Molecular Catalysis
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2018
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IF 0
Zhanao Lv,Cholho Choe,Yunfeng Wu,Haibin Wang,Zhuqi Chen,Guangxing Li,Guochuan Yin
This work demonstrates a novel strategy that the introduction of non-redox metal ions as Lewis acids to the classic dinuclear manganese complex [Mn IV 2 (μ-O) 3 (Me 3 tacn) 2 ](PF 6 ) 2 can greatly promote the alkene epoxidation efficiency under mild conditions with H 2 O 2 as the solely terminal oxidant because of its economic and environmental advantages. When [Mn IV 2 (μ-O) 3 (Me 3 tacn) 2 ](PF 6 ) 2 was used as the catalyst in the absence of Lewis acids, only 16.4% conversion of cyclooctene with 6.2% yield of epoxide was obtained and the obvious decomposition of H 2 O 2 was observed. However, the oxygen transfer efficiency of the catalyst was sharply improved with 100% conversion and 90.2% yield of epoxide under identical conditions when the non-redox metal ion, such as Sc 3+ , was introduced to the catalytic system. The novel strategy was successfully applied to the epoxidation reactions of different types of alkenes. Through UV–vis, FT-IR, EPR and CV characterizations, it was evidenced that the non-redox metal ions with high positive charge as Lewis acids could dissociate the sluggish dinuclear Mn-(μ-O) 3 -Mn core and the open-loop dinuclear manganese complex, HO-Mn III -(μ-O)-Mn IV = O or O = Mn IV -(μ-O)-Mn IV = O, was proposed as the active species, which was capable of the alkene epoxidation process. This work illustrated an alternative protocol to manipulate the reactivity of those sluggish catalysts by the introduction of non-redox metal ions and provided clues to understand the role of non-redox metal ions in metalloenzymes and heterogeneous catalysts.
研究领域:
化学
·
催化科学
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DOI
MOLECULES
·
2015
·Vol. 20
·期 9
·16709-16722
·
IF 2.416
Hai-Min Shen,Wen-Jie Zhou,Xin Ma,Hong-Ke Wu,Wu-Bin Yu,Ning Ai,Hong-Bing Ji,Hong-Xin Shi,Yuan-Bin She
A pH-dependence of the Brønsted acid-catalyzed oxidation of sulfides to the corresponding sulfoxides with H2O2is reported for the first time based on our systematic investigation of the catalytic performance of a series of Brønsted acids. For all of the Brønsted acids investigated, the catalytic performances do not depend on the catalyst loading (mol ratio of Brønsted acid to substrate), but rather depend on the pH value of the aqueous reaction solution. All of them can give more than 98% conversion and selectivity in their aqueous solution at pH 1.30, no matter how much the catalyst loading is and what the Brønsted acid is. This pH-dependence principle is a very novel perspective to understand the Brønsted-acid catalysis system compared with our common understanding of the subject.Keywords:sulfide;oxidation;sulfoxide;pH-dependence;Brønsted acid
研究领域:
化学
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催化科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Li He,Cuiqing Yu,Qiuyu Feng,Aimin Wu,Yunchun Li,Xianxiang Wang
Developing intelligent antibacterial platforms that dynamically modulate therapeutic activities in response to microenvironmental cues is essential to overcome the self-limiting nature and collateral oxidative damage of conventional chemodynamic therapy (CDT). Herein, a multifunctional and self-adaptive nanozyme platform, denoted as CuPDA@CaO 2 @Qu, is developed. It rationally integrates a copper-based metal-organic gel (CuPDA) for pH-dependent enzyme-mimetic switching, calcium peroxide (CaO 2 ) for endogenous hydrogen peroxide (H 2 O 2 ) self-supply, and the natural flavonoid quercetin (Qu) to reinforce anti-inflammatory and antioxidant functions, collectively enabling synergistic and stage-programmed therapy of infected wounds. Specifically, in acidic infected microenvironments, the peroxidase-mimic CuPDA catalyzes CaO 2 -derived H 2 O 2 into highly toxic hydroxyl radical (·OH), effectively disrupting biofilms and eradicating multidrug-resistant (MDR) bacteria, with enhanced efficacy through glutathione depletion. After bacterial clearance, CuPDA self-switches to antioxidant mode, exhibiting superoxide dismutase-glutathione peroxidase mimetic activities that synergize with Qu to scavenge excess reactive oxygen species (ROS), resolve inflammation, and promote M2 macrophage polarization. Moreover, the nanocomposite is capable of promoting cellular migration, collagen deposition, and neovascularization, significantly accelerating tissue healing. This self-adaptive platform demonstrates potent efficacy in MDR bacterial-infected wounds and offers a promising strategy for intelligent nanomedicine design.
