ACS Nano
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2016
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IF 13.334
Xuning Li,Zhimin Ao,Jiayi Liu,Hongqi Sun,Alexandre I. Rykov,Junhu Wang
Innovation in transition-metal nitride (TMN) preparation is highly desired for realization of various functionalities. Herein, series of graphene-encapsulated TMNs (FexMn6–xCo4–N@C) with well-controlled morphology have been synthesized through topotactic transformation of metal–organic frameworks in an N2 atmosphere. The as-synthesized FexMn6–xCo4–N@C nanodices were systematically characterized and functionalized as Fenton-like catalysts for catalytic bisphenol A (BPA) oxidation by activation of peroxymonosulfate (PMS). The catalytic performance of FexMn6–xCo4–N@C was found to be largely enhanced with increasing Mn content. Theoretical calculations illustrated that the dramatically reduced adsorption energy and facilitated electron transfer for PMS activation catalyzed by Mn4N are the main factors for the excellent activity. Both sulfate and hydroxyl radicals were identified during the PMS activation, and the BPA degradation pathway mainly through hydroxylation, oxidation, and decarboxylation was investigated. Based on the systematic characterization of the catalyst before and after the reaction, the overall PMS activation mechanism over FexMn6–xCo4–N@C was proposed. This study details the insights into versatile TMNs for sustainable remediation by activation of PMS.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Pan Zhang,Yirui Shu,Ye Wang,Xiaohou Zhou,Lin Yang,Xiushan Yang
Cobalt-doped ZnFe 2 O 4 supported on rice husk carbon (RHC) has been prepared by a microwave-assisted method as a catalyst for the degradation of bisphenol A (BPA) by persulfate (PS) oxidation . Ferrite is a good absorbing material, RHC contains abundant channels, which provide channels for microwaves(MW) reflecting and scattering, and accelerate the synthesis of ZC 1.3 FO. In addition, the polarization and synergistic effect of the contact interface between the two phases is enhanced, which not only improves the dispersity of the magnetic material, but also enhances electron delocalization in the mixed material, promoting electron transfer between Co 3+ /Co 2+ and Fe 3+ /Fe 2+ , and improving the catalytic activity . Our results have shown the degradation rate of BPA by ZnCo 1.3 Fe 0.7 O 4 -50 wt%RHC (ZC 1.3 FO-5C) (0.0697 L/mg min) to be 28 times higher than that by ZC 1.3 FO (0.00251 L/mg min), and the extents of leaching of cobalt and iron were lower than 45 μg/L. Particle video microscopy (PVM) have been used to confirm improved dispersion of composite particles compared to that of a single catalyst during degradation. Free radical quenching experiments, electron paramagnetic resonance (EPR), and X-ray photoelectron spectroscopy (XPS) have confirmed that BPA degradation was caused by the synergistic action of non-free radical and free radical pathways. Intermediates have been identified by electrospray ionization mass spectrometry (ESI-MS), on the basis of which a degradation pathway of BPA by activated PS oxidation in the presence of ZC 1.3 FO-5C is proposed. In brief, a ZC 1.3 FO-5C composite has been prepared by a microwave method to activate PS for the degradation of BPA, realizing the resource utilization of waste ferrous sulfate derived from titanium dioxide production, providing a new concept for the degradation of organic pollutants .
