APPLIED SURFACE SCIENCE
·
2021
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IF 6.707
Xin Jiang,Sanmei Liu,Wen Wang,Shunli Shi,Zhenxing Zeng,Chao Chen
Photocatlytic water disinfection for pathengenic miroorgasnisms removal is of great importance to public health safety, however the photocataltyic performance is unsatisfactory due to the low reactive oxygen species (ROS) generation. In this work, an innovative energy-transfer-mediated oxygen activation system on PCN-224-Zn is proposed for selective singlet oxygen generation without the need of electron-hole separation. The as-prepared PCN-224-Zn exhibits remarkable singlet triggered photocatalytic E-coli inactivation and organic pollutant degradation performance. The enhanced photocatalytic activity is attributed to the introduction of Zn into the metal-organic frameworks (MOFs) that facilitates the transformation of electron-hole couple from singlet to triplet state for selective singlet oxygen generation with high efficiency. This work provides a new oxygen activation pathway for efficient and selective ROS generation without the need of electron-hole separation.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Jing Zhang,Xiaojian Xu,Yue Qiang
An ultrasensitive electrochemical ochratoxin A (OTA) aptasensor was designed using AgPt bimetallic nanoparticles decorated iron-porphyrinic metal-organic framework (PCN-223-Fe) as electrochemical tracer. PCN-223-Fe was synthesized with zirconium ion as node and iron-porphyrin as linker, and in situ supported with PtAg bimetallic nanoparticles to obtain AgPt/PCN-223-Fe composite. Spindle-shaped AgPt/PCN-223-Fe was characterized by electron microscopies, X-ray diffraction and X-ray photoelectron spectroscopy. Due to the synergistic effect, AgPt/PCN-223-Fe modified electrode exhibited enhanced electrocatalytic activity to oxygen reduction. Sequentially, AgPt/PCN-223-Fe was combined with streptavidin (SA) to prepare electrochemical tracer. SA/AgPt/PCN-223-Fe introduced into the electrode surface capturing OTA aptamer through the recognition of biotin and streptavidin, which lead to a strong electrochemical signal from oxygen reduction. When OTA existed in solution, the aptamer was bonded with OTA preferentially, and electrochemical signal reduced. The proposed approach showed a wide linear range from 20 fg mL −1 to 2 ng mL −1 and a low detection limit of 14 fg mL −1 (S/N = 3). Meanwhile, the aptasensor showed good reproducibility, stability and selectivity, which was successfully applied for OTA detection in red wine and corn samples. This strategy broadens application of metal-organic frameworks, and could be used for other toxins detection.
研究领域:
分析化学
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食品安全
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材料科学
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环境科学
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Zixun Fang,Yao Zhou,Yang Yang,Yidong Hou,Can Yang,Jinshui Zhang
Artificial Z-scheme photocatalytic systems, inspired by natural photosynthesis, have been widely employed for pollutant removal. In this study, we fabricated a ternary Z-scheme Bi 2 O 3 /Bi/porous carbon nitride (PCN) heterojunction with an intimately coupled interface through a simple EG-assisted solvothermal approach to improving photocatalytic performance of NO oxidation. The in-situ generated metallic Bi acts as an electron mediator, effectively accelerating the separation and transfer of photoexcited carriers. The unique Z-scheme charge transfer mechanism provides the strong redox abilities and isolates the active sites for specific reactions, thus promoting photocatalytic NO oxidation activity. As a result, the optimized Bi 2 O 3 /Bi/PCN sample achieved a NO removal efficiency of 94.6%, outperforming single-component catalysts and most previously reported heterojunction-based photocatalysts. Additionally, in-situ Fourier transform infrared spectroscopy was employed to propose the NO removal mechanism, offering valuable insight into the conversion pathway. Such a heterogeneous Z-scheme photocatalytic system with a strong redox ability, high charge-separation efficiency, and long-term stability, demonstrates significantly enhanced photoactivity for pollutant removal and is expected to attract increasing interest for other photocatalytic applications.
研究领域:
环境科学
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材料科学
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光催化技术
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Min Xie,Qiaozhen Xu,Tao Lv,Hong Liu
The search for effective and highly selective photocatalysts for CO 2 transformation is exceptionally desirable yet challenging. Herein, a novel BiVO 4 @PCN-224(Cu) heterostructure was constructed by growing BiVO 4 nanosheets on the surface of PCN-224(Cu) rods for visible-light-driven CO 2 photoreduction. The obtained BiVO 4 @PCN-224(Cu) heterostructure could selectively reduce CO 2 into CO in the absence of sacrificial reagents. The CO yield over the optimized sample reached 70.5 μmol g −1 h −1 (corresponding to an apparent quantum yield of 0.42% at 450 nm), a 5.1-fold increase over pristine PCN-224(Cu). The boosted activity of the hybrid could be credited to the S-scheme heterojunction formed at the interface of PCN-224(Cu) and BiVO 4 , which facilitated the separation of photogenerated charges and ameliorated the redox capability. In-situ XPS and hydroxyl radical determination confirmed the S-scheme charge transfer mode. This study provides a new strategy for constructing S-scheme heterojunctions involving metalloporphyrin-based metal-organic frameworks for high-performance CO 2 conversion.