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高影响因子
FUEL
·
2022
·
IF 8.035
Zhaoyang Qi,Huaifang Li,Jie Chen,Changshen Ye,Ting Qiu
The carboxyl functionalized ionic liquid ([mim(CH 2 ) 3 COOH]Cl) was prepared as a linker to combine phosphotungstic acid (HPW) and Zr(IV) ion. The obtained [mim(CH 2 ) 3 COO] 3 PW-Zr composite acted as a heterogeneous catalyst for removing DBT from liquid fuel with H 2 O 2 as an oxidant. As a result, [mim(CH 2 ) 3 COO] 3 PW-Zr possessed high catalytic activity in extractive and catalytic oxidative desulfurization (ECODS). Moreover, the [mim(CH 2 ) 3 COO] 3 PW-Zr was further exploited to grow on the surface of PEI/silica gel. And the fabricated large-grained Zr-PWIL@PEI/silica gel was used in the continuous ECODS process, and the removal of DBT could still reach more than 95% after running continuously for 16 h. More importantly, the synergistic catalytic mechanism between HPW and Zr(IV) in the ECODS process has been investigated in detail by experiments and DFT calculations. As a result, a plausible mechanism has been proposed and verified, which contains two parts: the Lewis acidic center activating H 2 O 2 to form superoxide ion radicals ( OOH), and the OOH oxidizing HPW to peroxotungstate (W(O 2 ) n ), which has a high oxidizability and stability. Thus, the effective combination of Zr(IV) and HPW active sites is a very effective strategy to promote desulfurization efficiency and utilization efficiency of H 2 O 2 . Besides, we also found the distance between the corresponding active sites of catalysts plays an essential role in ECODS reaction as it strongly influences the synergistic effect between different active sites.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2014
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IF 3.209
Ben Qi,Lan-Lan Lou,Yanbing Wang,Kai Yu,Ying Yang,Shuangxi Liu
Manganese containing mesoporous materials Mn-MCM-41 were prepared by template-ion exchange (TIE), in situ reduction (ISR), direct hydrothermal (DHT) and wetness impregnation (WI) methods. The samples were characterized by XRD , N 2 adsorption–desorption, HR-TEM, TG, UV–Vis, H 2 -TPR and ESR techniques, which illustrated that the definite structure of the MCM-41 was retained after introducing Mn into MCM-41 by different method. The catalytic activity and selectivity of the Mn-MCM-41 in the epoxidation of styrene with 30% H 2 O 2 as an oxidant agent were explored. The TIE catalysts showed the highest activity but Mn 2+ was leached during the reaction. The ISR catalysts exhibited high activity for epoxidation of styrene. Furthermore, recycling studies proved the ISR catalysts as heterogeneous catalysts , which did not lose the catalytic activity after four recycles appreciably. However, the DHT and WI catalysts showed poor performance in the catalytic epoxidation of styrene. Various parameters such as different reaction molar ratio of H 2 O 2 /styrene, catalyst amount, and kinds of solvents were studied to optimize the reaction conditions.
研究领域:
催化化学
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材料化学
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有机合成
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多相催化
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环境友好氧化过程
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DOI
高影响因子
Journal of Nano Research
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2017
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IF 0.511
Wen Juan Dong,Ji Yan Han,Xin Wu,Li Fan,Wen Ting Liang
A novel near-infrared fluorescence quenching method has been developed for the determination of hydrogen peroxide based on N-acetyl-L-cysteine-capped gold nanoparticles (NAC-AuNPs) as a fluorescence probe. The prepared gold nanoparticles with the size of about 1.91 nm exhibited strong near-infrared fluorescence emission at 693 nm with excitation wavelength at 450 nm in aqueous solution. The fluorescence intensity of NAC-AuNPs was quenched dramatically by adding hydrogen peroxide. Therefore, it could be used to detect hydrogen peroxide based on the fluorescence quenching intensity was linear with the concentration of hydrogen peroxide. Under the optimal experimental conditions, the linear range and detection limit were 1.0×10-6 –3.0×10-2 mol/L and 1.0×10-7 mol/L, respectively. The possible quenching mechanism was investigated by time-resolved fluorescence spectroscopy. The proposed method was simple, sensitive and showed good repeatability and stability.
