Advanced Healthcare Materials
·
2026
·
IF 11
Jiarong Liang,Si Wang,Zhonghui Ma,Fei Kuang,Xiangkun Li,Zhilong Gong,Jinzhu Su,Zhiyi Wang
Combining efficient photocatalytic activity with precise targeting is crucial for covalent organic framework (COF)-based nanomedicines to remodel the immunosuppressive microenvironment and sensitize “cold” tumors to immunotherapy. Herein, we constructed two isomorphic frameworks featuring distinct electronic topologies: a zwitterionic squaric acid (SA) COF with inherent electrostatic asymmetry, and a charge-neutral terephthaldehyde (TA) COF. The spatial divergence of ion centers in SA COF triggers intense molecular-level ionic displacement polarization, creating a robust internal electric field. Such unique field-effect regulation accelerates photogenerated charge separation for efficient superoxide anion production, enhances intersystem crossing for singlet oxygen generation, and promotes nonradiative energy relaxation for high-performance photothermal conversion under dual-wavelength irradiation. After PEGylation and iRGD modification, the formulated SA@PEG-iRGD exhibits excellent physiological stability and active deep tumor penetration. With near-infrared absorption, it enables high-contrast photoacoustic imaging for guided dual-wavelength (660/808 nm) phototherapy. This spatiotemporally controlled therapeutic cascade triggers lethal ferroptosis and precise photothermal ablation, potently activating immunogenic cell death. Combined with aPD-L1 therapy, it eliminates primary tumors, produces abscopal effects, and establishes immune memory against recurrence and metastasis. This study highlights the value of electronic structure engineering in COF-based precision nanomedicine.
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LANGMUIR
·
2026
·
IF 4.4
Chao Ge,Yunlan Gu,Bin He,Yanqing Wang,Yawen Tang,Tongfei Li
The advancement of catalysts that are both platinum-group-metal (PGM)-free and iron-free is essential for the oxygen reduction reaction (ORR), which is kinetically slow, particularly in anion-exchange membrane fuel cells (AEMFCs). One of the primary obstacles lies in achieving adequate activity and stability within the membrane electrode assembly (MEA) under real-world hydrogen-air operating conditions. Herein, an effective MnN4 site encased within N-doped carbon nanofibers (denoted as MnN4@N-CNFs) is designed for efficient ORR electrocatalysis. Benefiting from the electronic structure modulation of MnN4 moieties through strong interfacial coupling with the carbon matrix, and structural advantages of the 3D hierarchical porosity synergizing with N-doped carbon-MnN4 coordination systems, the as-resultant MnN4@N-CNFs demonstrate a high half-wave potential of 0.89 V, outstanding durability, and impressive methanol tolerance under alkaline environments, outperforming commercial Pt/C and a diversity of reported counterparts. Notably, the engineered catalyst demonstrates remarkable fuel cell performance with a peak power density of 222.0 mW cm–2 during practical AEMFC operation, while maintaining stable operation for over 15 h, representing a 3-fold enhancement over conventional Pt/C-based counterparts. This study establishes fundamental design principles for high-efficiency AEMFCs through atomic-level engineering of precisely coordinated metal–N–C active sites, providing a robust framework for next-generation electrocatalyst development.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Xiaojie Zhang,Jinchen Zhao,Yan Zhao,Zhumabay Bakenov,Yongguang Zhang
The lithium sulfur (Li-S) battery holds great promise in next-generation energy storage technologies. However, the lithium polysulfide (LiPS) shuttle and slow reaction kinetics still limit its commercial development. Here, a squaraine-based porous organic framework (POF) with sulfophilic and lithiophilic moieties was developed as the separator modifications for the first time. The POF coating layer on the common separator builds a strong barrier against the LiPS shuttling, resulting in a robust inhibition on the shuttle effect as well as boosted sulfur reaction kinetics. Therefore, the POF-PP separator demonstrates stable cycling performance with a low capacity attenuation rate of 0.04% over 500 cycles and high areal discharge capacity of 4.67 mAh cm −2 with a sulfur loading of 5 mg cm −2 , which show high potential for high loading and practical Li-S battery.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Jiaqi Liu,Fuyi Sun,Yuanyuan Che,Kaihuan Nie,Zhihao Zhang,Zhen Yang,Liangliang Lin
Metal organic frameworks (MOFs) have shown widespread applications in many aspects owing to their unique structures. In this study, a thin and homogenous UTSA-280/PEI-HPAN nanofiltration membrane was fabricated by combining interfacial reaction and in-situ self-assembly reaction, which showed rejections of 83.79%, 86.17%, 99.42% and 98.93% for MO, AF, MB and CR solutions together with permeances up to 262.54, 197.51, 145.97 and 170.63 L·m −2 ·h −1 ·MPa −1 , respectively. In addition, the UTSA-280/PEI-HPAN membranes demonstrated a preferable stability in 48 h continuous test, a good anti-fouling property in both HA and BSA fouling test and an outstanding reusability, and they also showed high permeances and rejections even after four cycles. The results indicate that the stable UTSA-280/PEI-HPAN hybrid membrane with high separation performances can be a promising material for wastewater treatment .
