MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Mengying Luo,Yinnan Song,Niaz Ali Khan,Wanru Wei,Ying Lu,Qinghua Zhao,Haiqing Jiang,Mufang Li,Dong Wang
H 2 O 2 sensor is widely used in biomedicine, environmental governance and food processing. However, it is limited by the complex preparation processes and high cost of raw materials. In this work, we develop a facile, simple and cost-effective method to fabricate H 2 O 2 sensor based on a screen-printed electrode via in-situ growth method. The copper was first electrodeposited on the working electrode of screen-printed electrode (SPE) as a sacrificial layer, subsequently, the SPE was immersed in horseradish peroxidase (HRP) containing phosphate buffer saline (PBS). The Cu ions formed by oxidation of the copper layer combined with HRP and phosphate ions to construct HRP-Cu 3 (PO 4 ) 2 hybrid nanoflowers on its surface. The fabrication process is straightforward, without complex reaction conditions and dangerous drugs, which is conducive to mass production. This sensor showed a good linear response to H 2 O 2 with a detection limit of 1.8 μM and a sensitivity of 263.3 μA∙mM −1 ∙cm −2 . Additionally, it possessed excellent selectivity and long-time stability. The performance of this sensor was investigated in various beverages such as milk, beer, and juice, showing reliable detection of H 2 O 2 which highlights the potential practical applications of the sensor.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Lina Yan,Chao Wang,Yueshuai Wang,Yahui Wang,Zhaozhao Wang,Lirong Zheng,Yue Lu,Ruzhi Wang,Ge Chen
Electrochemical production of hydrogen peroxide (H 2 O 2 ) is a sustainable and environmentally benign process. The electrochemical oxygen reduction process (ORR) via a two electron pathway (2e - ORR) offers a practical method for on-site H 2 O 2 generation. As an earth-abundant catalyst, the cobalt-nitrogen coordinated systems integrated into the carbon matrix (Co-NC) has caused wide attention for its high activity in 2e - ORR. Even though most of the reported Co-NC catalysts have classical planar Co-N 4 coordination, axial coordination engineering has recently emerged as an effective way to control the active sites in the axial direction by using different coordination ligands. The structure-function link between the Co-N configuration of non-planar coordination and 2e - ORR activity is, however, not fully understood. An axial-N coordinated Co-N 5 motif embedded in hierarchically porous graphite-3R carbon (Co-N 5 C) was effectively synthesized using a template-sacrificing method. The Co-N 5 C has a high selectivity for 2e - ORR and a high H 2 O 2 molar production rate of up to 6.78 mol peroxide/g catalyst /h in acidic media, both of which are better than its Co-N 4 counterpart. DFT analyses demonstrate that axial-N ligands regulated the d -band center of the Co atom in the Co-N 5 C catalyst, inducing a shift in Δ G *OOH near the Sabatier volcano plot's peak (Δ G *OOH = 4.22 eV). This optimized the binding of the *OOH intermediate and then enhanced the protonation of *OOH to produce H 2 O 2 more efficiently.