研究领域:
分析化学
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生物医学工程
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纳米技术
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DOI
高影响因子
ChemPlusChem
·
2026
·Vol. 91
·期 8
·e70223
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IF 3.1
Huan V Doan,Huong T T Tran,Duyen T Le,Xuan N Pham
In this study, a novel Ni–MoO 3 @MIL‐101(Cr) composite catalyst was synthesized via a one‐step hydrothermal method for the oxidative desulfurization (ODS) of dibenzothiophene (DBT). The catalyst combines the high specific surface area of MIL‐101(Cr) with the redox properties of Ni–MoO 3 , providing an effective synergy between adsorption and catalytic oxidation. The incorporation of Ni as a promoter significantly enhances catalytic activity, enabling complete sulfur removal (∼100%) under mild conditions (50 °C) within 60 min. Structural characterizations (scanning electron microscopy, X‐ray diffraction, and SAED) reveal that the catalyst retains its nanosheet–nanorod morphology and crystalline MoO 3 phase after repeated use, with only a slight decrease in the crystallinity of the MIL‐101(Cr) framework. Mechanistic analyses using X‐ray photoelectron spectroscopy, Raman, and temperature‐programmed reduction demonstrate that surface oxygen vacancies and Lewis acid sites promote ODS activity, while highly dispersed Ni–MoO 3 species facilitate H 2 O 2 activation and Mo 6+ /Mo 5+ redox cycling, leading to efficient generation of reactive oxygen species. The catalyst also exhibits excellent stability, maintaining 98.7% DBT conversion after five cycles. These results demonstrate that the strong Ni–Mo synergistic effect and efficient oxygen activation make Ni–MoO 3 @MIL‐101(Cr) a robust and highly efficient catalyst for deep fuel desulfurization. This study presents a significant advancement in the field of oxidative desulfurization by developing a synergistic Ni–MoO 3 redox catalytic system confined within the porous MIL‐101(Cr) framework. Unlike conventional catalysts, the designed material effectively enhances H 2 O 2 activation through cooperative interactions between Ni and Mo species, enabling rapid and ultra‐deep removal of refractory sulfur compounds under mild conditions. The integration of redox‐active sites with a high‐surface‐area MOF support not only improves catalytic efficiency but also ensures excellent stability and recyclability. This work provides new insights into the rational design of bimetallic catalysts for green fuel purification and offers a promising strategy for achieving sustainable and energy‐efficient desulfurization processes.
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PubMed
高影响因子
Nanomaterials
·
2026
·Vol. 16
·期 16
·984
·
IF 4.8
Yangfan Du,Guanglong Jing,Keyi Han,Xin Zhang,Liang Hou,Yong Li
The global demand for hydrogen peroxide (H2O2) continues to increase, and photocatalytic H2O2production is regarded as a promising alternative technology due to its mild, safe, and environmentally friendly characteristics. ZnIn2S4has demonstrated promising application potential in photocatalytic H2O2production owing to its unique two-dimensional layered structure and broad spectral response. However, its performance is severely limited by rapid charge recombination and sluggish charge migration. To address this challenge, a ZnIn2S4/C3N4S-scheme heterojunction was successfully constructed via a simple oil-bath method by assembling ZnIn2S4nanoflowers on C3N4nanosheets. Systematic structural characterizations and performance evaluations demonstrate that the construction of the S-scheme heterojunction effectively promotes the spatial separation and surface migration of photogenerated charge carriers, thereby significantly enhancing photocatalytic activity. Under optimal conditions, the ZIS/CN-10 sample (C3N4to ZnIn2S4mass ratio of 10%) achieves the highest photocatalytic H2O2production rate of 825.8 μmol g−1h−1. This work provides new insights and theoretical guidance for the rational design of efficient and stable ZnIn2S4-based photocatalysts.
