CHIRALITY
·
2025
·Vol. 37
·期 8
·e70050
·
IF 3
Xiangwen Chen,Xuan Chen,Juan Pan,Shuqi Deng,Qiubing Qin,Qiang Fu,Jiliang Cao
In this work, the silica gel bonded amylose[( S )-α-methylbenzyl carbamate] (CHIRALPAK IH) was chosen as the chiral stationary phase (CSP) for the separation of five quinolone enantiomers by high-performance liquid chromatography (HPLC), namely, ofloxacin, flumequine, nadifloxacin, lomefloxacin, and clinafloxacin. The mobile phase composition, organic modifier, and acid–base additive were systematically investigated for the baseline separation of these five interested quinolones. The optimized mobile phases were n -hexane–ethanol–acetic acid–diethylamine (60:40:0.2:0.2, v / v / v / v ) for ofloxacin and nadifloxacin, n -hexane–ethanol–acetic acid–diethylamine (60:40:0.2:0.2, v / v / v / v ) for flumequine, n -hexane–isopropanol–acetic acid–diethylamine (60:40:0.3:0.3, v / v / v / v ) for lomefloxacin, and n -hexane–ethanol–acetic acid–diethylamine (70:30:0.3:0.3, v / v / v / v ) for clinafloxacin. The interaction forces between the amylose CSP and target quinolones were simulated by computerized molecular docking to study their enantiorecognition mechanisms. The results indicated that hydrogen bonding, π–π stacking, and hydrophobic interactions collectively contributed to the stereoselective binding. The differences in these interaction forces between the quinolone enantiomers, particularly the greater contribution of hydrogen bonding in one enantiomer compared to the other, led to a significant difference in binding energy. This differential binding energy ultimately governed the elution order and enabled chiral recognition of the five quinolone enantiomers.
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Materials Today Chemistry
·
2024
·
IF 6.7
Xiangdong Shi,Xiaoyun Qin,Xuanyu Yang,Xiangyu Wei,Ying Liu,Sihui Li,Guixia Liu,Jinxian Wang,Xiangting Dong,Fenghua Chen
It is challenging and still difficult to adjust and boost the catalytic performance of photocatalysts via the synergistic achievement of heteroatom doping, vacancies engineering, morphology regulation, and appropriate structural design. Herein, we developed an efficient method to synthesize 3D hierarchical porous BiOI–Bi 2 S 3 S-scheme heterojunction with oxygen vacancies (Ov-BBS) induced by sulfur doping and systematically investigated regulation of oxygen vacancies by sulfur doping and their effects on photocatalytic performance. Results showed that sulfur species promoted the formation of S-scheme heterojunction but depleted oxygen vacancies in Ov-BiOI. The optimal sulfur doped catalyst (Ov-BBS-0.1) exhibited excellent UV–vis light photocatalytic activity towards four representative pollutants, affording removal rate of 97.1 % for MB, 97.6 % for RhB, 99.4 % for Cr(VI), and 92.0 % for TC, respectively, which were higher than those of pristine Bi 2 S 3 , BiOI, Ov-BiOI, Ov-BiOI/Bi 2 S 3 mixture, Ov-BBS-0.05, and Ov-BBS-0.2. Deep characterizations and theoretical studies certified that the four-pronged enhancement strategy of 3D hierarchical porous structure, oxygen vacancies, sulfur doping and the constructed S-scheme heterojunction, not only enriched accessible active sites, but also promoted electronic polarization and modulated electronic structure, resulting in rapid separation and migration of photogenerated carriers. Moreover, considering the excellent stability and cyclic photocatalytic performance, the film prepared by pumping Ov-BBS dispersion was also satisfactory in the practical application of circulating sewage treatment. Overall, the present work provides a novel approach for the design of more photocatalysts with high efficiency.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Wei Li,Siyuan Cao,Xu Yin,Qi Zhang,Liankai Gu,Hongwei Zhu,Kajia Wei,Weiqing Han
Seeking efficient and facile methods for precise oxygen vacancy (Ov)-content regulation is challenging for practical application. Herein, we propose a confinement-based Ov optimization strategy, and construct Fe 3 O 4 with controllable Ov confined in S-doped mesoporous carbon (Fe 3 O 4 @SMC) catalyst to enhance nonradical oxidation of PMS. The confinement effect induced the O 2p orbitals p-band-center shift in Fe 3 O 4 @SMC, which promoted Ov formation, thus achieving 100 % BPA degradation within 9 min via an electron-transfer process (ETP) dominated nonradical pathway with a 125.8-fold higher k obs value than unconfinement catalyst. Ov content variation under confinement, triggered by tuning confined support defect level, steered nonradical transition from single-electron-activated singlet oxygen route to two-electron-transferred ETP pathway, which improved selectivity (> 95 % of electron-rich pollutants removal), adaptability and durability (10 h continuous-flow operation) of catalyst. This work paves the way for modulating Ov in iron-oxides via confinement engineering and offers new insights into the Ov-induced mechanism in confined environments.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hao Du,Rubin Huo,Aoxiang Liu,Yuxin Hui,Bo Shen,Ningyi Li,Yun Ji,Qin Jin,Baobing Zheng,Guoxiang Yang,Zhe Zhang,Qi Wang