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Journal of Environmental Chemical Engineering
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2026
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IF 7.5
Yunhe Cui,Yue Tao,Hudong Fan,Ting Liu,Ying Zhang
SiO 2 @PDA-Lac achieved BPA-dominant removal with synchronous DBP reduction. • PDA-coated mesopores enhanced pollutant enrichment and laccase anchoring. • SiO 2 @PDA-Lac retained BPA/DBP removal after 5 cycles and 50 d storage. • Docking and GC-MS revealed competitive binding and divergent pathways. • ECOSAR predicted overall toxicity reduction after enzymatic transformation. The potential co-occurrence of bisphenol A (BPA) and dibutyl phthalate (DBP) in contaminated water motivates the development of treatment strategies for binary pollutant systems. Herein, a polydopamine-functionalized mesoporous silica immobilized laccase system (SiO 2 @PDA-Lac) was developed for BPA-dominant removal and synchronous DBP reduction. Immobilization time was first selected by balancing initial activity and cycling stability. With the time fixed at 6 h, immobilization pH, temperature, and laccase concentration were further optimized by RSM using relative enzyme activity as the response, yielding pH 4.0, 25 °C, and 80 mg/mL laccase. In the binary system at an initial pollutant concentration of 100 mg/L, SiO 2 @PDA-Lac removed approximately 81% of BPA and 20% of DBP. Control experiments with free laccase and inactivated SiO 2 @PDA-Lac indicated that BPA removal was driven by coupled interfacial adsorption and enzymatic catalysis, whereas DBP reduction was lower but still measurably assisted by immobilized laccase. SiO 2 @PDA-Lac retained detectable performance after five cycles, with BPA and DBP removal remaining at 57% and 14%, respectively, and maintained removal activity after 50 d of storage. Molecular docking and molecular dynamics simulations suggested that BPA and DBP may occupy partially overlapping binding microenvironments. GC-MS and ECOSAR analyses indicated possible transformation pathways with an overall tendency toward lower predicted ecological risk. These results demonstrate the feasibility of SiO₂@PDA-Lac for BPA-dominant removal and concurrent DBP reduction in a model BPA/DBP binary system. Download: Download high-res image (314KB) Download: Download full-size image
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Journal of Energy Storage
·
2023
·
IF 9.4
Shichao Feng,Xiaodong Qin,Dongying Hu
In this research, the layered bionic wood films were designed and constructed inspired by the “reinforced concrete”-like chemical structure of wood combined with the macrostructure of bark and phloem. Specifically, a simple strategy for immobilizing diol eutectic phase change components with intelligent discoloration/chromogenic leaching in wood by using delignification wood (DE) with capillary penetration was adopted. The “reinforced concrete” structure solves the problem of easy leakage and weak strength due to strong molecular bonding. The bionic wood film has a high phase change enthalpy (155.5 J/g) and suitable phase change temperature (29.9 °C). On this basis, combined with PVA/glycerol as a flexible matrix as the inner bark of wood and phloem connecting each layer, combined with PVA/glycerol/PLO-8C as a key self-luminescent energy-enriched material as the outer bark of wood, the flexible and self-luminescent energy-saving wood films were reconstructed in a biomimetic way with a high mechanical strength (65.53 MPa). Through the change of color, the phase transition process and the current ambient temperature can be intuitively judged. The surface morphology and luminescence intensity were also not affected after 50 cycles of absorption and luminescence. This study provides a broader development direction for the application of intelligent enhanced energy enrichment of PCM-based on bionic wood construction.
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POLYMER
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2023
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IF 4.6
Yang Yang,Bo Jiang,Yingshuang Shang,Qinfei Xu,Junjie He,Xuefeng Li,Haibo Zhang
The limited diffusion and entanglement of the chains between beads cause pronounced anisotropy in the mechanical properties of 3D printed parts. Therefore, amorphous poly (aryl ether ketone) (aPAEK) containing fluorene groups with high intrinsic strength and good interfacial fusion is synthesized and employed to improve the interlayer adhesion of poly (ether ether ketone) (PEEK) parts. Herein, we designed an aPAEK with high intrinsic strength and good interfacial fusion with PEEK blends. The tensile strength of 30 mol% fluorene groups aPAEK was improved to 75 MPa, and the interlayer strength of 20 wt% blends was increased by 315 % compared to PEEK. Moreover, the selection of an appropriate molecular weight for aPAEK is crucial in maintaining the elevated tensile strength while promoting interlayer diffusion during the printing process. These results highlight a novel strategy for the design and development of blend polymers for interlayer reinforcement in 3D printing applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Wei Zhang,Runtang Liu,Longwen Lei,Binbin Nian,Shipin Yang,Yi Hu
