro and in vivo experiments demonstrated that PDN@AGL could protect intestinal tissues by reducing lipid peroxidation, lowering ROS levels and inhibiting ferroptosis during II/R injury. Furthermore, our study revealed, for the first time, that the regulation of the ATF3/SLC7A11 pathway by PDN@AGL may play a crucial role in mitigating II/R injury. In conclusion, our study confirmed the beneficial effects of PDN@AGL in combating II/R injury through the ATF3/SLC7A11-mediated regulation of ferroptosis and oxidative stress. These findings lay the groundwork for the potential application of PDN@AGL in the treatment of II/R injury.
研究领域:
药理学
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纳米技术
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胃肠病学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Hai-Peng Li,Zhi-Neng You,Yuan-Yang Liu,Gao-Wei Zheng,Heng Gong,Yiming Mo,Ning Zhu,Yun-Peng Bai,Jian-He Xu
Water-forming NAD(P)H oxidases (NOXs) constitute a clean NAD(P)+ regeneration strategy for NAD(P)+-dependent biotransformations to produce high value-added chemicals because they only consume oxygen and generate water. However, the application of NOXs is still challenging because of limited oxygen transfer in batch reactions. Here, we report an efficient continuous-flow microreactor (CFMR) to improve the oxygen transfer and reaction performance in NAD+-dependent chenodeoxycholic acid oxidation catalyzed by 7α-hydroxysteroid dehydrogenase (7α-HSDH) for the production of 7-oxo-lithocholic acid, a key precursor of ursodeoxycholic acid. The recycling efficiency of NAD+ by NOX from Streptococcus mutans (SmNOX) was significantly improved in this CFMR. Compared with a conventional batch stirred tank reactor, the space–time yield of production of 7-oxo-lithocholic acid was increased by 96-fold. Furthermore, the total turnover number of NAD+ was improved 10-fold, and the enzyme consumption number was decreased 7-fold. Combining the NOX/O2 system with this microreactor technology provides a general platform that enables various NAD(P)+-dependent biotransformations in a green and sustainable manner, which will be helpful in the design of ecofriendly bioprocesses for production of functional chemicals on a large scale.
研究领域:
生物化学
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合成生物学
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绿色化学
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产品关联
DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 8
·1-12
·
IF 3.8
Li Qi,Zhu Yanping,Liu Yanbiao,Chen Xiaoguang,Jiang Nan,Yan Mengying,Li Xuhua,Xing Haoyu,Bao Yinzhou,Huang Manhong
Antimonate (Sb(V)), sulfate and acid orange 7 (AO7) are common pollutants in printing and dyeing wastewater. Currently, there have been no reports about the effects of sulfate and AO7 on Sb(V) removal by anaerobic granular sludge (AnGS). In this study, the Sb(V) removal and Sb(Ш) accumulation was revealed in presence of sulfate and AO7, and the role of adding granular activated carbon (GAC) was investigated. Results showed that sulfate inhibited Sb(V) removal by AnGS (S + Sb, k = 0.101). GAC alleviated the inhibition of sulfate on Sb(V) removal and Sb(V) removal rate increased by 1.9 times (GAC + S + Sb, k = 0.187). Meanwhile, GAC promoted sulfate reduction by AnGS. AO7 inhibited sulfate reduction, thereby alleviating the inhibition of sulfate on Sb(V) removal, and Sb(V) removal rate increased by 1.5 times (S + Sb + dye, k = 0.147). When Sb(V), sulfate and AO7 coexisted, adding GAC actually inhibited Sb(V) removal (GAC + S + Sb + dye, k = 0.067), which may be due to GAC promoted the reduction of sulfate and AO7 by AnGS. The microbial community analysis revealed that Acinetobacter genus was related to Sb(V) reduction, with higher relative abundance in GAC + S + Sb (49.4%) and S + Sb + dye groups (28.9%). These results provided guidance for anaerobic treatment of printing and dyeing wastewater. Graphical Abstract
研究领域:
环境科学
·
微生物学
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DOI
高影响因子
FOOD CHEMISTRY
·
2022
·
IF 9.231
Xin Zhang,Li Tian,Zhuo Sun,Qian Wu,Xiangyu Shan,Yingjie Zhao,Ruizhan Chen,Juan Lu
A molecular-imprinted electrochemiluminescence sensor for procymidone (PCM) detection was reported based on Ru(bpy) 3 2+ @ZIF-7. A novel self-accelerated Ru(bpy) 3 2+ @ZIF-7 was prepared by one-step synthesis method, which exhibited high electrochemiluminescence (ECL) emission as a coreactant in the presence of tri- n -propylamine (TPrA). Concretely, ZIF-7 was not only the carrier of Ru(bpy) 3 2+ , but also the co-reaction promoter of Ru(bpy) 3 2+ /TPrA ECL system. The introduction of molecular imprint polymer (MIP) with PCM gave new characteristics of specific recognition of analyte PCM. The change value of ECL intensity (ΔI) was proportional to the logarithm of PCM concentration, with a wide linear range and a low detection limit of 1.0 × 10 −10 to 1.0 × 10 −6 mol L −1 and 2.0 × 10 −11 mol L −1 , respectively. The presented MIP-ECL sensor had high sensitivity, selectivity and stability, and had great potential in the field of food safety detection.
