ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Pengfei Li,Yang Deng,Haiyuan Wang,Yali Luo,Yin Che,Ruijuan Bian,Ruoyun Gao,Xianfeng Wu,Zhen Zhang,Xu Wu
Understanding the microenvironment structure-activity relationship of singlet-atom catalysts (SACs) is imperative for the development of high-performance photocatalytic devices. However, the challenge remains to finely regulate the coordination microenvironment of SACs. Herein, single-atom N x ─Cu─O 4-x ( x = 1–4) photocatalysts with different coordination environments are successfully prepared based on pre-design reticular supramolecular covalent organic frameworks (COFs) for direct photocatalytic 1 O 2 production from O 2 . The results show that the high activity of Cu SACs is closely related to the N,O-coordination microenvironment, which is primarily ascribed to the different electrophilicity of the N, O atom. The electron configuration of N 3- Cu-O 1 endows photocatalyst enhanced charge transfer capability and the nearest D-band center to the Fermi level. The “end-on” type adsorption configuration of O 2 at the N 3 ─Cu─O 1 active site can promote the breaking of Cu─O bonds rather than O─O bonds. As a result, the N 3 -Cu-O 1 @COF photocatalyst exhibits the most optimal formation and desorption energies for intermediates •OOH, which provides an advantageous reaction pathway with fewer steps and a lower barrier for 1 O 2 production. This work highlights the structure-activity relationship of SACs for long-term applications.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Simeng Wu,Jiangyiming Jiang,Chengjuan Wang,Yanxiang Wang
Morphological engineering is crucial for conceiving high-efficiency electromagnetic wave (EMW) absorption materials. However, for carbon fiber-based composites, the management of micromorphology is significantly astricted by complex fabrication. It remains highly challenging to clarify the micromorphological influences on the EMW loss mechanism of carbon fiber-based absorption materials. In this work, micromorphology-optimized Cu/C nanocomposite fibers are prepared by virtue of a metal–organic framework (MOF) template-assisted strategy. Through skillfully grafting the morphology-regulation capacity of MOFs onto composite fibers, the Oswald maturation and particle distribution issues of Cu nanoparticles are settled, and the efficient electron transport pathways are established by the bead-like structure of the fiber matrix. Compared to prepared conventional Cu/C nanocomposite fibers, the MOF template-assisted strategy stimulates a remarkable leap in EMW absorption performance. The minimum reflection loss value of Cu/C-40 can reach −64.5 dB, 15.96 times lower than that of a conventional sample (Cu/C-2). The maximum effective absorption bandwidth extends to 6.08 GHz, contrasting the ineffective performance of Cu/C-2. Systematic research demonstrates that the enabled graphite-catalytic function of Cu nanoparticles collaborated with an optimized conductive network structure plays a pivotal role in creating field-induced leakage currents, facilitating conductive loss, the primary contributor to EMW dissipation. This work establishes a correlation mechanism between micromorphology and EMW loss, presenting a compelling example of customizable carbon fiber-based absorbers.
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高影响因子
TRIBOLOGY INTERNATIONAL
·
2025
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IF 6.9
Shanshan Li,Chuanping Gao,Chunjian Duan,Shengmao Zhang,Pingyu Zhang,Zhijun Zhang
Oil-based superlubricity introduces a novel approach to energy conservation. Facing two main obstacles at present, i.e., higher viscosity of lubricating oil and special tribopairs, a novel solid-liquid combined system is built in this work, which is mainly based on excellent tribological property of oil-soluble dialkyl-dithiophosphoric-modified Cu nanoparticles (DDP-Cu NPs) and superior self-lubricating capability of polymeric tribopairs. In this system, polyetheretherketone (PEEK) is coupled with polytetrafluoroethylene (PTFE) to form a similar/dissimilar tribopair; and neat PAO40 (a real serving lubricating oil with high viscosity in poly-alpha olefin oil family), or PAO40 containing oil-soluble DDP-Cu NPs (PAO40 + Cu), is used as a lubricant during the sliding test. The results show that only dissimilar tribopair, i.e., PEEK-PTFE, can achieve oil-based superlubricity under the selected sliding conditions, which can be attributed to the synergistic effect between PEEK-PTFE tribopair and PAO40/PAO40 + 0.25 Cu. Furthermore, due to lower cohesive energy density (CED), PTFE is more likely to be transferred onto PEEK together with some tribochemical reactions, finally generating a high-performance tribofilm rich in carboxylated PTFE. In addition, it is concluded that, when lubricated with PAO40, the above synergistic effect is a key to achieve superlubricity; and for PAO40 + 0.25 Cu, the carboxylated PTFE and the exposed Cu core will create chelate effect, which can not only further enhance this synergistic effect, but also improve the wear-resistance of the system reaching near-zero wear. This work not only provides a novel idea for designing oil-based superlubricity system, but broadens the type of tribopair materials achieving oil-based superlubricity to some extent.