Efficient and stable catalysis has always been a fundamental concept in enzyme-catalyzed industrial processes. However, the poor stability of laccase has hindered its application in industry. The conventional methods of immobilization have proven to be ineffective in achieving both stability enhancement and the maintenance of high activity simultaneously. To address this challenge, we have constructed a magnetic core–shell structured metal–organic framework doped with copper ions (MCIL@Cu-UiO-66-NH2), which leverage the synergistic effects of copper ion activation and covalently binding to immobilize laccase. The resulting immobilized laccase exhibited high activity recovery (89%) and stability, retaining 90% relative activity after 30 days of storage and 66% of its initial activity after being exposed to a temperature of 60 °C for 6 h. The application of immobilized laccase in the removal of aqueous organic pollutants was also investigated. The results demonstrate that immobilized laccase can remove 2,4-dichlorophenol completely within 8 h and maintains approximately 90% removal efficiency after undergoing five cycles. Moreover, immobilized laccase also exhibited favorable results in the removal of other phenolic pollutants and typical aromatic pollutants, which are difficult to degrade, such as indole and anthracene. The copper ion-doped magnetic MOF composite novel introduced in this work demonstrated promising potential as an efficient carrier for laccase immobilization, and the immobilized laccase exhibits practical application prospects in the field of wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Limin Duan,Huihao Jiang,Borui Cai,Wenhao Wu,Daohui Lin,Kun Yang
Generating defect sites in iron based metal–organic frameworks (Fe-MOFs) by introducing defective ligands has recently emerged as an effective approach to optimize Fenton-like activity, but the structure–activity relationship between defective ligands and Fenton-like reaction is still not fully understood. Herein, a series of defective MIL-100(Fe), i.e., Dx-MIL-100(Fe), were constructed via introducing defective ligands with various functional groups including -N,–NO 2 ,-Cl and –OH. It was observed that defect density and Fenton-like activity of D X -MIL-100(Fe) is positively correlated with the electronegativity of functional groups in defective ligands. With the increasing defect density, the stability and recyclability of D X -MIL-100(Fe) in Fenton-like reaction was not decreased, which is attributed to increasing coordination bond energy between defective ligands and Fe-O cluster. The high defect density results in the increase of electron density of Fe and rate of Fe Ⅲ reduction. Therefore, D N -MIL-100(Fe) possessing highest defect density exhibited superior Fenton-like activity with the pseudo-first-order kinetic constant up to 0.089 min −1 for Bisphenol A degradation, which is 148.3 times than that of perfect MIL-100(Fe). Meanwhile, D N -MIL-100(Fe) showed excellent pH adaptability, anti-interference ability and cycle stability. This work unravels the role of functional groups in defective ligands on regulating defect density, Fenton-like activity and stability for the first time, which can provide a novel platform for precisely designing Fe-MOFs as promising Fenton-like catalyst.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
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2023
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IF 2.5
Weiping Xu,Guochen Wang,Dong Chen,Wantai Yang,Yuhong Ma
As an effort to improve toughness of epoxy resins without scarifying their heat resistance, four novel polyether sulphones (PESs) with epoxy groups (PES-Es) are developed as efficient toughness modifiers of epoxy resins. The influences of PES-E on the mechanical property, curing kinetics, thermal, and mechanical properties of the diglycidyl ether with bisphenol-A (DGEBA) are investigated. The impact strength of PES-E/DGEBA composites is significantly improved from 16.6 to 28.9 kJ m −2 with optimal content of PES-E. Different from the composites of typical PES and epoxy which have two-phase structure, PES-E/DGEBA composites exhibit a single-phase structure owing to the participation of PES-E in the curing reaction of epoxy groups and good solubility of PES-E in DGEBA. Furthermore, the thermal stability of the PES-E/DGEBA composites is slightly increased compared to the neat epoxy resin due to the formation of crosslinked semi-interpenetrating polymer networks. The glass transitionnal temperature ( T g ) of PES-E/DGEBA composites is up to about 184 °C, 46 °C higher than the neat epoxy resin with the same hardener, which have great potential in high-performance composites. The method developed in this seminal report makes it possible to improve the toughness of epoxy resins without trading-off the T g and tensile strength.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-15
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IF 16.6
Wei Shengjie,Sun Yibing,Qiu Yun-Ze,Li Ang,Chiang Ching-Yu,Xiao Hai,Qian Jieshu,Li Yadong
Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect engineering of single Fe-N 4 sites in ZnO-Carbon nano-reactor, as efficient catalyst in Fenton-like reaction for degradation of phenol. The carbon vacancies are easily constructed adjacent to single Fe-N 4 sites during synthesis, facilitating the formation of C-O bonding and lowering the energy barrier of rate-determining-step during degradation of phenol. Consequently, the catalyst Fe-NCv-900 with carbon vacancies exhibits a much improved activity than the Fe-NC-900 without abundant carbon vacancies, with 13.5 times improvement in the first-order rate constant of phenol degradation. The Fe-NCv-900 shows high activity (97% removal ratio of phenol in only 5 min), good recyclability and the wide-ranging pH universality (pH range 3-9). This work not only provides a rational strategy for improving the Fenton-like activity of metal single-atom catalysts, but also deepens the fundamental understanding on how periphery carbon environment affects the property and performance of metal-N 4 sites.