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Small
·
2023
·Vol. 19
·期 16
·2206124
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IF 13.3
Futing Yang,Wenjie Yu,Qiying Yu,Xiyu Liu,Chunping Liu,Chong Lu,Xinghua Liao,Yi Liu,Na Peng
The apoptosis-resistant mechanism of photodynamic therapy (PDT) usually results in limited therapeutic efficacy. The development of new strategies for sensitizing targeted ferroptosis that bypass apoptosis resistance is of great significance to improve the antitumor efficacy of PDT. In this study, a novel amphiphilic copolymer whose main chain contains reactive oxygen species (ROS)-responsive groups and the end of side chains contains triphenylphosphine is synthesized, to encapsulate porphyrinic metal–organic framework PCN-224 via self-assembly which are hydrothermally synthesized by coordination of zirconium (IV) with tetra-kis(4-caboxyphenyl) porphyrin, and loaded carbon monoxide releasing molecule 401 (CORM-401) by their hollow structures (PCN-CORM), and finally, surface-coated with hyaluronic acid. The nanosystem can sequentially localize to mitochondria which is an important target to induce apoptosis and ferroptosis in cancer cells. Upon excitation with near-infrared light, PCN-224 is activated to produce amounts of ROS, and simultaneously triggers the rapid intracellular release of CO. More importantly, the released CO can sensitize ferroptosis and promote apoptosis to significantly enhance the antitumor efficacy of PCN-224 both in vitro and in vivo. These results illustrate that the mitochondria-targeted drug delivery system combined PDT with CO leads to an effective antitumor efficacy, which maybe a promising way to enhance the treatment efficiency of PDT.
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ACS Applied Energy Materials
·
2018
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IF 0
Bao-Xia Dong,She-Liang Qian,Fan-Yan Bu,Yi-Chen Wu,Li-Gang Feng,Yun-Lei Teng,Wen-Long Liu,Zong-Wei Li
Heterogeneous electrocatalysis provides better control of the chemical surroundings of the catalyst’s active site for improved performance, offers the possibility of overcoming drawbacks of deactivation caused by aggregation or dimerization in homogeneous condition, and permits the use of benign aqueous solutions. Employing metal–organic frameworks (MOFs) or covalent–organic frameworks (COFs) to support the active molecular catalyst of porphyrin for electrochemical conversion of CO2 to CO is a promising strategy. We have rationally introduced a 3D highly stable porphyrin-based MOF of PCN-222(Fe) into heterogeneous catalysis through the simple dip-coating method. The composite catalyst PCN-222(Fe)/C (mass ratio = 1:2) exhibited high catalytic performance for electrochemical conversion of CO2 to CO with 494 mV overpotential (where j = 1.2 mA cm–2) and maximum 91% FECO in a CO2-saturated 0.5 M KHCO3 aqueous solution, achieving a TOF of 0.336 site–1 s–1. The catalyst was found to retain its crystallinity and stability after 10 h of electrolysis at −0.60 V versus RHE (average FECO 80.4%; RHE, reversible hydrogen electrode), which generates 334 μmol of CO with the TOF of 0.012 s–1 (0.286 site–1 s–1). These results indicate that the PCN-222(Fe)/C has a substantial catalytic effect on the electrochemical reduction of CO2 due to the combination of the intrinsic activity of the porphyrin molecule, and the promising CO2 adsorption ability endowed by the conserved porosity, as well as the high conductivity of carbon black.