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NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Yuying Zhang,Na Li,Lianmei Chen,Fangrui Yu,Xueru Sheng,Jian Zhang,Qingwei Ping,Hongbin Li
Laccase immobilization is an effective way to realize the industrial application of laccase, but the loss of immobilized laccase activity is serious, which is an urgent problem to be solved. In this study, a novel laccase immobilization material was prepared by mixing waste Mn–Cu-loaded activated carbon with cellulose solution and regenerated in hydrochloric acid solution, which significantly improved the immobilized laccase activity. The optimum immobilization conditions (T, pH and initial laccase concentration) of Mn–Cu-AC/cellulose beads (Mn–Cu-ACC) for laccase were studied by the response surface method. Under the optimum conditions (T = 43 °C, pH = 4.0 and c = 6.8 g L−1), immobilized laccase (Laccase@Mn–Cu-ACC) showed excellent performance in terms of pH stability, thermostability and storage stability. And the enzyme activity of the laccase immobilized on the Mn–Cu-ACC carrier remarkably increased by 29.6% compared to that of the ACC. At last, the Laccase@Mn–Cu-ACC was used for the degradation of bisphenol A (BPA). Under the optimum conditions (t = 5.5 h, T = 45 °C, pH = 4.0 and initial cBPA = 70 mg L−1), the removal rate of BPA reached 72.3% in the first cycle, and after 5 cycles of reusing the immobilized laccase, the relative removal rate of BPA was retained at 53.2% of the initial removal rate. This study developed a new type of immobilized laccase carrier and provided a new path for the application of waste heavy metal loaded activated carbon.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 11
·1-11
·
IF 5.3
Xu Yuanyuan,Yin Qingqing,Du Ningjing,Yi Yinhui,Zhu Gangbing
By preparing Cu@CuO aerogel as a nanozyme which exhibits prominent peroxidase-like (POD) activity, an innovative homogeneous electrochemistry (HEC) coupled with the colorimetry dual-model sensing strategy is proposed to detect perfluorooctane sulfonate (PFOS) for the first time. Cu@CuO aerogel accelerates the oxidation process of colorless o-phenylenediamine to form yellow 2,3-diaminophenazinc (DAP), and meanwhile, DAP as an electroactive substance creates a reduction peak current upon the electrochemical measurements. Interestingly, in the presence of PFOS, the POD activity of Cu@CuO aerogel is inhibited since the specific coordination between PFOS and Cu(II) can cover the active sites, resulting in the color of the sensing system becoming light and the peak current of DAP decreasing. This innovative dual-mode detection method showed excellent electrochemical detection of PFOS in the concentration range 10.0 ~ 1125.0 nM with a limit of detection (LOD) as low as 3.3 nM and a LOD of 20.8 nM in the colorimetric detection in the range 62.3 ~ 875 nM. Furthermore, the sensor was successfully used for the analysis of real samples with an RSD value ≤ 6.5%. The successful application of this two-mode sensing method for the determination of PFOS holds promise for the detection of other contaminants in the future. Graphical Abstract
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高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 6
·1-10
·
IF 5.3
Zhong Yujun,Li Zhiyang,Zhang Anlin,Peng Yuqing,Zhou Hao,Wang Bin,Xie Lianwu,Guo Yaping
A novel electrochemical sensor, MIP/Cu-MOF/rGO/AuNPs/GCE, was developed by depositing gold nanoparticles, coating Cu-MOF/GO on the surface of glassy carbon electrode (GCE) before electroreducing graphene oxide (GO) to rGO and covering molecularly imprinted membrane by electropolymerization for highly sensitive detection of electroneutral organophosphorus pesticide residues in agricultural product. Cyclic voltammetry, differential pulse voltametry, scanning electron microscopy, energy-dispersive spectroscopy, and atomic force microscopy were used to characterize the imprinted sensor. Several key factors such as chitosan concentration, suspension volume, pH of polymerization solution, and polymerization scanning rate during preparation of the imprinted sensor were optimized in detail. When electroneutral phosmet was used as a template, the linear range of MIP/Cu-MOF/rGO/AuNPs/GCE for detecting phosmet was 1.00 × 10 −14 –5.00 × 10 −7 mol/L with the limit of detection of 7.20 × 10 −15 mol/L at working potentials of − 0.2 to 0.6 V. The selectivity, reproducibility, and repeatability of MIP/Cu-MOF/rGO/AuNPs/GCE were all acceptable. The recoveries of this method for determining phosmet in real samples ranged from 94.2 to 106.5%. The MIP/Cu-MOF/rGO/AuNPs/GCE sensor could be applied to detect electroneutral pesticide residues in organisms and agricultural products. Graphical Abstract
