MATERIALS SCIENCE & ENGINEERING R-REPORTS
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2024
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IF 31.6
Jun Li,Xiangmei Liu,Chaofeng Wang,Yufeng Zheng,Zhenduo Cui,Zhaoyang Li,Shengli Zhu,Hui Jiang,Yu Zhang,Paul K. Chu,Shuilin Wu
The deep-seated drug-resistant bacterial infection is one of the most noticeable public-health threat owing to poor drug therapeutic effect, high recurrence, and devastating complication. Herein, we propose a bactericidal strategy of bio-heterointerface charging through ultrasound-boosted bacterial extracellular and intracellular electron transfer for eradicating implant-related drug-resistant bacterial infection, where a TiO 2 -modified porphyrin-based two-dimensional metal-organic framework (2DMOF-TiO 2 ) is selected as a sonosensitizer. The ultrasound-boosted extracellular and intracellular electron transfer between methicillin-resistant Staphylococcus aureus and 2DMOF-TiO 2 induces rapid reactive oxygen species (ROS) burst surrounding bacterial outer and inner, contributing to intracellular oxidation, membrane potential decrease (∼5 mV), membrane disruption, and pyrimidine metabolism disorder, thus causing bacterial death. The in vivo results of 2DMOF-TiO 2 implant exhibit rapid sonocatalytic anti-infection and enhanced osseointegration at bone-implant interface. This platform may inspire the universal thinking about ultrasound-boosted extracellular and intracellular electron-transfer-induced ROS and provide a superior therapeutic candidate for various deep-seated infectious diseases.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Huan Zheng,Yingnan Guo,Xiaoyu Hao,Yin Zhang,Jialong Yu,Bangmin Zhang,Li Guan,Xu Li,Xiaolei Huang,Fenghe Wang
Designing high-performance, cost-effective, and durable electrocatalysts for hydrogen evolution reactions is essential and challenging. The design of electrode surface architecture to accomplish rapid gas bubble release is a promising strategy. Herein, we design a unique network-structured catalyst by constructing NiFe alloy on a submicron carbon fiber network substrate (NiFe/SCFN). The unique structure imparts superaerophobicity to NiFe/SCFN and facilitates gas bubbles removal, thereby accelerating mass transfer. Benefiting from electrode alloying, the hydrogen adsorption free energy was reduced to − 0.026 eV (Fe sites) and 0.077 eV (Ni sites) on the catalyst surface, improving the electronic conductivity. NiFe/SCFN achieves low overpotentials of 19.2 mV and 199 mV at 10 mA∙cm −2 and 100 mA∙cm −2 with excellent stability, owing to the unique network structure and the NiFe alloy's electronic structure. This work provides a new strategy for designing effective catalysts with transition metals.
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Journal of Materials Chemistry C
·
2025
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IF 5.1
Shenghao Wang,Yajuan Wang,Linbo Cao,Jiasheng Zhang,Yuqing Liu,Bo Wang,Mingmin Li
Utilisation of highly efficient catalysts for photo-Fenton-like reactions, although challenging, is urgently desired to alleviate the serious global burden caused by organic pollutants. In this work, an example of two-dimensional (2D) porphyrin (TCPP) MOF arrays vertically grown on a copper foam (CF) was synthesized under hydrothermal conditions. The honeycomb-like structure offers a large surface area and capacious porous space for fast mass transfer and enrichment of organic pollutants. The highly dispersed active site (M–N4) of nanosheet arrays promotes the utilization of visible light to generate and separate photoelectrons and holes. In addition, the photocatalytic efficiency was further strengthened by the introduction of bimetallic sites. The macro-integrated structure can be conveniently recovered for cyclic catalysis, thus reducing costs and avoiding secondary pollution. These features together permit the self-supported 2D TCPP-MOF array's remarkable performance in persistent mineralization of various organic pollutants with different surface charges owing to the production of reactive oxygen species (ROS). This study provides a general method to rationally design and optimize photo-Fenton-like catalytic performance based on 2D MOFs for water remediation.
