APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Shuangshuang Liu,Rui Zhao,Zhen Lu,Linxi Hou
Artificial photosynthesis of hydrogen peroxide (H 2 O 2 ) via conjugated microporous polymer (CMP) as photocatalysts offers a promising path for solar-to-chemical energy conversion. However, the rapid recombination of photogenerated carriers and the sluggish reaction kinetics during CMP photocatalysis still remains a challenge. As a crucial strategy for regulating the pore microenvironments and charge-transfer pathways, the linkage chemistry of CMP provides a critical handle to address these limitations. Herein, three different linkages structure of CMPs with acylhydrazine (TFBE-TD), sp 2 -carbon (TFBE-PDAN) and imine (TFBE-PA) were designed as photocatalysts to elucidate the structures-performance relationships for H 2 O 2 production from water and air, without sacrificial agents. Compared with TFBE-PA, TFBE-TD and TFBE-PDAN exhibit 5.7 times and 4 times higher H 2 O 2 generation rates in pure water, respectively. This enhancement is due to the effective reinforcement of the photogenerated electron delocalization by the acylhydrazine and the sp 2 -carbon linkage structure, facilitating the electron transfer process. Furthermore, DFT calculations reveal that by adjusting the linkage structure of CMPs, the adsorption capacity of O 2 can be effectively enhanced and the reaction activation energy can be reduced, thereby promoting the ORR pathway for efficient photosynthetic H 2 O 2 production. This work establishes linkage chemistry as a key design principle for high-performance CMP photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Da-Wei Wang,Ming-Yue Tian,Fang-Qi Wang,Xi-Wen He,Wen-You Li,Yu-Kui Zhang
Chemodynamic therapy (CDT) is an emerging treatment strategy that kills tumor cells by generating hydroxyl radicals (·OH) via the activation of Fenton/Fenton-like reactions within the tumor microenvironment (TME). Although CDT overcomes drug resistance issues and has minimal side effects, it still faces multiple challenges including low endogenous hydrogen peroxide (H 2 O 2 ) levels, inadequate catalytic efficiency, and targeting issues. To overcome these limitations, a novel precision-targeted responsive molecularly imprinted nanozyme (GZMIP) was developed. Using zeolitic imidazolate framework-8 (ZIF-8)-coated glucose oxidase (GOx) as a carrier (GZ) and the epitope of lactate transporter (MCT4) as the template, an imprinted layer was prepared on the GZ surface via radical polymerization reactions, followed by elution to obtain GZMIP. GZMIP targeted tumor cells with overexpressed MCT4. Upon entering cells, GZMIP occurred responsive cleavage in the acidic environment and GSH overexpressed TME, releasing GOx and copper(II) acrylate (CuA) monomers from the imprinted layer. GOx catalyzed intracellular glucose (Glu) to generate H 2 O 2 , while GSH reduced CuA to Cu + . The subsequent cascade reaction between Cu + and H 2 O 2 generated highly toxic ·OH, inducing cell death. Both in vitro and in vivo experiments demonstrated that GZMIP effectively inhibited tumor cell proliferation, showed a 75 ± 5 % growth inhibition rate in tumor-bearing mouse models, and exhibited excellent biocompatibility. This study innovatively integrated molecular imprinted polymers with nanozyme technology to establish a Fenton-like cascade catalytic system, simultaneously achieving precise delivery and controlled release of catalytic components. This approach significantly improving tumor targeting and therapeutic efficacy, providing a promising strategy for enhanced CDT.