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高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 192
·期 1
·1-13
·
IF 5.3
Liu Junjie,Wu Shengxi,Zhang Lu,Zhang Mingjun,Wu Haotian,Shi Miwan,Weng Yuan,Ye Wenqiao,Gu Kui
A novel proposal is introduced with an unlabeled electrochemical immunosensor for the detection of tumor broad-spectrum biomarker vascular endothelial growth factor (VEGF165) Copper-based metal organic frameworks (Cu MOFs)-carbon nanotubes (MWCNTs) were employed as its substrates, functionalized with methylene blue (MB) for signal enhancement. Cu-MOFs-MWCNTs nanocomposites were synthesized successfully via a solvothermal method and were then deposited on the surface of a glassy carbon electrode (GCE), with the addition of methylene blue to amplify the signal. Due to the expansive specific surface area provided by the carbon nanotubes and the amino groups facilitated by the metal–organic framework nanomaterials, the anti-VEGF165 monoclonal antibody was immobilized on the electrochemical immunosensor through covalent bonding, which could bind specifically to VEGF165, thereby causing a detectable change in the current. The developed immunosensor exhibited a linear detection range for VEGF165 spanning from 1 to 100,000 pg/ml, with the R 2 value of 0.997 by differential pulse voltammetry (DPV) method, and the limit of detection was as low as 0.9686. Additionally, the electrochemical immunosensor presented commendable selectivity, availability, and reproducibility, along with an effective capacity for detecting VEGF165 in clinical samples. Consequently, the immunosensor is expected to revolutionize early screening for VEGF165-related diseases, which offer a promising, cost-effective, and precise diagnostic tool for clinical utility. Graphical
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 8
·1-11
·
IF 5.3
Tong Yanli,Chen Meng,Huang Xing,Xu Yuzhi,Zhang Lang,Yu Zhenning,Liu Si-Yang,Dai Zong
Detecting lipopolysaccharide (LPS) using electrochemical methods is significant because of their exceptional sensitivity, simplicity, and user-friendliness. Two-dimensional metal–organic framework (2D-MOF) that merges the benefits of MOF and 2D nanostructure has exhibited remarkable performance in constructing electrochemical sensors, notably surpassing traditional 3D-MOFs. In this study, Cu[tetrakis(4-carboxylphenyl)porphyrin] (Cu-TCPP) and Cu(tetrahydroxyquinone) (Cu-THQ) 2D nanosheets were synthesized and applied on a glassy carbon electrode (GCE). The 2D-MOF nanosheets, which serve as supporting layers, exhibit improved electron transfer and electronic conductivity characteristics. Subsequently, the modified electrode was subjected to electrodeposition with Au nanostructures, resulting in the formation of Au/Cu-TCPP/GCE and Au/Cu-THQ/GCE. Notably, the Au/Cu-THQ/GCE demonstrated superior electrochemical activity because of the 2D morphology, redox ligand, dense Cu sites, and improved deposition of flower-like Au nanostructure based on Cu-THQ. The electron transfer specific surface area was increased by the improved deposition of Au nanostructures, which facilitates enriched binding of LPS aptamer and significantly improved the detection performance of Apt/Au/Cu-THQ/GCE electrochemical aptasensor. The limit of detection for LPS reached 0.15 fg/mL with a linear range of 1 fg/mL − 100 pg/mL. The proposed aptasensor demonstrated the ability to detect LPS in serum samples with satisfactory accuracy, indicating significant potential for clinical diagnosis. Graphical Abstract