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ANALYST
·
2024
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IF 3.6
Fengyao Yu,Longyue Qin,Hua Zhang,Longshua Qin,Hao Fan
In this study, we innovatively synthesized bipyridine ruthenium cluster nanosheets (RuMOFNCs), a novel metal–organic framework material that exhibits both fluorescence and electrochemiluminescence. Gold nanoparticles (AuNPs) were anchored onto RuMOFNCs via bipyridine chelation, enhancing optical signals and creating sites for attaching biologically functional probes. We employed tetraferrocene-modified DNA probes, linked via gold–sulfur (Au–S) bonds, to construct a dual-mode fluorescence–electrochemiluminescence biosensor. This sensor, exploiting exonuclease III (Exo III)-mediated cyclic amplification, inhibits the electron transfer from RuMOFNC to tetraferrocene, resulting in amplified fluorescence and electrochemiluminescence signals. The sensor demonstrates exceptional sensitivity for detecting the BRAF gene, with fluorescence and electrochemiluminescence detection limits of 10.3 aM (range: 0.1 fM to 1 nM) and 3.1 aM (range: 1 aM to 10 pM), respectively. These capabilities are attributed to RuMOFNCs’ luminescence properties, tetraferrocene's quenching effect, and the specificity of base pairing. This study's findings hold substantial promise for biomedical research and clinical diagnostics, particularly in precision medicine and early disease detection.
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PubMed
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BIOSENSORS & BIOELECTRONICS
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2024
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IF 10.7
Jingyu Hou,Jun Wang,Jiawen Han,Juan Wang,Daiyong Chao,Qing Dong,Daoqing Fan,Shaojun Dong
As the well-known test-indicator for early prostate cancer (PCa), sarcosine (SA) is closely related to the differential pathological process, which makes its accurate determination increasingly significant. Herein, we for the first time expanded the peroxidase (POD)-like property of facile-synthesized Zn-TCPP(Fe) MOF to fluorescent substrates and exploited it to ratiometric fluorescent (RF) sensing. By harnessing the effective catalytic oxidation of MOF nanozyme toward two fluorescent substrates (Scopoletin, SC; Amplex Red, AR) with contrary changes, and target-responsive (SA + SOx)/MOF/(SC + AR) tandem catalytic reaction, we constructed the first MOF nanozyme-based RF sensor for the quantitative determination of SA. Superior to previous works, the operation of this RF sensor is under the guidance of AND-(ANDˆNAND) contrary logic circuit. The dual-channel binary output changes (from 1/0 to 0/1) not only enable the intelligent logical recognition of SA, bringing strengthened reliability and accuracy, but also manifest the proof-of-concept discrimination of PCa individuals and healthy ones. Through recording the fluorescence alterations of SC (F 465 ) and AR (F 585 ), two segments of linear relationships between ratiometric values (F 585 /F 465 ) and varied contents of SA are realized successfully. The LOD for SA could reach to as low as 39.98 nM, which outperforms all nanozyme-originated SA sensors reported till now. Moreover, this sensor also demonstrates high selectivity and satisfactory performance in human serum samples. Furthermore, the portable sensing of SA is realized under the assistance of smartphone-based RGB analysis, demonstrating the potential of point-of-care diagnostics of PCa in the future.
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FUEL
·
2024
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IF 6.7
Chongchong Chen,Hexiang Gao,Hui Li,Mingchao Wang,Jie Zhang,Tengfei Li,Wenjia Wu,Zhirong Yang,Jingtao Wang
The poor water-stability and cross-layer proton transfer property pose a challenge to the lamellar metal–organic frameworks (MOFs) membrane when acting as a promising proton exchange membrane. Herein, we report an adipic acid-mediated strategy to improve the water-stability and the cross-layer proton conductivity of CuTCPP lamellar MOF membrane, which achieves a maximum power density and current density of 112.6 mW cm −2 and 424.4 mA cm −2 , respectively. Adipic acid with extra functional groups (–PO 3 H 2 , –COOH) stably bridges the adjacent crystal layers via the terminal carboxylic acid anchoring Cu sites. In particular, the extra functional groups introduced into the adipic acid regulate the allocation of hydrogen bonding networks in an umbrella-shape around adipic acid with copper-porphyrin structures as external margin, enriching the coherence of hydrogen bonding network on the proton transport path. Benefiting from the regular pore structure of MOF, the optimized hydrogen bonding networks in adjacent crystal layers construct a more abundant through-plane transfer pathway. The resultant through-plane proton conductivities of CuTCPP-PO 3 H 2 /–COOH membranes are up to 108/89 mS cm −1 at 80 °C and 100 % RH, which is ∼ 6-fold higher than that of the pristine CuTCPP membrane (13 mS cm −1 ), with a conductivity attenuation of < 5 % during a humidity cycling test for 12 times.