研究领域:
纳米医学
·
癌症治疗
·
生物无机化学
·
药物递送
·
活性氧生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Fengyi Wang,Hong Li,Shenshen Zhang,Bin Duan,Niu Huang,Yong Zheng,Binbin Jia,Siran Xu,Wei Liu,Liqun Ye
The development of non-noble metal catalysts with high activity and selectivity is critical for the electrocatalytic production of hydrogen peroxide (H 2 O 2 ). Herein, we report a composite catalyst (CTF/BHN) fabricated by chelating a basic bismuth salt (BHN) with a bipyridine-containing covalent triazine framework (CTF), forming strong Bi-bipyridine bonds at the interface. This catalyst exhibits exceptional H 2 O 2 selectivity (92–98 %) over a wide potential range (0.3–0.62 V vs. RHE). In H-type cell tests, it achieves a Faraday efficiency of 88.9 % at 20 mA cm −2 , with a high H 2 O 2 production rate of 1.65 mol g −1 h −1 , and maintains stable performance for 42 h. In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and X-ray photoelectron spectroscopy (XPS) reveal that the superior performance stems from synergistic interfacial effects: electron transfer from BHN to CTF enhances charge transport, while polarized interfaces promote water dissociation and protonation of pyridine groups in CTF to form Py*H intermediates. Py*H acts as a proton relay, facilitating the protonation of adsorbed *O 2 to *OOH at Bi active sites. Concurrently, the enhanced interaction between *OOH and the catalyst surface (evidenced by the blue-shifted *OOH peak) stabilizes *OOH and suppresses its dissociation, thereby driving the 2e − ORR pathway for efficient H 2 O 2 generation.
研究领域:
电催化
·
能源化学
·
材料化学
·
环境化学
·
分子催化
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Xingjiang Liu,Long He,Liu Yang,Yani Geng,Lei Yang,Xiangzhi Song
A highly sensitive and selective fluorescence probe for H 2 O 2 has been developed based on an iminocoumarin derivative using aromatic boronic ester as sensing unit. A significant fluorescence enhancement was observed with λ max em = 619 nm when this probe was treated with H 2 O 2 . In the detection of H 2 O 2 , this probe exhibited a large Stokes shift (148 nm) and a low detection limit (6.0 × 10 −8 mol/L). Furthermore, cell imaging studies had revealed that this probe had the potential to detect intracellular H 2 O 2 in living cells.
✓ 已验证
DOI
高影响因子
Journal of the Iranian Chemical Society
·
2023
·Vol. 20
·期 11
·2703-2712
·
IF 2.4
Zhang Chenglu,Nie Shiru,Ding Yanwei,Liu Chang,Zhang Yanpeng,Zhang Yang,Guo Jinghao
An “off–on–off” fluorescent probe NapEb for high selectivity and reversible response to H 2 O 2 and GSH was synthesized. Inspired by the role of GSH in the human body, the –Se–N– bond in ebselen was successfully used as the recognition site. The probe NapEb is sensitive (LOD = 8.4 µM) and fast for H 2 O 2 (within 200 s). It can be used not only for qualitative and quantitative detection of H 2 O 2 in real samples, but also has been successfully used for the imaging detection of H 2 O 2 in MCF-7 cells with good effect. Moreover, continuous fluorescence recognition of GSH has also achieved significant results, the process is reversible and can be repeated for 5 times. The experimental results show that satisfactory results can also be obtained by structural modification at the 3-position of naphthalimide.
研究领域:
生物化学
·
分析化学
·
医学检测
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 15
·2899-2911
·
IF 7.571
Zhi Li,Changning Xue,Lifen Zhang,Yuman Zhang,Yao Yu,Qianrui Liu,XinHong Guo,ZhenZhong Zhang
Oxidative stress can lead to a variety of diseases, and oxalate bonds can consume excess reactive oxygen species (ROS) in cells. In this study, a H2O2-responsive prodrug-nanosystem was synthesized using oxalate-bond-connecting water-soluble drugs (Tre) with a fluorescent indicator (PBI). The maximum fluorescence emission wavelength of PBI–Tre was at 548 nm, and the changes of nanoparticles could be directly observed in the cells. PBI–Tre was coated with hyaluronic acid (HA) to improve their intracellular uptake and ability to target macrophages. The particle size of HA–PBI–Tre was 200–300 nm, and the zeta potential was −36.9 mV. The results showed that the nano-drug loading system could easily decrease the ROS level, inhibit the production of inflammatory factors, remove the accumulation of lipids in foam cells. These nanoparticles could hinder foaming progress in the RAW264. 7 cell line.