Herein, a photo-self-Fenton system of resorcinol-formaldehyde resins/MIL-88A(Fe) (RF/88A) S-scheme heterojunction was successfully established to in-situ generate and activate H 2 O 2 toward tetracycline (TC) degradation and sterilization under visible light illumination. As a result, the 35 %-RF/88A (the mass ratio of RF to 88A was 35 %) can remove most TC and kill approximately 100 % E. coli and S. aureus . Notably, the composites presented superior repeatability and wide pH application range. Fukui index identified the reaction sites of TC molecule and quantitative structure-activity relationship (QSAR) forecasted intermediates toxicity. Density functional theory (DFT) calculations were performed to investigate electron transfer mechanism of the heterojunctions on a molecular scale. Such a S-scheme charge transfer route was also proved by in situ irradiated X-ray photoelectron and electron paramagnetic resonance measurements. In summary, this research innovatively provides deep insights into the in-situ generation and activation of H 2 O 2 and exhibited an environmentally friendly way toward pollutant degradation and sterilization.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2018
·
IF 3.974
Ruilong Li,Huadong Tan,Linlin Zhang,Shaopeng Wang,Yinghui Wang,Kefu Yu
Microplastics sorption of persistent organic pollutants (POPs) was the core processes that cause negative effects to biota, and their influencing factors and related mechanisms are poorly understood. In this study, we explored the impacts of water extractable organic matter (WEOM), an important source of endogenous dissolved organic matter in mangrove sediment, on the sorption coefficients of typical parent, alkyl and N/O/S-containing polycyclic aromatic hydrocarbons (PAHs) by microplastics. The presence of L-WEOM (D) impeded the PAHs sorption as the coefficients ( K f ) decreased to 10.17 (μg/kg)/(μg/L) n and to 8.39 (μg/kg)/(μg/L) n for fluorene (Flu) and 1-methyl-fluorene (1-M-Flu), respectively. The K f exhibited good linear relationships with the aliphaticity of L-WEOM ( p < 0.05) rather than the aromatic carbon/alkyl carbon content ( p > 0.05). Under the presences of L-WEOM (D), (S) and (K), the lone pair electrons of N/O/S-containing PAHs was the dominant factor contributing to the obvious difference of the K f values from the other groups. Moreover, the largest impact of L-WEOM (D) on the Flu sorption was in the case of PVC microplastics, while almost no effect was in the case of PS microplastics. The findings of our work may be helpful in improving our understanding of the role of WEOM on the sorption of PAHs to microplastics in the field mangrove sediment.
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DALTON TRANSACTIONS
·
2016
·Vol. 45
·期 47
·19062-19071
·
IF 4.177
Guang-Ning Liu,Ke Li,Qing-Shun Fan,Hui Sun,Xin-Yu Li,Xiao-Nan Han,Yu Li,Zhen-Wei Zhang,Cuncheng Li
Solvothermal reactions of AgI with the vulcanization accelerator 2,2′-dibenzothiazolyl disulfide and hydroiodic acid in alcohols afford two hybrid iodoargentates with one-dimensional structures, namely (Et2mbt)[Ag2I3] (1, Hmbt = 2-mercaptobenzothiazole) and {(Hmbt)[AgI]}n (2). The syntheses of both 1 and 2 involve unprecedented multiple in situ reactions. Specifically, a simultaneous disulfide bond cleavage, N and S donor atoms bialkylation, and self-assembly reaction lead to 1 that contains a discrete N,S-biethylated cation (Et2mbt)+ and a rare inorganic (Ag2I3)− anionic chain, while a simultaneous disulfide bond cleavage, N-protonation and self-assembly reaction affords 2 which features zwitterionic Hmbt molecules coordinating with the opposite side Ag atoms of a neutral inorganic (AgI)n chain via forming Ag–S coordination bonds. The simultaneous alkylation on a thiazolyl-N donor and a thiol-S donor atom for a thiazolyl-based heterocycle using inexpensive alcohols and haloids under solvothermal conditions instead of traditional two-step organic synthesis was found for the first time. The two compounds have band gaps of 2.95 eV for 1, and 2.78 eV for 2 exhibiting an observed blue shift compared with bulk AgI. Also, 1 and 2 can be used as effective heterogeneous photocatalysts for methyl orange dye treatment under UV light irradiation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Hui Li,Ziqun Wang,Yunhui He,Sugang Meng,Yun Xu,Shifu Chen,Xianliang Fu