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VACUUM
·
2025
·
IF 3.9
Jinlu Yang,Tianyi Zhang,Silong Wang,Shengsi Wang,Hongyuan Ding,Jianghui Xie,Dengji Xu,Que Huang,Changcheng Liu
The electrospinning technique not only encapsulates the phase change material (PCM) within a fibrous matrix, thereby preventing its leakage, but also addresses the application limitations associated with graphitic carbon (GC) containing carbonized zeolitic imidazolate framework-67 (ZIF-67). In this study, we prepared flexible nanocomposite fiber membranes using the electrospinning technique. The fibrous membranes exhibit both the excellent thermal management capabilities inherent to phase change materials and the low thermal conductivity characteristic of thermal insulation materials. This phenomenon can be attributed to the fibrous membranes' reliance on molecular chain vibrations and the thermal energy transfer facilitated by gases within the free volume, which makes heat transfer more challenging in these membranes. Conversely, the incorporation of GC enhances the thermal stability and photothermal conversion capabilities of the fibrous membranes. In the simulated heat retention experiment, the fibrous membranes display superior heat preservation performance, and the differential scanning calorimetry (DSC) test reveals that these membranes possess enhanced heat storage capacity. The excellent heat storage and thermal insulation capabilities of the fibrous membranes suggest promising applications in the thermal insulation domain.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Qianqian Xing,Xiaoliang Jia,Shiyu Jia,Yongqin Qi,Yuqi Wang,Yingxiong Wang,Xianglin Hou
The traditional synthesis methods of cyclopropyl methyl ketone (CPMK) have some disadvantages such as low yield, slow reaction rate and unclear catalytic mechanism. To solve these problems, a new strategy is developed to synthesize CPMK from 5‑chloro-2-pentanone (CPE) using 1,8-diazabicyclo[5.4.0]undec‑7-ene (DBU). Experiment results show that the yield of CPMK reached a maximum of 96.5 % in DBU at 40 °C for 30min. The mechanism study shows that the hydrogen bond between DBU and CPE is the key to drive the deprotonation and cyclization of CPE. The hydrogen bond is formed between the N atom on C = N of DBU and the α-H on the methylene group associated with the carbonyl group on CPE. The catalyst DBU is converted into [DBUH] + Cl − , which can be reclaimed and recycled completely. The density functional theory (DFT) calculation confirmed the existence of molecular hydrogen bonds and proved that the hydrogen bond driving force is the key to the reaction. The hydrogen bond driven mechanism provides a new idea for the basic research of cyclization reaction.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Binxuan Diao,Chenhao Cong,Fenglin Sun,Hongjiang Li,Haoran Zhang,Xuhao Wang,Mingliang Jin,Sooman Lim,Xinlin Li,Se Hyun Kim
The self-stacking propensity of metal–organic frameworks (MOFs) during synthesis, combined with their intrinsic limitations in electrical conductivity and mechanical stability, constrains their utility as high-capacity energy sources in wearable electronics. Here, we employ a surfactant-assisted method to mitigate the Z-axis stacking of zinc metalloporphyrin organic frameworks (NMOFs), yielding ultrathin two-dimensional (2D) material sheets. By integrating carboxyl multiwalled carbon nanotubes into these nanosheets (denoted as C-NMOF-x), the lamellar structure of MOF is preserved while promoting the formation of rich multistage micropores and continuous conductive channels. This structural refinement remarkably enhances electrochemical properties, including capacitance, electronic conductivity, and cycling stability. Leveraging synergistic interactions, the resulting C-NMOF-4 composite achieves a specific capacitance of 0.152 mAh/g in a three-electrode system at a current density of 1 A/g. Furthermore, the modulated C-NMOF-4 composites are successfully formulated into homogeneous e-inks suitable for dispensing printing, enabling the mass production of flexible micro-supercapacitors (MSCs). Notably, these MSCs maintain 95 % of their capacitance even after 180° bending under wearable conditions. This surface and interface microstructure modulation strategy holds promise for enhancing the synergistic coupling effects of 2D materials and offers new avenues for the application of innovative 2D materials in wearable electronics.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
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IF 5.8