研究领域:
纳米技术
·
药学
·
细胞生物学
·
炎症研究
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Zhaoyang Wang,Yuehua Shi,Yu Shi,Jiahe Zhang,Ran Hao,Gangwan Zhang,Leyong Zeng
Tumor microenvironment (TME) responsive chemodynamic therapy (CDT) showed an important application in inhibiting tumor growth by producing the highly toxic hydroxyl radical (·OH), but insufficient hydrogen peroxide (H2O2) and overexpressed glutathione (GSH) limited its application. Herein, by integrating photothermal therapy (PTT) and CDT, a new kind of mesoporous polydopamine (MPDA)-based cascade-reaction nanoplatform (MPDA@AuNPs-Cu) was designed for enhanced antitumor therapy, in which ultrasmall gold nanoparticles (AuNPs) with glucose oxidase (GOx)-like activity were deposited on MPDA for providing H2O2, and Cu2+ was chelated for GSH-responsive Fenton-like reaction. It was demonstrated that the MPDA@AuNPs-Cu nanoprobe showed high photothermal conversion efficiency and excellent biocompatibility. Moreover, the MPDA@AuNPs-Cu nanoprobe exhibited strong ·OH generation because of H2O2 self-generation and photothermal stimulation. Importantly, compared with MPDA-Cu, MPDA@AuNPs-Cu exhibited enhanced in vitro and in vivo CDT/PTT performance, by which the tumor growth was completely inhibited, achieving TME-responsive antitumor efficacy.
研究领域:
纳米技术
·
癌症治疗
·
生物医学工程
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Mengzhao Jiao,Zhengjun Li,Xianglai Li,Zijie Zhang,Qipeng Yuan,Frank Vriesekoop,Hao Liang,Juewen Liu
Self-inactivation of oxidases due to by-product hydrogen peroxide (H 2 O 2 ) is a main obstacle to applying these enzymes in chemical production. Herein, we report an efficient cascade strategy of co-immobilizing a natural oxidase and catalase-mimicking coordination nanoparticles. Fe 3+ and adenosine monophosphate (AMP) formed coordination nanoparticles with comparable performance as natural catalase at ambient conditions for degrading H 2 O 2 , but the former still maintained about 90% or 75% catalytic activity after pH 2.0 or 90 °C treatment, respectively. Upon polymerization with a few acrylic monomers, glycolic acid oxidase (GyAO) was co-immobilized with Fe 3+ /AMP within a nanogel. Benefiting from the confinement and protection effect of the nanogel, the catalytic activity increased by 5-fold at pH 4, and 10-fold at 80 °C, and the catalytic activity of the nanogel still retained more than 65% after recycling 20 times. More importantly, the tolerance of the nanogel to glycolic acid enhanced 100 times compared with the free GyAO enzyme. This study has expanded the application of nanozymes to industrial catalysis, where harsh conditions are expected.
研究领域:
生物化学
·
工业酶学
·
纳米材料科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ting Li,Zikai Wang,Zexin Zhang,Kun Feng,Jianru Liang,Dianzhan Wang,Lixiang Zhou
Spontaneous generation of H 2 O 2 and activation in heterogeneous Fenton is a promising technology for waste-water treatment. Here organic carbon modified Fe 3 O 4 /schwertmannite (Fe 3 O 4 /Sch/OC) by introducing Fe 3 O 4 in the Acidithiobacillus ferrooxidans -driven Fe 2+ oxidation process to give catalysts. In-situ H 2 O 2 could be generated via Fe 3 O 4 /Sch/OC-driven oxygen reduction reaction (ORR), moreover, the in-situ H 2 O 2 was disintegrated to produce •OH in Fe 3 O 4 /Sch/OC-driven Fenton reaction to degrade the methylene blue (MB). The catalysts were characterized by XRD , SEM, BET and XPS spectroscopy. Oxygen-containing functional groups (e.g., C = O, –COOH, –OH) on Fe 3 O 4 /Sch/OC surface could provide more active sites for the adsorption and reduction of O 2 . The carbon-modification promoted both the selectivity of 2e − ORR and Fe 2+ content of catalyst. Thus, Fe 3 O 4 /Sch/OC exhibited a higher H 2 O 2 selectivity (~65%) and MB degradation efficiency (~81%) than Sch, Fe 3 O 4 , or Fe 3 O 4 /Sch. In addition, in-situ H 2 O 2 could be produced at a wide initial pH range (3–9). The degradation pathways of MB were also proposed based on theoretically calculated and LC-MS data. The finding opens up a new way for developing a cost-effective Sch-based catalyst for producing in-situ H 2 O 2 and degrading pollutants.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2021
·
IF 9.297
Jing Su,Tao Lyu,Mick Cooper,Robert J.G. Mortimer,Gang Pan