研究领域:
分析化学
·
食品安全检测
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Lina Yang,Suimin Deng,Hailing Liu,Xiangfeng Wang,Pingye Deng,Yuan Liu,Mengxia Xie
The pollution of water environment resulted from antibiotic abuse and harmful cyanobacteria blooms poses a serious threat to the ecological environment and human health, thus development of effective approaches to degrade and remove these pollutants is crucial to guarantee environmental security. In this work, TiO 2 /Hemin@MAF-7 composites with photo-Fenton-like cascade catalytic degradation activity have been successfully prepared by a self-assembly method. The photocatalysts exhibit high degradation efficiency towards tetracycline antibiotics in water solution under UV light irradiation. Furthermore, the TiO 2 /Hemin@MAF-7 composites have the potential ability to degrade other organic pollutants under the irradiation of visible light. A possible photocatalytic degradation mechanism of the photocatalyst is proposed, which follows a Z-scheme heterojunction type. The introduction of the hemin component into the heterojunction composites significantly promotes the separation of the photo-generated charges on the catalyst, which drives the photo-Fenton-like cascade catalytic cycle degradation reaction. Additionally, the photocatalyst can effectively inhibit the growth of the Microcystis aeruginosa in water environment by damaging the structure of algal cells. This work provides a practical solution for the degradation of antibiotic residues and control of harmful cyanobacteria blooms in wastewaters, and offers a promising strategy for efficiently removing multiple emerging contaminants in water environments.
研究领域:
环境科学
·
生物学
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产品关联
DOI
高影响因子
MOLECULAR PHARMACEUTICS
·
2023
·
IF 4.9
Wen-Juan Ma,Hua-Yu Chen,Yong-Liang Huang,Jia-Mei Chen,Tong-Bu Lu
This study is designed to compare drug encapsulation by cucurbit[7]uril and β-cyclodextrin, using fluorofenidone as a model drug. Single-crystal X-ray diffraction analysis was employed to successfully determine the crystal structures of fluorofenidone·H+@cucurbit[7]uril Form, fluorofenidone@cucurbit[7]uril Form, and fluorofenidone@β-cyclodextrin Form. Keto–enol tautomerization of fluorofenidone mediated by cucurbit[7]uril in acid solution is confirmed by crystal structures, pH titration, and nuclear magnetic resonance experiments. However, β-cyclodextrin cannot cause the keto–enol tautomerization of fluorofenidone under similar conditions. The phase solubility study demonstrates that cucurbit[7]uril has a much higher solubilization capacity for fluorofenidone than β-cyclodextrin in 0.1 M HCl since the Kc values of fluorofenidone with cucurbit[7]uril and β-cyclodextrin were 1223.97 ± 452.68 and 78.49 ± 10.56 M–1, respectively. Excellent solubility can be attributed to the keto–enol tautomerization of fluorofenidone under the conditions of cucurbit[7]uril in acid solution. The enol form of fluorofenidone is encapsulated by cucurbit[7]uril by hydrogen bonding interaction and hydrophobic interaction to increase binding affinity. Rat pharmacokinetic studies demonstrate that the area under the plasma concentration–time curve from time 0 to 7 h value of fluorofenidone@cucurbit[7]uril complex is 1.70-fold greater than that of free fluorofenidone, and the mean residence time from time 0 to 7 h is slightly prolonged from 1.29 to 1.76 h (P < 0.01) after oral administration. However, no significant difference is found between fluorofenidone and fluorofenidone@β-cyclodextrin complex. This work indicates that the induction of keto–enol tautomerization of drugs using macrocyclic molecules has the potential to be an effective method to improve their solubility and bioavailability, providing valuable insights for the application of macrocyclic molecules in the biomedical field.
研究领域:
药学
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生物化学
·
药物递送系统
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产品关联
DOI
PubMed
高影响因子
Bioresources and Bioprocessing
·
2023
·Vol. 10
·期 1
·1-12
·
IF 4.6
Dai Mohan,Xu Binpeng,Guo Qing,Wan Junfen,Cao Xuejun
Ursodeoxycholic acid (UDCA) is not only safer than chenodeoxycholic acid in the treatment of hepatobiliary diseases, but also has a wide range of applications in Acute Kidney Injury and Parkinson’s Disease. The purpose of this experiment is to improve the conversion rate of 7-ketocholic acid (7K-LCA) and the yield of ursodeoxycholic acid in aprotic solvents during electrochemical reduction process. Three aprotic solvents were investigated as electrolytes. 1,3-Dimethyl-2-imidazolidinone (DMI) has a stable five-membered ring structure, and 7K-LCA has undergone two nucleophilic reactions and “Walden” inversion, the 7K-LCK was stereoselectively reduced to UDCA. Hexamethylphosphoramide (HMPA) and 1,3-methyl-3,4,5,6-Tetrahydro-2(1 H )-pyrimidinone (DMPU) can be attacked by chloride ions to produce by-products. Molecular orbital theory-based simulations were conducted to study the reducibility of three aprotic solvents [hexamethylphosphoramide (HMPA), 1,3-methyl-3,4,5,6-Tetrahydro-2(1 H )-pyrimidinone (DMPU), and 1,3-Dimethyl-2-imidazolidinone (DMI)] in combination with experiments. Choose the best solvent based on the simulation results, the electrolysis reaction can be carried out by applying current and voltage when lithium chloride is used as electrolytes. Calculations using Materials Studio showed that Cu, Pb, Hg–Cu, and Ni exhibited the highest binding energies to the substrate in this system. Using Cu as the electrode when the solvent is a 1:1 mix of DMI and HMPA, the conversion rate of 7-ketocholic acid (could reach 98%, the yield of ursodeoxycholic acid was up to 80%. Under the same conditions, linear voltammetry was performed on the electrochemical workstation to study the electrolysis behavior, and the obtained results were consistent with the experiment. Graphical Abstract
研究领域:
药理学
·
有机化学
·
生物化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）