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 45
·期 2
·679-684
·
IF 3.288
Rui Xue,Hao Gou,Li Zhang,Yinsheng Liu,Honghong Rao,Guohu Zhao
A new two-dimensional covalent organic polymer material (ST-1) was synthesized by the condensation of squaric acid and melamine. The preparation is simple and cheap. Fourier transform infrared spectra (FT-IR), X-ray photoelectron spectroscopy (XPS), N2 adsorption–desorption, powder X-ray diffraction (XRD), scanning electron microscopy (SEM) and thermogravimetric analysis (TGA) were employed to characterize the structure and properties of ST-1. This material presents the highest specific capacitance value of 177.6 F g−1 at a current density of 0.3 A g−1 in a three electrode configuration in a 6 M potassium hydroxide electrolyte. The retention rate of the specific capacitance can be maintained at about 60.24% when the current density is increased by 50 times. It is worth mentioning that ST-1 also demonstrates about 94% capacitance retention after 10 000 galvanostatic charge–discharge cycles.
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Analytical Methods
·
2018
·Vol. 10
·期 6
·611-616
·
IF 2.073
Yue Gao,Xiaolu Yan,Meng Li,Han Gao,Jing Sun,Shuyun Zhu,Shuang Han,Li-Na Jia,Xian-En Zhao,Hua Wang
A novel turn-on fluorescent sensor for the detection of ascorbic acid (AA) has been developed based on the fluorescence resonance energy transfer (FRET) between graphene quantum dots (GQDs) and squaric acid (SQA)-iron(III). In this assay, iron(III) can rapidly coordinate with the SQA to produce SQA-iron(III). The absorbance band of SQA-iron(III) could be largely overlapped with the emission band of GQDs, thus resulting in the fluorescence resonance energy transfer (FRET)-induced fluorescence quenching of GQDs. Moreover, the fluorescence of GQDs can be sensitively turned on by AA through the oxidation-reduction between iron(III) and AA. After the transformation of SQA-iron(III) to SQA-iron(II), because the absorbance of the solution reduces, the FRET decreases. This FRET-based nanosensor shows high selective and sensitive response in the concentration of AA ranging from 1.0 to 95 μM with the detection limit as lower as 200 nM, which is lower than that of other fluorescent assays. Finally, the proposed sensing system was successfully applied to the direct analysis of AA in the real samples with satisfactory results.
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TALANTA
·
2016
·
IF 4.035
Hongyu Chen,Aijin Fang,Li He,Youyu Zhang,Shouzhuo Yao
Diabetes mellitus is an epidemic disease that it has became a worldwide public health problem. Thus, blood glucose monitoring has attracted extensive attention. Here, we report a nanosensor based on inner filter effect (IFE) between upconversion nanoparticles (UCNPs) and squaric acid (SQA)-iron(III) for the highly sensitive and selective detection of glucose levels in human serum. In this assay, GOx-catalyzed oxidization of glucose produces gluconic acid and hydrogen peroxide (H 2 O 2 ). The latter can catalytically oxidize iron(II) to iron(III) which can rapidly (<1 min) coordinate with the SQA to produce (SQA)-iron(III). The absorption band of (SQA)-iron(III) largely covered the emission band of UCNPs, resulting the fluorescence emission of UCNPs was effectively quenched. Therefore, the glucose can be monitored based on the formation of SQA-iron(III). Under the optimal condition, the fluorescence quenching efficiency shows a good linear response to glucose concentration in the ranges of 7–340 μmol/L with a detection limit of 2.3 μmol/L. The developed method has been further applied to monitor glucose levels in human serum with satisfactory results. Compared with other fluorescence methods , current method displayed high sensitivity and signal-to-noise ratio. Meanwhile, this nanosystem is also generalizable and can be easily expanded to the detection of various H 2 O 2 -involved analytes.