Rational synthesis of photocatalytic materials is an effective way to improve their performance. In this work, to optimize the S precursors, a series of Mn x Cd 1−x S (MCS) were first hydrothermally synthesized with the prevalent thiourea (TA), thioacetamide (TAA) and L-cysteine (L-Cys) as the S sources. The optimum feed ratio of Mn/Cd was then determined based on the optimized S precursor. The effects of S precursors and the feed ratio of Mn/Cd on the phase structure, absorption, morphology, band structure, and the photocatalytic hydrogen evolution reaction (HER) performance of MCS were investigated systematically. The hexagonal phase structures of MnS, CdS, and MCS are favored by TA and L-Cys as the S sources, while their cubic phases are benefited by TAA. TAA is the preferred S source for the preparation of highly active MCS and the solid solution is formed through the consolidation of cubic α-MnS into cubic CdS. The activity of MCS can be improved with the increase of Mn content from x = 0–0.6. The sample with x = 0.6 shows the highest HER activity (2253 μmol·h −1 ·g −1 ) and the performance is almost 6 times higher than CdS (416 μmol·h −1 ·g −1 ). The enhanced activity can be attributed to the improved separation efficiency of photo-induced charge carriers and the negative-shifts of E cb , which are induced by the introduction of Mn. A segregation of inert α−MnS from MCS is occurred when Mn content is >0.6, resulting in a decay of the HER activity. A change of the semiconductivity from n-type to bipolar type is occurred in MCS due to the uneven sulfidation of Mn in MCS.
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ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2020
·
IF 3.023
Zeyu Yang,Wenjie Ye,Youyu Xie,Qinghai Liu,Rong Chen,Hualei Wang,Dongzhi Wei
Bioreductions catalyzed by alcohol dehydrogenases (ADHs) play an important role in the synthesis of chiral alcohols. However, the synthesis of ethyl (S)-4-chloro-3-hydroxybutyrate [(S)-CHBE], an important drug intermediate, has significant challenges concerning high substrate or product inhibition toward ADHs, which complicates its production. Herein, we evaluated a novel ADH, SmADH31, obtained from the Stenotrophomonas maltophilia genome, which can tolerate extremely high concentrations (6 M) of both substrate and product. The coexpression of SmADH31 and glucose dehydrogenase from Bacillus subtilis in Escherichia coli meant that as much as 660 g L–1 (4.0 M) ethyl 4-chloroacetoacetate was completely converted into (S)-CHBE in a monophasic aqueous system with a >99.9% ee value and a high space-time yield (2664 g L–1 d–1). Molecular dynamics simulation shed light on the high activity and stereoselectivity of SmADH31. Moreover, five other optically pure chiral alcohols were synthesized at high concentrations (100–462 g L–1) as a result of the broad substrate spectrum of SmADH31. All these compounds act as important drug intermediates, demonstrating the industrial potential of SmADH31-mediated bioreductions.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2020
·Vol. 412
·期 23
·5843-5851
·
IF 3.637
Chen Hongqi,Yang Xueping,Liu Yunchun,Wang Lun
Glutathione S-transferase (GST) is a detoxification enzyme of the liver and kidney. Based on the toxicological effect of GST, it is of great significance to develop a rapid and sensitive detection method for GST. In this work, a new luminescence resonance energy transfer (LRET) system has been designed to detect glutathione S-transferase in the near-infrared (NIR) region by utilizing NaGdF 4 :Yb 3+ ,Tm 3+ @NaYF 4 upconversion nanoparticles (UCNPs) as the donor and NIR dye-806@Glutathione (IR806@GSH) as the acceptor. NaGdF 4 :Yb 3+ ,Tm 3+ @NaYF 4 UCNPs were synthesized by a coprecipitation method and surface modification of NOBF 4 . The donor (positively charged) interacted with the acceptor (negatively charged) via electrostatic interactions to bring them into close proximity; then, LRET occurred and the luminescence was quenched. In the presence of GST, GST can specifically interact with the GSH of IR806@GSH molecule, making IR806@GSH far away from the donor surface, inhibiting the LRET, and restoring the luminescence of the UCNPs. There was a good linear relationship between the luminescence recovery intensity of UCNPs and GST concentration, ranging from 0.11 to 14.19 nM, and the detection of limit was 0.06 nM. The method has been used in the detection of GST in human serum samples and is expected to have potential applications in the biological field.