Chenxuan Xie,Mingzhe Li,Ziyu Ling,Xiaofen Wang,Yuzhen Lv,Kepi Chen
Highly efficient and stable electrocatalysts toward hydrogen evolution reaction (HER) under large current density are essential for alkaline water splitting. Herein, an active and durable CoMoO 4 -based HER electrocatalyst is developed, with a coupling of surface phosphorization and polypyrrole (PPy) modification to accelerate water dissociation and prevent alkaline corrosion during HER process, ensuring great catalyst stability. The prepared PPy-CoMoO 4 /P@NF catalyst achieves perfect HER activity with only 242.1 mV overpotential at the industrial current density of 1000 mA·cm −2 in 1.0 M KOH as well as a low Tafel slope of 39.0 mV dec −1 . Moreover, PPy modification greatly inhibits the alkaline corrosion and the catalyst exhibits stable operation for 100 h at 1000 mA·cm −2 with a conservation rate of 98.5 %. Electrochemical tests and theoretical calculations reveal that the multiple interfaces formed by CoMoO 4 /CoP/PPy significantly reduce the energy barrier of hydrolysis and improve the interfacial adsorption of H ads . Meanwhile, the surface phosphating changes the Gibbs free energy of rate-determining step (RDS) from −0.54 to −0.29 eV, optimizing the energy barriers for hydrogen adsorption-desorption. Remarkably, an electrolyzer with PPy-CoMoO 4 /P @NF as cathode catalyst only needs a cell voltage of 1.92 V at 1000 mA cm −2 for overall water splitting. This study provides an effective way to develop highly efficient and stable HER catalysts toward industrial water splitting.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
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IF 7.7
Lingnan Kong,Quanhua Xie,Yuanyuan He,Shiyu Dong,Yang Liu,Wenliang Fan,Haiyan Yao,Mingfu Zhao,Nianbing Zhong
This paper proposes a polyvinyl alcohol/AlFFIVE-1-Ni (PVA/KAUST-8)-coated long-period fiber grating (LPFG) SO 2 concentration sensor to accurately monitor SO 2 concentrations online. To enhance the adhesion strength between the fiber and a SO 2 -sensitive film, the etched LPFG surface was silanized using 3-aminopropyltriethoxysilane, and then coated with a PVA/KAUST-8 SO 2 -sensitive sol using the doctor blading method. A fluorosilane hydrophobic coating was deposited on the SO 2 -sensitive membrane surface and integrated with a LPFG temperature sensor, thereby effectively eliminating measurement interference caused by ambient temperature and humidity fluctuations during SO 2 concentration detection. The morphology and composition of the SO 2 -sensitive films were characterized using optical microscopy, field-emission scanning electron microscopy, X-ray diffraction analysis, and X-ray photoelectron spectroscopy. Furthermore, the working principle of the sensors for the detection of SO 2 was established. Under optimized parameters (LPFG diameter: 60 μm; PVA doping in PVA/KAUST-8: 12 wt%; SO 2 -sensitive film: 45 μm; fluorosilane composite layers: 12) within a humidity range of 0–60 % RH and a temperature range of 25–45 °C, the sensor demonstrated a good selective SO 2 detection with 2.79 pm/ppm sensitivity, 1.07 ppm detection limit, 390 s response time, and 8.89 % maximum relative error.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Xu Guangyuan,Peng Xingjie,Wu Chuanqiang,Xi Shibo,Xiang Huixin,Feng Lei,Liu Zhendong,Duan Yi,Gan Lijin,Chen Si,Kong Yuan,Ma Yanzhe,Nie Fujing,Zhao Jie,Hai Xiao,Wei Wei,Zhou Meng,Wang Tianfu,Yao Chuanhao,Zhou Wu,Yan Huan
CO 2 electroreduction to CO promises to give an efficient strategy for CO 2 fixation and transformation. However, current reported active sites fail to deliver sufficient activity with high CO Faradic efficiency (FEco) over a wide range of potential. Here, we show a general synthetic protocol to fabricate a batch of highly pure and active NiN 2 catalysts with precise engineering of the uniform-large ( UL ) vacancy around the active sites, which is accomplished through the ‘pre-deposition + pyrolysis’ of various atomically precise Ni clusters (Ni n ) and in-situ etching of the support by the ‘nano bomb’ (sulfur-ligand in the clusters). The NiN 2 sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h −1 with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN 2 site with UL vacancy contributes to this remarkable catalytic performance compared to the counterparts. This general synthetic strategy enables us to simultaneously engineer active sites and surrounding vacancies with the employment of atomically precise metal clusters, thereby enhancing catalytic performance for other specific reactions.
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