Arsenic (As) is a toxic contaminant in surface waters and groundwater. Oxidation of arsenite (As(III)) to less toxic arsenate (As(V)) by hydrogen peroxide (H 2 O 2 ) is desirable for enhancing the immobilisation of Arsenic (As). However, this As(III) oxidation process is constrained by the strong pH dependence and the generated As(V) must also be removed for complete As remediation. This study developed and evaluated a novel heterogeneous catalytic system using manganese-doped Lanthanum oxycarbonate (MnL) to catalyse the oxidation of As(III) by H 2 O 2 and simultaneously adsorb the generated As(V). The presence of MnL enhanced the removal rate of As(III) by 35 times compared with systems utilising H 2 O 2 alone. Additionally, this superior performance was observed over a wide pH range (5–9), which demonstrated this approach could bypass the well-known pH restriction on oxidation by H 2 O 2 . Mechanistic studies revealed that the long-lived superoxide radicals (·O 2 − /·OOH), present on the particle surfaces and derived from the dissociation of the Lewis acid-base adduct (La–OOH*), were the dominant active species for As(III) oxidation. Mn atoms with low valence states played a crucial role in As(III) oxidation through the provision of extra active sites to facilitate radical production. The La and Mn sites in MnL could rapidly immobilize the generated As(V) by forming precipitates, resulting in a final As removal efficiency of 99% even after three cycles of reutilisation. Overall, this study demonstrates the viability of the proposed novel multi-functional catalyst for efficient As remediation from aqueous environments .
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Zhe Yang,Chao Shan,Yuchen Mei,Zhao Jiang,Xiaohong Guan,Bingcai Pan
This study demonstrates a simple method to prepare zero valent iron (ZVI)-based agent (prtZVI) with outstanding reducing power via pretreating ZVI with H 2 O 2 /HCl. Characterization of the prtZVI system with 57 Fe Mössbauer spectroscopy, XRD, TEM and chemical analysis indicates that it is a well dispersed system, containing nanosized solids such as ZVI, magnetite, Fe II -associated iron oxides/(oxy)hydroxides, as well as soluble species like Fe 2+ and Cl − . Highly effective reduction of nitrate (20 mg N/L initially) by prtZVI could be realized in a broad pH range (4–10), short reaction time, and at low solid dosage, which is much superior to ZVIs pretreated by H 2 O 2 , HCl, or NaCl alone and the traditional ZVI systems as well. Long-term storage of the prtZVI system (30 d) did not pose any negative effect on the nitrate reduction. 15 N isotopic analysis reveals that NH 4 + is the major aqueous product (>95%) and N 2 is the only gaseous one. Considering the outstanding reduction efficiency, simple synthesis, and long-term stability, the prtZVI system could serve as a promising ZVI technology for reductive removal of contaminants of concern.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Kang Tang,Weilong Hou,Xiaoshu Wang,Wen Xu,Xinqing Lu,Rui Ma,Yanghe Fu,Weidong Zhu
The titanosilicate zeolite catalyzed epoxidation of propylene with hydrogen peroxide (H 2 O 2 , HP) to propylene oxide (PO), the so-called HPPO, is more eco-efficient, compared to the chlorohydrin process and the epoxidation using organic hydroperoxides. However, the zeolite catalysts used in the HPPO process are easily deactivated, because the main byproduct propylene glycol (PG) and other heavy byproducts with high boiling points, derived from the solvolysis of PO, are deposited inside the zeolite micropores. In the present work, trimethylsilylated Ti-MWW zeolites, named Si–Ti-MWW, were developed for the HPPO process. In combination with the results from extensive characterizations for the prepared zeolites, it is found that the trimethylsilylation merely occurs on the external surface of Ti-MWW crystals and can significantly enhance the hydrophobicity , but not alter the coordination states of the Ti species and textural properties of the zeolites. The catalytic properties of Ti-MWW and Si–Ti-MWW were compared in propylene epoxidation. The results show that the solvolysis of PO to the byproducts can be effectively inhibited over the hydrophobic zeolite surface, making Si–Ti-MWW exhibit a much higher selectivity for PO and a much better stability and reusability than the parent Ti-MWW in the HPPO process. The current study, therefore, provides a new approach to develop efficient catalysts for the HPPO process.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）