研究领域:
电化学
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催化
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材料科学
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环境化学
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Journal of Environmental Chemical Engineering
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2025
·
IF 7.2
Mengyao Gui,Hongwei Yang,Erming Ouyang
Polystyrene nanoplastics (NPs), ubiquitous contaminants in aquatic ecosystems, are known to impede conventional anoxic denitrification processes. However, their effects on aerobic denitrification systems remained poorly understood. This study systematically elucidates the mechanistic interactions between polystyrene NPs and aerobic denitrification performance. Results revealed polystyrene NPs caused concentration-dependent suppression of denitrification efficiency in the aerobic denitrifier Pseudomonas stutzeri PCN-1 under controlled laboratory conditions (aerobic, 30 ℃). At NPs concentrations escalating from 100 to 1000 μg L⁻¹ , nitrate removal rates decreased markedly (0.4–3.3 mg L⁻¹ h⁻¹), paralleled by progressive accumulation of nitrite (8.8–87.2 mg L⁻¹) and N₂O (31.2–58.3 mg L⁻¹). Mechanistic analyses revealed that polystyrene NPs induced biotoxic effects through two primary pathways: (1) disruption of cellular membrane integrity and (2) excessive generation of reactive oxygen species (ROS), collectively impairing bacterial viability and metabolic activity. Furthermore, critical denitrification processes were compromised, including diminished electron transport system activity, reduced catalytic activities of key denitrification enzymes, and downregulation in transcriptional expression of functional genes (e.g. napA , nirS , cnorB , and nosZ ). These multilevel inhibitions collectively contributed to the observed deterioration in nitrogen removal capacity. This investigation provides novel insights into the ecotoxicological risks posed by NPs to microbial nitrogen cycling in aquatic environments.
研究领域:
环境微生物学
·
生态毒理学
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高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Xuejiao Tang,Xiujie Peng,Haitao Liao,Xiaoying Zeng,Xiaoying Zhang,Yu Zhu,Chao Weng,Ping Shen
The rational development of the third component is the key to obtaining highly efficient ternary organic solar cells (OSCs). In this contribution, one tetracyanobutadiene-functionalized small molecule, IDT-T-PCN, featuring a noncoplanar molecular backbone, is selected and employed as a third component to construct PM6:Y6:IDT-T-PCN ternary OSCs. Results demonstrate that IDT-T-PCN exhibits complementary absorption and cascade energy-level alignment with the host materials (PM6 and Y6), which are beneficial for improving light-capture capability and charge transfer properties. Absorption spectra and contact angle measurements reveal that there is good compatibility and strong interaction between IDT-T-PCN and Y6, which can affect the crystallization and molecular aggregation of the host materials, especially Y6. The morphology, structure, and formation kinetics characterizations of the active layer film have unveiled that IDT-T-PCN plays a critical role in optimizing phase separation and morphology, modulating molecular aggregation, and enhancing crystallization and orderly molecular stacking of the ternary blend. Therefore, the ternary OSCs exhibit improved charge dissociation and collection probability, enhanced charge transport, and reduced charge recombination, leading to improvements in all photovoltaic parameters. Specially, the ternary OSCs incorporated with IDT-T-PCN achieve a decent PCE of 17.36%, which is obviously higher than that of the host PM6:Y6 binary device (PCE = 15.84%) owing to the simultaneous increase of VOC, JSC, and FF. This work highlights the role of careful material selection and design of the third component with the aim of optimizing device physics processes, crystallinity, and morphology of the blend film, ultimately realizing high-performance ternary OSCs.
研究领域:
材料科学
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有机电子学
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光伏技术
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高分子科学
·
纳米技术
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Yuling Chen,Wei Huang,Chendi Wang,Xinyu Zhai,Ting Zhang,Yang Wang,Xiaoya Hu
Metalloporphyrinic frameworks have demonstrated to be an alternative candidate for natural enzymes due to their diverse structures and unique peroxidase-mimicking properties. In this study, a manganese–metalloporphyrin framework (PCN-222(Mn)) was synthesized as a biomimetic metal–organic framework (MOF). This catalyst exhibited highly intrinsic peroxidase-like activity with 3,3′,5,5′-tetramethylbenzidine as the chromogenic substrate. Additionally, a higher peroxidase-like activity was observed in a wider pH range (from 3.0 to 8.0), which is undoubtedly advantageous for PCN-222(Mn) to detect H2O2 under physiological and pathological environments. Based on the excellent peroxidase-mimicking activities of PCN-222(Mn), a novel hydrogen peroxide (H2O2) nonenzymic amperometric biosensor was constructed through electro-polymerizing a conductive and stable poly-glutamic acid (PGA) film on the surface of a PCN-222(Mn)-modified electrode (PGA/PCN-222(Mn)/GCE). Resulting from the synergistic activity of PCN-222(Mn) and PGA film, a sensitive, selective, and reliable method was established for H2O2 detection with a linear range of 5 × 10–7 to 1.01 × 10–3 mol/L and detection limit of 3.1 × 10–8 mol/L. In addition, PGA/PCN-222(Mn) has a long-term stability and can be used over 90 cycles without any decrease in analytical performance. These outstanding performances of the developed approach in sensitive and selective determination of H2O2 from human serum provides effective proof for its potential application in monitoring low-abundance H2O2 from complicated biological samples. This research not only expands the electrochemical applications of metalloporphyrin frameworks but also demonstrates a promising strategy for increasing the conductivity and stability of MOF-based electrode materials.