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ANALYTICAL CHEMISTRY
·
2014
·
IF 5.825
Wenqiang Lai,Dianping Tang,Junyang Zhuang,Guonan Chen,Huanghao Yang
This work reports on a simple and feasible colorimetric immunoassay with signal amplification for sensitive determination of prostate-specific antigen (PSA, used as a model) at an ultralow concentration by using a new enzyme-chromogenic substrate system. We discovered that glucose oxidase (GOx), the enzyme broadly used in enzyme-linked immunosorbent assay (ELISA), has the ability to stimulate in situ formation of squaric acid (SQA)-iron(III) chelate. GOx-catalyzed oxidization of glucose leads to the formation of gluconic acid and hydrogen peroxide (H2O2). The latter can catalytically oxidize iron(II) to iron(III), which can rapidly (<1 min) coordinate with the SQA. Formation of the iron-squarate complex causes the color of the solution to change from bluish purple to bluish red accompanying the increasing absorbance with the increment of iron(III) concentration. On the basis of the SQA-iron(III) system, a new immunoassay protocol with GOx-labeled anti-PSA detection antibody can be designed for the detection of target PSA on capture antibody-functionalized magnetic immunosensing probe, monitored by recording the color or absorbance (λ = 468 nm) of the generated SQA-iron(III) chelate. The absorbance intensity shows to be dependent on the concentration of target PSA. A linear dependence between the absorbance and target PSA concentration is obtained under optimal conditions in the range from 1.0 pg mL–1 to 30 ng mL–1 with a detection limit (LOD) of 0.5 pg mL–1 (0.5 ppt) estimated at the 3Sblank level. The sensitivity displays to be 3–5 orders of magnitude better than those of most commercialized human PSA ELISA kits. In addition, the developed colorimetric immunoassay was validated by assaying 12 human serum samples, receiving in good accordance with those obtained by the commercialized PSA ELISA kit. Importantly, the SQA-based immunosensing system can be further extended for the detection of other low-abundance proteins or biomarkers by controlling the target antibody.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Xinghang Duan,Qiaolin Li,Tiantian Cao,Shengxiang Xiong,Gang Chen,Chengjun Dong,Hongtao Guan,Zongyou Yin
The development of advanced electromagnetic (EM) wave absorbers is crucial for applications in stealth technology and EM interference shielding. A major challenge in this field is achieving high absorption efficiency across a broad frequency range while maintaining lightweight and structurally robust materials. In this study, we successfully developed a precise and flexible synthesis strategy to prepare hollow C/Co/Mo2C cubes using Zn/Co(C4O4)(H2O)2 as a flexible template, which offers the advantages of simultaneous removal and easy control of metal Co content. The shell of the hollow cubes can be further optimized by changing the oxidizer content for polypyrrole (PPy). At optimum shell thickness and Co content, the C/Co/Mo2C-0.4 composites, featuring hollow but perforated structures, exhibit superior EM wave absorption properties, with a minimum reflection loss (RLmin) of −73.46 dB and an effective absorption bandwidth (EAB) of 5.20 GHz at 2.0 mm with 15 wt% filler. Detailed investigations reveal that the hollow C/Co/Mo2C-0.4 cubes provide polarization loss, conduction loss, magnetic loss, and optimal impedance matching characteristics, significantly enhancing EM wave absorption performance. This work offers a promising strategy for assembling multiple components into a hollow architecture, offering superior molybdenum carbide microwave absorbers.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Gong Cheng,Chao Sui,Weizhe Hao,Zifu Zang,Yushun Zhao,Yichen Zhou,Chenxi Zhao,Lei Wen,Junjiao Li,Yuna Sang,Xiaodong He,Chao Wang