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高影响因子
ACTA PHYSICO-CHIMICA SINICA
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2026
·
IF 13.5
Yanyan Zhao,Jing Zhang,Xiaolong Li,Hailun Su,Lin Yang,Jianjun Zhang
A stable Py-HOF was prepared by employing H 4 TBAPy as precursor. • A TiO 2 /Py-HOF composite with excellent photocatalytic activity was constructed. • T/Py-HOF shows stability due to strong H-bonds and π–π interactions of H 4 TBAPy. • S-scheme charge transfer pathway was verified via ISI-XPS, fs-TAS, and DFT. • T/Py-HOF display good photocatalytic H 2 O 2 production yield and sterilization. Hydrogen-bonded organic frameworks (HOFs) hold substantial potential for application in photocatalysis. However, their practical application in photocatalytic H 2 O 2 generation and antibacterial activity remains hampered by intrinsically inefficient electron-hole separation and inadequate structural stability. Herein, a Py-HOF photocatalyst was prepared by employing 1,3,6,8-tetrakis (p-benzoic acid) pyrene (H 4 TBAPy) as precursor via self-assembly method, and the titanium dioxide/Hydrogen-bonded organic framework (TiO 2 /Py-HOF, T/Py-HOF) S-scheme heterojunction was rationally fabricated via an in-situ synthesis. Due to the strong hydrogen bonds and π–π interactions of H 4 TBAPy, the T/Py-HOF S-scheme heterojunction displays super stability. Furthermore, in-situ irradiated XPS, femtosecond transient absorption spectroscopy, and DFT calculations verify the S-scheme carrier migration mechanism within the T/Py-HOF heterojunction. Thanks to the ultrafast charge-transfer and excellent redox ability of the T/Py-HOF S-scheme photocatalyst, the optimally formulated T/Py-HOF-5% achieves a remarkable H 2 O 2 production rate of 1890 μmol g −1 h −1 , corresponding to approximately 15.24 and 6.19-fold enhancements compare to the pure TiO 2 and bare Py-HOF, respectively, along with excellent stability. Furthermore, the T/Py-HOF heterojunction also exhibits superior photocatalytic sterilization activity against Escherichia coli (E. coli) , achieving almost 100% of E. coli inactivation after 90 min light irradiation. Collectively, this work offers a novel insight for designing high-efficiency HOF-based S-scheme photocatalysts in energy and environment applications. A novel TiO 2 /Py-HOF S-scheme heterojunction was fabricated for efficient photocatalytic H 2 O 2 production and excellent photocatalytic E. coli sterilization. Download: Download high-res image (202KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Xuedong Zhang,Lele Ni,Mustafa Evren Ersahin,Hale Ozgun,Guoshuai Liu
Synergistic microenvironment enables low-energy electro-Fenton SMZ degradation. • Amino-CNT site enhances oxygen utilization and FeN 5 boosts •OH generation. • Stable SMZ removal over 20 cycles and across pH 3–11 and real water matrices. The practical effectiveness of the electro-Fenton (EF) technology is severely constrained by sluggish oxygen mass transport and inefficient activation of hydrogen peroxide (H 2 O 2 ). Herein, a synergistic catalytic microenvironment was constructed by integrating a biomimetic FeN 5 single-atom nanozyme with an amino-functionalized carbon nanotube support (CNT−NH 2 ) to overcome these dual challenges. Experimental and theoretical results reveal that the −NH 2 groups on CNT−NH 2 induce a local oxygen-enriched interface, significantly enhancing oxygen (O 2 ) supply and promoting the 2e − oxygen reduction reaction (2e − ORR) for efficient in situ H 2 O 2 generation. Simultaneously, the FeN 5 sites facilitate hydroxyl radical (•OH) production by mimicking peroxidase activity, thereby lowering the activation energy for O−O bond cleavage in H 2 O 2 . The resultant FeN 5 −CNT−NH 2 EF system achieves complete degradation of sulfamethoxazole (100% in 45 min) with a remarkably low specific energy consumption (0.0235 kWh g −1 TOC), and demonstrates excellent stability and broad applicability in complex water matrices. This work provides a novel perspective for constructing high-performance EF process through synergistic microenvironment engineering. Download: Download high-res image (144KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Linhai Sun,Jianhong Hu,Busheng Wang,Baoxin Ge,Pengyang Jiang,Yuqi Zeng,Caijin Huang,Kaining Ding