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高影响因子
ANALYTICA CHIMICA ACTA
·
2026
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IF 6.1
Xi Bian,Kang Cheng,Hao Gao,Shaokai Jian,Zeyu Lin,Xinxin Zhang,Chengji Sui,Dafeng Jiang,Yongchao Lai
In-tube SPME-SERS platform enables rapid pollutant screening. • Dynamic flow enhances mass transfer and extraction capacity. • Sampling, enrichment, and detection are completed within 3 min. • The method successfully screens multiple hydrophobic pollutants in water. Background Given the persistence, bioaccumulation, and toxicity of hydrophobic pollutants (HPs), rapid and reliable screening methods are critically needed. Herein, we propose an integrated approach coupling surface-enhanced Raman spectroscopy (SERS) with in-tube solid-phase microextraction (in-tube SPME) for the rapid screening of HPs. The device integrates a dual-functional substrate (tert-dodecylthiol-modified silver nanostructures) within a quartz capillary and a syringe pump for flow control. During analysis, sample solutions are pumped through the capillary, enabling rapid HP adsorption onto the substrate via hydrophobic interactions under continuous flow. Results This dynamic configuration enhances mass transfer efficiency, facilitating rapid SERS detection with a portable Raman spectrometer. The entire “sampling and detection” workflow of the in-tube SPME-SERS method can be completed within 3 min. This method exhibits a good linear relationship (R 2 = 0.997) for the quantitative determination of Sudan III over the concentration range of 5–100 nM, with a limit of detection (LOD) as low as 0.658 nM, demonstrating outstanding sensitivity. Furthermore, the method shows satisfactory performance in terms of spatial homogeneity, batch-to-batch reproducibility, and long-term stability. Significance By balancing speed and accuracy in environmental HP analysis, this work provides a robust framework for portable screening platforms with significant potential for ecological monitoring and exposome research. Download: Download high-res image (211KB) Download: Download full-size image
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MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Xin-Yan Zhang,Xu-Xia Yan,Shao-Yu Sun,Cheng-Zhen Wu,Hui-Dong Qiu,Qian-Yu Zhou
Laccase-like Cu-GMP complex forms directly without tedious synthesis. • The homogeneous system effectively avoids light-scattering interference. • The platform detects 2,4-DCP, BPA and epinephrine with low detection limits. • Smartphone-based colorimetry enables portable, low-cost on-site detection. • Good recoveries are achieved in lake water and human serum samples. The rapid and sensitive screening of phenolic compounds is essential for environmental safety and clinical diagnostics. Although laccase-like Cu-based nanozymes offer cost-effective alternatives to natural enzymes, most existing platforms rely on heterogeneous nanoparticles. These systems not only require tedious pre-treatment, but also suffer from light scattering that compromises colorimetric accuracy. Herein, a homogeneous colorimetric sensing platform based on the laccase-like activity of a copper-guanosine 5′-monophosphate (Cu-GMP) complex was developed. The complex is prepared directly in solution without the need for time-consuming synthesis. Furthermore, this homogeneous system eliminates light-scattering interference due to its intrinsic optical transparency. Benefiting from its catalytic versatility, the platform enabled the quantification of three phenolic targets. 2,4-dichlorophenol (2,4-DCP) and bisphenol A (BPA) were detected via 4-aminoantipyrine (4-AAP)-mediated coupling, while epinephrine was quantified by direct catalytic oxidation, with detection limits of 0.22, 0.59, and 0.21 μM, respectively. Additionally, integrating this system with smartphone technology enabled a portable platform for on-site quantification, demonstrating reliable accuracy in lake water and human serum samples. Overall, this work provides a versatile and low-cost homogeneous strategy for the point-of-need screening of phenolic pollutants and biomarkers. Download: Download high-res image (123KB) Download: Download full-size image
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Xianheng Li,Huan Li,Keqiang Lai,Junjian Miao,Jie Zhao
A novel hydrophobic natural deep eutectic solvent (NADES) was designed and prepared to selectively enrich biphenolic compounds. The NADES was prepared by blending different molar ratios of octanol and menthol. Various important parameters that influence the extraction efficiency were optimized, including the composition of NADES components, volume, the influence of salt, extraction time, and pH. The experimental results demonstrated that the method exhibited a wide linear range (5–1000 μg/L) with a linear correlation coefficient (R 2 ) exceeding 0.995. The limits of detection (LOD) and quantification (LOQ) ranged from 0.44 to 0.96 μg L −1 and 1.33 to 3.16 μg L −1 , respectively. Furthermore, quantum chemical calculations were utilized to analyze the electrostatic potentials of menthol, octanol, water, and the three biphenolic compounds, providing insights into the extraction mechanism of NADESs. The environmental impact of the proposed method was assessed using the ComplexGAPI and Whiteness method, revealing its eco-friendliness. Finally, the method was successfully employed for the extraction and determination of the three bisphenols in beverage samples.
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