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ChemSusChem
·
2024
·
IF 7.5
Qiuping Zhou,Xinyuan Jiang,Xuecheng Zhang,Dawei Wang,Guang Yang,He Zhou,Yuchao Wu,Fang Guo,Ming Chen,Guowang Diao,Lubin Ni
Graphical A Polyoxomolybdate-based metal-organic framework-derived Cu-embedded molybdenum dioxide hybrid nanoparticles was first applied as sulfur host in aluminum-sulfur batteries to resolve remaining critical challenge of polysulfide shuttle effect. The pouch cell with Cu/MoO 2 @C cathode cycled at 100 mA g −1 exhibits an initial discharge capacity of 150 mAh g −1 and maintains 100 cycles. High-performance rechargeable aluminum-sulfur batteries (RASB) have great potential for various applications owing to their high theoretical capacity, abundant sulfur resources, and good safety. Nevertheless, the practical application of RASB still faces several challenges, including the polysulfide shuttle phenomenon and low sulfur utilization efficiency. Here, we first developed a synergistic copper heterogeneous metal oxide MoO 2 derived from polymolybdate-based metal-organic framework as an efficient catalyst for mitigating polysulfide diffusion. This composite enhances sulfur utilization and electrical conductivity of the cathode. DFT calculations and experimental results reveal the catalyst Cu/MoO 2 @C not only effectively anchors aluminum polysulfides (AlPSs) to mitigate the shuttle effect, but also significantly promotes the catalytic conversion of AlPSs on the sulfur cathode side during charging and discharging. The unique nanostructure contains abundant electrocatalytic active sites of oxide nanoparticles and Cu clusters, resulting in excellent electrochemical performance. Consequently, the established RASB exhibits an initial capacity of 875 mAh g −1 at 500 mA g −1 and maintains a capacity of 967 mAh g −1 even at a high temperature of 50 °C.
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EUROPEAN POLYMER JOURNAL
·
2024
·
IF 5.8
Lingshan Li,Qian Zhou,Jingyi Zhao,Yuangong Zhang,Zhaolei Jia,Xuan Liu,Hailei Zhang,Xinwu Ba,Libin Bai
Multiblock copolymer macrochain-transfer agents (MBP-CTAs) can be used to synthesize MBPs in one pot via reversible addition-fragmentation chain-transfer (RAFT) polymerization. MBP-CTAs can be efficiently synthesized via a copper-catalyzed azide-alkyne cycloaddition reaction. However, traditional purification methods cannot sufficiently purify MBP-CTAs, resulting in the failure of RAFT. In this study, it was discovered that using a supported catalytic system, namely, Cu@A-HNTs, inhibited the connection between Cu and S. The residual Cu content in the MBP-CTA was successfully reduced to a low level (7.88 µg/mg). Then, hydrophilic and hydrophobic MBPs were synthesized through RAFT polymerization using the MBP-CTAs. Subsequently, multiblock copoly(methyl methacrylate-b-butyl methacrylate-CTA)s (PMMA-b-PBMA-c-CTA)s were successfully prepared. The MBP-CTAs and MBPs were characterized using ultraviolet–visible spectroscopy, 1 H nuclear magnetic resonance, size-exclusion chromatography, matrix-assisted laser desorption/ionization-time-of-flight mass spectrometry, differential scanning calorimetry measurements and uniaxial tensile tests. The results of performance testing of PMMA-b-PBMA-c-CTAs demonstrated that their fracture stress and strain significantly increased comparing with that of PMMA-b-CTAs.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zeyun Yang,Hao Guo,Zhiguo Yu,Mingyue Wang,Xiaoqin Wei,Zongyan Lu,Lei Sun,Henglong Ren,Wu Yang
As a vital biological polypeptide molecule, glutathione (GSH) is involved in the regulation of various life activities. Accurate and sensitive detection of GSH in human body is of great significance for the preliminary diagnosis of related diseases. In this research, Cu(II) modified TADH COF, which has been prepared by Cu 2+ post-synthesis modification of the COF obtained through a condensation reaction of 1,3,5-(4-aminophenyl) benzene (TAPB) and 2,5-dihydroxy-1,4-benzenedicarboxaldehyde (DHTP), and methylene blue (MB) molecules are combined to construct a ratiometric electrochemical sensor for achieving specific and ultra-sensitive detection of GSH. As