研究领域:
生物化学
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分析化学
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材料科学
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高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
·
IF 7.926
Jinjuan Xue,Meng Yuan,Jiamin Gao,Zewu Zhang,Mingxin Wang,Shuaishuai Ma
In this work, a novel PCN-222 metal−organic framework based multitasking membrane was developed for separation of emulsified oils as well as photo-Fenton degradation of refractory aromatic pollutants and inactivation of pathogenic bacteria in water. Fe(III)@PCN-222 nanorods were prepared via impregnation method and subjected to amino-modification, and then robustly anchored on polydopamine (PDA) decorated PVDF membrane via catechol-amine reaction. The as-prepared N-Fe(III)@PCN-222/PDA/PVDF composite membrane exhibited underwater superoleophobicity, and showed high separation efficiency (above 99.4 %) as well as relatively favorable permeation flux (874.9–1592.3 Lm −2 h −1 ) in the separation of emulsified oils ranged from nanoscale to microscale from water. Meanwhile, the membrane serving as a recyclable photo-Fenton platform showed an extensive degradation capacity towards aromatic contaminants and high inactivation activity against bacteria under visible light. The grafted Fe(III) is used as an electron acceptor to promote the separation of photo-generated charge carriers, adjusted the band structure to shorten the bandgap value, and can be reduced to Fe(II) by photo-generated electrons as a Fenton-like catalyst. The photo-Fenton mechanism was studied in detail from the aspects of photoelectric properties, band structure and reactive oxygen species . This work could promote the application of PCN subclass MOFs based superwetting membrane as a recyclable platform for complex wastewater treatment .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Zheng Wang,Hui Li,Chuang Jiang,Wenya Liu,Siyu Zhang,Yibin Zhou,Kang Liu,Yaqing Xiao,Ruyan Hou,Xiaochun Wan,Yingnan Liu
Herein, a novel dual-mode probe for organophosphorus pesticides (OPs) colorimetric and photothermal detection was developed based on manganese modified porphyrin metal–organic framework (PCN-224-Mn). PCN-224-Mn had excellent oxidase-like activity and oxidized colorless 3,3,5,5-tetramethylbenzidine (TMB) to blue–green oxidation state TMB (oxTMB), which exhibited high temperature under near-infrared irradiation. l -ascorbate-2-phosphate was hydrolyzed by acid phosphatase to produce ascorbic acid, which weakened colorimetric and photothermal signals by impacting oxTMB generation. The presence of OPs blocked the production of ascorbic acid by irreversibly inhibiting the activity of acid phosphatase, causing the restoration of chromogenic reaction and the increase of temperature. Under the optimal conditions, the probe showed a good linear response to OPs in the concentration range of 5 ∼ 10000 ng/mL, using glyphosate as the analog. The detection limits of glyphosate in colorimetric mode and photothermal mode were 1.47 ng/mL and 2.00 ng/mL, respectively. The probe was successfully used for sensitive identification of OPs residues in tea, brown rice, and wheat flour. This work proposes a simple and reliable colorimetric/photothermal platform for OPs identification, which overcomes the problem that single-mode detection probes are susceptible to external factors, and has broad application potential in the field of food safety.
研究领域:
分析化学
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环境科学
·
食品科学
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DOI
PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Xin-Yue Wang,Yi-Ming Gu,Xu-Peng Zong,Sheng-Sheng Zhao,Shu-Dong Wang
The inevitable combustion of fossil fuels in human industrial activities results in significant greenhouse gas emissions, leading to the pressing challenge of CO 2 /N 2 separation in humid flue gas. Iron-based Metal-organic frameworks (MOFs) have proven to be cheap, robust against water vapor attack due to the enhanced coordination bonds. In this study, we present two distinct MOFs i.e., DNL-9(Fe) and PCN-233(FeM II ), constructed by Fe clusters and 2,5-furandicarboxylic acid ligands. Static adsorption experiments revealed that DNL-9(Fe), featuring an exclusive Fe-F-Fe spiral packing structure, exhibited higher surface areas and enhanced CO 2 adsorption performance that outcompeted PCN-233 candidates. DNL-9(Fe) demonstrated a high IAST selectivity of CO 2 /N 2 at 247 (15/85, v/v, P/P 0 = 0.01), superior to the most of state-of-the-art Fe-MOFs reported up to date. The further theoretical calculations elucidated the binding sites of the framework with CO 2 molecules. Importantly, DNL-9(Fe) showed sufficient water stability and cyclic separation, as confirmed by dynamic breakthrough tests, indicating it as a promising candidate for practical CO 2 capture from humid flue gas.
研究领域:
化学
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材料科学
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环境科学
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高影响因子
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