A luminescence resonance energy transfer system was developed for determination of glutathione S-transferase in the near-infrared region by utilizing NaGdF 4 :Yb 3+ ,Tm 3+ @NaYF 4 upconversion nanoparticles as the donor and NIR dye-806@Glutathione as the acceptor
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COLLOID AND POLYMER SCIENCE
·
2009
·Vol. 287
·期 4
·495-500
·
IF 1.736
Wang Chen-Yi,Li Peng-Hui,Li Guang,Jiang Jian-Ming
A series of novel fluorinated poly(ether ketone amide)s (PEKAs) were prepared from an unsymmetrical aromatic diamine, (4′-(4″-amino-2″-trifluoromethylphenoxy)-3′,5′-dimethylphenyl)(4-aminophenyl)-methanone ( 1 ), with various aromatic dicarboxylic acids using the phosphorylation polycondensation technique. The PEKAs had inherent viscosities ranging from 0.43 to 0.65 dl/g. All the fluorinated PEKAs could be soluble in many polar organic solvents such as N -methyl-2-pyrrolidinone (NMP), N,N ′-dimethylacetamide (DMAc), N,N ′-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and tetrahydrofuran (THF). Flexible and tough polymer films could be prepared by casting from DMAc solvent. The PEKA films exhibited high optical transparency with a cutoff wavelength of 354–365 nm and good mechanical properties with tensile strengths of 78–98 MPa and elongations at break of 11.5–18.5%. They showed glass-transition temperatures in the range of 288−323 °C and the onset decomposition temperatures in the range of 450−461 °C in nitrogen atmosphere. Meanwhile, the PEKA films possessed low dielectric constants of 1.98–2.71 at 1 MHz and low moisture absorption (<2%). Due to their properties, the fluorinated PEKAs could be considered as photoelectric and microelectronic materials.
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JOURNAL OF MATERIALS RESEARCH
·
2019
·Vol. 34
·期 4
·545-554
·
IF 1.982
Yong Xu,Linshuang Li,Jianfei Che,Zhifeng Ye
A series of optically transparent and colorless semi-fluorinated poly(ether imide)s (PEIs) (III) were prepared from non-fluorinated 1,4-bis(3,4-dicarboxyphenoxy)benzene dianhydride (HQDPA) with various trifluoromethyl-substituted diamines. The III series showed more colorless and higher optical transparency with a cutoff absorption wavelength (λ0) below 370 nm than the IV series based on the corresponding non-fluorinated analogues and V series derived from CF3-free pyromellitic dianhydride (PMDA). Compared with the fluorinated VI series based on fluorinated 4,4′-hexafluoroisopropylidenediphthalic anhydride (6FDA), the semi-fluorinated III series not only exhibited much better optical transparency, but also had better mechanical and thermal properties. The III series had a tensile strength of 79.8–109.5 MPa, modulus of elasticity of 3.0–7.7 GPa and elongation at break of 14.2–26.7%, together with glass-transition temperatures (Tg) ranging from 214.3 to 265.1 °C and temperatures of 5% weight loss (T5%) beyond 530 °C. Meanwhile, the novel semi-fluorinated PEI IIIb was optically transparent and colorless with a λ0 of 367 nm coupled with dielectric constants below 3.2 and contact angles against water over 112°. In particular, the optically transparent IIIa exhibited the best tensile strength of 109.5 MPa when compared with already reported counterparts.
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Advanced Sustainable Systems
·
2022
·Vol. 6
·期 7
·2200060
·
IF 6.737
Hengfei Qin,Shipeng Luo,Yan Li,Yifan Zhang,Ruoyu Dong,Yang Zhou,Jing Luo,Yeling Zhu,Feng Jiang
The hydrogen production by water electrolysis has attracted great research interest as a sustainable approach for clean energy production. However, such process is plagued by the use of high-cost precious metal-based catalysts (such as Pt, RuO 2 ). Hereby, the use of a low-cost Nitrogen and Sulfur co-doped carbon-supported cobalt sulfide dual-functional electrocatalyst derived from imidazole modified lignin for overall water splitting is presented. To introduce nitrogen and sulfur heteroatoms in the carbon structure, lignin is modified by imidazolation through thiol-alkynes click reaction. Imidazole-lignin shows a strong chelation tendancy with cobalt salt, and N and the S co-doped cobalt sulfide catalyst (IL-Co@GC-PO) is obtained by pyrolysis. The IL-Co@GC-PO has an oxygen evolution potential of 1.57 V and a hydrogen evolution overpotential of 204 mV at a current density of 10 mA cm −2 . During the overall water splitting process, the IL-Co@GC-PO catalysts require only 1.58 V to reach a current density of 10 mA cm −2 , which is equivalent to the performance of the system composed of the noble metal Pt/C||RuO 2 . This work not only provides a strategy for the preparation of N and S co-doped cobalt sulfide catalysts, but also provides guidance for using lignin as a carbon source to design and develop cheap electrocatalysts.
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