a stable and active covalent organic framework material, TADH COF possesses the special O(–OH) and N(C N) binding sites, which can load and coordinate with Cu 2+ effectively. The obtained Cu(II)-TADH COF serves as a sensitive electrode material for sensing GSH due to “extrusion effect” caused CuCl solid-state electrochemical signal degeneration by the specific binding of Cu and GSH while MB provides a stable electrical signal in the electrochemical sensing process as an internal reference for eliminating errors and making the detection results more accurate. The constructed electrochemical sensing platform Cu(II)-TADH COF/MB/GCE exhibited an ultrahigh sensitivity with a limit of detection (LOD) of 0.0093 nM (S/N = 3), wide linear range of 0.05 nM–40 μM and high accuracy. For the detection of GSH in real samples including human blood, serum and urine samples, the sensor also showed excellent sensing performance. This is the first research on ratiometric electrochemical sensing platform for the ultra-sensitive detection of glutathione based on covalent organic frameworks, which provides an original and novel strategy for the electrochemical detection of GSH with COF materials.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2024
·Vol. 149
·期 12
·6007-6019
·
IF 3
Li Haijian,Chen Chao,Xu Yi,Qin Zhao,Xie Xiao,Yao Ergang,Xu Siyu,Qu Wengang,Yi Jianhua,Zhao Fengqi
The intense exhaust plumes of the CMDB propellants can be suppressed by the containing potassium salts, but the potassium compounds increased remarkably the combustion pressure exponent of propellants, destroying the combustion plateau effects and resulting in the combustion instability of the rocket motors, so it is critical to reveal the reaction mechanisms of the potassium salts during the combustion process of propellants. In the work, the influence of three potassium hexanitro complexes, K 2 Pb[ M (NO 2 ) 6 ] ( M = Co, Cu, Ni), on the ignition and combustion properties, especially pressure exponent, of solid propellants has been investigated by using the laser ignition apparatus, burning rate instrument, combustion wave temperature, flame morphology, quenched surface, and emission spectrometer. When the hexanitro complexes replaced the β -Pb, the ignition delay time of the propellants was shorter at the low laser flux. The study on the combustion properties showed that the burning rate and pressure exponent of propellant containing K 2 Pb[Cu(NO 2 ) 6 ] was extremely close to the basic propellant ( β -Pb) due to similar temperature gradient until ~ 1942 °C. The flat combustion cross section on the flame morphology of the propellant containing K 2 Pb[Cu(NO 2 ) 6 ] was found to favor the low-pressure exponent. The carbon skeleton, metal agglomerations, and K release identified by using the quenched surface and emission spectra were closely related to the response characteristics of the combustion pressure exponent of the propellants due to the influence of different hexanitro complexes. The relationship between the burning rate of the propellants and the maximum self-heating rate of the mixtures containing the propellant energetic oxides and hexanitro complexes was also revealed, which can predict the relative burning rate for the same propellant system. More importantly, the reasons for the deterioration of the combustion pressure components due to flash suppressors were elucidated clearly from the experimental results and theoretical analysis, which involve three destroying mechanisms: (i) catalytic metals “poison,” (ii) carbon skeleton disappearance, and (iii) high thermal decomposition temperature of potassium compounds. The study also revealed the inhibition mechanism of potassium flash suppressors on the catalytic properties of catalysts during the combustion process of the CMDB propellants. Graphical abstract The influence of three potassium hexanitro complexes on the ignition and combustion properties of solid propellants have been investigated, and the reasons for the deterioration of the combustion pressure components due to flash suppressors were elucidated clearly.
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