Regional topological regulation of charge transport and proton-transfer dynamics. • Acid-free photoinduced self-protonation and cooperative proton transfer. • Catalytic and preparative validation of the proposed strategy. The inherent trade-off between electron transport efficiency and proton transfer dynamics in COFs is a fundamental limitation for its application in photocatalysis. Herein, we report a regionalized topology engineering strategy that molecularly programs the stoichiometric ratio and regional arrangement of imine and hydrazone linkages within DABH-COF, thereby coordinating charge transport and proton-transfer kinetics. This tailored structure enables photo-triggered protonation under visible light, whereby dynamic imine bonds undergo in-situ protonation to create a proton-rich microenvironment that favors the 2e − ORR, while adjacent hydrazone bonds facilitate rapid proton transfer through a hydrogen-bond network. DFT calculations show that this cooperative effect lowers the free-energy requirement for *OOH formation from 0.26 to 0.20 eV during the 2e − ORR, thereby favoring electron–proton transfer. Moreover, the achievement of gram-scale synthesis (1.2 g) of highly crystalline DABH-COF addresses scalability challenges in COF production. DABH-COF exhibits a superior visible-light-driven H 2 O 2 -production rate of 4340 μmol g −1 h −1 without any sacrificial agents and an AQY of 12.4% (420 nm). This study provides a way for constructing effective COF-based photocatalysts through regional topology engineering. Through regionalized topology engineering, the imine and hydrazone bonds are molecularly programmed by monomer connectivity within DABH-COF, which enables in-situ protonation and synergistical electron–proton dynamics for high-performance photocatalysis. Download: Download high-res image (159KB) Download: Download full-size image
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高影响因子
Biomedicines
·
2026
·Vol. 14
·期 9
·2015
·
IF 4.5
Junkai Zhao,Mengting Xie,Jianghao Yu,Ran Yan,Yue Wang
Background/Objectives: Thrombotic cardiovascular diseases remain a major cause of morbidity and mortality worldwide. Current antithrombotic therapies are limited by insufficient thrombus targeting. This study aimed to develop a fibrin-binding peptide-functionalized, hydrogen peroxide (H2O2)-responsive polymeric micelle and to evaluate its physicochemical properties and biological effects under H2O2-induced endothelial oxidative stress and preliminary FeCl3-induced thrombosis conditions.Methods: A fibrin-binding peptide, P2 (VTFIKC), was screened using computer-aided drug design and evaluated through microscale thermophoresis and in vitro thrombus adhesion assays. An all-trans retinoic acid (atRA)-based boronate ester prodrug, BORA, was synthesized to enable H2O2-triggered degradation and drug release. BORA was co-assembled with P2-modified Mal-PEG-b-PAsp to prepare P2-Mal-PEG-b-PAsp/BORA micelles. Their physicochemical properties, H2O2responsiveness, H2O2-scavenging activity, cytocompatibility, cytoprotective effects, anti-inflammatory activity, and preliminary in vivo efficacy were evaluated.Results: The resulting micelles exhibited a suitable nanoscale size, acceptable cytocompatibility, H2O2-responsive changes in particle size distribution, and concentration-dependent H2O2-scavenging activity. In H2O2-stimulated human umbilical vein endothelial cells, micelle treatment was associated with improved cell viability, lower intracellular ROS-associated fluorescence, and reduced TNF-α and IL-1β concentrations. In a FeCl3-induced rat carotid artery thrombosis model, P2-Mal-PEG-b-PAsp/BORA micelles altered platelet- and leukocyte-related hematological indices and exhibited preferential accumulation in the thrombotic carotid artery.Conclusions: P2-Mal-PEG-b-PAsp/BORA micelles combine P2-mediated fibrin-binding potential, H2O2-responsive release behavior, and H2O2-scavenging activity. The findings provide preliminary support for further investigation of this peptide-functionalized nanoplatform.
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高影响因子
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