Smart composite materials are attracting increasing attention for their novel stimulus-response characteristics. Among them, Cellulose nanofibers (CNF)-based smart composites are widely used due to their excellent properties. For enhancing the response rate and stability of CNF-based smart composite actuator, a novel covalent organic framework (COF) nanoparticle is synthesized via molecular design to enhance CNF-based multi-responsive composite materials. COF-TASA, characterized by a high specific surface area, exhibits the highest photothermal conversion efficiency of 79.9% for COF materials to date. A multi-stimuli responsive actuator is prepared through the compounding of COF-TASA, CNF, and polyvinylidene fluoride (PVDF). The smart membrane demonstrates a reversible ability to change shape when exposed to near-infrared (NIR) light and humidity. This is caused by the asymmetric deformation of the COC and PVDF layers. Finally, the mechanism for the enhancement of the smart response rate of the system by COF-TASA is successfully elucidated through experiments and molecular dynamics (MD) simulations, indicating that the introduction of COF forms ordered channels in the COC, greatly enhancing the specific surface area and the transport speed of water molecules. This COF-enhanced smart actuator is anticipated to provide important solutions for smart control, smart detection, and environmental energy collection.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Chongxi Zhang,Fengting Li,Dong Wu,Qingmeng Guo,Zhanning Liu,Zhikun Wang,Zixi Kang,Lili Fan,Daofeng Sun
Integration of cobalt phosphides (Co2P and CoP) in a carbon matrix shows great promise for developing high-performance catalysts for water electrolysis. Nevertheless, the controlled synthesis of these two phases with an effective interface, uniform dispersion, and a simplified synthesis process is still challenging. Herein, we proposed a strategy that involves pre-construction of the Co/CoO@C heterostructure followed by post-conversion by phosphorization to achieve the precise synthesis of the Co2P/CoP@C heterostructure, which was realized by utilizing a MOF as the self-sacrificial template. The oxygen-coordinated MOF that shows advantages in building the Co/CoO heterostructure was employed in this work and grown into a high-quality membrane via cathodic electrodeposition on the graphite substrate (Gss). The obtained catalyst (Gss-Co2P/CoP@C-800) requires 146 and 365 mV overpotentials to achieve a current density of 100 mA cm−2 for the HER and OER, respectively, and 1.54 V to achieve a current density of 10 mA cm−2 for water electrolysis. Beyond the significantly enhanced conductivity that originates from the robust interaction between the MOF and Gss, the establishment of an effective Co2P/CoP interface also plays a pivotal role in contributing to the high performance of Gss-Co2P/CoP@C-800. As revealed by density functional theory (DFT) calculations, the unique d-orbital electron distribution of Co2P/CoP and the enhanced state density near the Fermi level facilitate its efficient electron transport and render the Co2P/CoP heterostructure region a crucial active site for water electrolysis. This study will provide new insights into the rational design and construction of heterostructures based on MOFs for efficient and green energy conversions.
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Small Methods
·
2024
·
IF 10.7
Li Chen,Cuiyun Zhou,Feng Jiang,Li Zhang,Chuanlai Xu
Phenylpyrazoles are widely used pesticides in the food industry. It is highly desirable to develop efficient pre-treatment and analysis methods to extract and detect phenylpyrazoles in complex food matrices. Herein, the study reports novel squaraine-linked zwitterionic core-shell magnetic covalent organic frameworks (MCOFs), which are found to be excellent pretreatment materials for the detection of trace phenylpyrazoles in samples. By coupling MCOFs to magnetic solid-phase extraction (MSPE) with Ultra Performance Liquid Chromatography-Tandem Mass Spectrometry (UPLC-MS/MS) analysis, the detection of phenylpyrazoles (fipronil, fipronil sulfone, fipronil sulfide, fipronil de-sulfoxide, fipronil desulfinyl, ethiprole, and flufiprole) is achieved and shows good linearity at concentrations of 1–800 µg L −1 (R 2 ≥ 0.9930). The limit of detection (LOD), limit of quantification (LOQ), and recovery rates are 0.01–0.50 µg kg −1 , 0.04-1.72 µg kg −1 , and 70.96–115.32%, respectively. More importantly, this method is successfully applied to determine the phenylpyrazoles in commercial egg, poultry, milk, jujube, cabbage, tea, and rice with a detection rate of ≈0.04%. Therefore, the developed method may contribute to a new strategy for the purification and multi-target extraction of complex food matrices.
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