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MOLECULES
·
2023
·Vol. 28
·期 9
·3736
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IF 4.6
Gege Yang,Ying Chen,Rui Shi,Rongrong Chen,Shanshan Gao,Xin Zhang,Yuan Rao,Ying Lu,Yuancheng Peng,Zhihe Qing,Chunxia Song
Platinum nanoparticles (PtNPs) are classical peroxidase-like nanozyme; self-agglomeration of nanoparticles leads to the undesirable reduction in stability and catalytic activity. Herein, a hybrid peroxidase-like nanocatalyst consisting of PtNPs in situ growing on g–C3N4nanosheets with enhanced peroxidase-mimic catalytic activity ([email protected]–C3N4nanosheets) was prepared for H2O2and oxidase-based colorimetric assay. g–C3N4nanosheets can be used as carriers to solve the problem of poor stability of PtNPs. We observed that the catalytic ability could be maintained for more than 90 days.[email protected]–C3N4nanosheets could quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB), and the absorbance of blue color oxidized TMB (oxTMB) showed a robust linear relationship with the concentration of H2O2(the detection limit (LOD): 3.33 μM). By utilizing H2O2as a mediator, this strategy can be applied to oxidase-based biomolecules (glucose, organophosphorus, and so on, that generate or consume hydrogen peroxide) sensing. As a proof of concept, a sensitive assay of cholesterol that combined[email protected]–C3N4nanosheets with cholesterol oxidase (ChOx) cascade catalytic reaction was constructed with an LOD of 9.35 μM in a widespread range from 10 to 800 μM (R2= 0.9981). In addition, we also verified its ability to detect cholesterol in fetal bovine serum. These results showed application prospect of[email protected]–C3N4nanosheets-based colorimetry in sensing and clinical medical detection.Keywords:[email protected]–C3N4nanosheets;peroxidase-mimic;H2O2;oxidase-based sensing
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PubMed
高影响因子
JOURNAL OF BIOMATERIALS APPLICATIONS
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2023
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IF 2.9
Mengyu Zhu,Yang Zhang,Chi Zhang,Lei Chen,Ying Kuang
Oxidative damage of neurons is one of the key pathological markers of Alzheimer’s disease (AD), which eventually leads to neuronal apoptosis and loss. Nuclear factor E2-related factor 2 (Nrf2) is a key regulator of antioxidant response and is considered to be an important therapeutic target for neurodegenerative diseases. In this study, the selenated derivative of antioxidant rutin (Se-Rutin) was synthesized with sodium selenate (Na2SeO3) as raw material by a simple electrostatic-compound in situ selenium reduction method. The effects of Se-Rutin on H2O2 induced oxidative damage in Pheochromocytoma PC12 cells were evaluated by cell viability, apoptosis, reactive oxygen species level and the expression of antioxidant response element (Nrf2). The results showed that H2O2 treatment significantly increased the level of apoptosis and reactive oxygen species, while the level of Nrf2 and HO-1 decreased. However, Se-Rutin significantly reduced H2O2 induced apoptosis and cytotoxicity, and increased the expression of Nrf2 and HO-1, both of which were better than that of pure rutin. Therefore, the activation of Nrf2/HO-1 signaling pathway may be the basis of Se-Rutin’s anti-oxidative damage to AD.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Mengli Xu,Yuan Shen,Linyu Wang,Coucong Gong,Shouhui Chen
In this work, a novel H 2 O 2 biosensor was developed based on the composites of microperoxidase-11 (MP-11) encapsulated in graphene oxide (GO)-PCN-333 (Al) (PCN stands for porous coordination network, one of the metal-organic frameworks). The PCN-333(Al) firmly and uniformly grew on the surface of GO sheet with large specific surface and excellent electrical conductivity, which provided a lots of pores for the encapsulation of MP-11 in the composites and selectively accumulated analytes into its mesopores to improve the selectivity of enzymatic reaction. The MP-11 molecules might freely move through mesopores of PCN-333 (Al) to maintain bioactivity, which remarkably enhanced the mass transfer rate and quickened the electron transfer for electrochemical biosensors. Scanning electron microscopy was used to characterize the GO and PCN-333(Al)-GO composites. Cyclic voltammetry and differential pulse voltammetry were used to characterize the electrochemical behaviors and performance of the H 2 O 2 biosensor. The target electrode showed excellent performance with a wide linear range from 10 μ M to 800 μ M, a low detection limit of 3 μ M, good stability and high selectivity, which was superior to some other H 2 O 2 biosensors.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiangcheng Zhang,Jingzhen Zhang,Jie Miao,Xue Wen,Chao Chen,Baoxue Zhou,Mingce Long
Photocatalytic H 2 O 2 production is a promising strategy for decentralized applications, but to realize efficient H 2 O 2 production in the ambient conditions and absence of organic sacrifice remains challengeable. Herein, anthraquinone functionalized covalent organic frameworks (TpAQ-COFs) were fabricated by β-ketoenamines links of 2,6-diaminoanthraquinone (AQ) and 2, 4, 6-triformylphloroglucinol (Tp), and the structures and compositions were tuned by controlling the condensation time. The increase of time favors the assembly of TpAQ-COFs into more ordered lamellar stacking structure, and induces the increase of enol-imine form. The critical role of anthraquinone moieties as the active sites for oxygen reduction was proved, that is, facilitating charge separation and enhancing the activity and selectivity of H 2 O 2 production. Upon visible light irradiation, the TpAQ-COF synthesized after 12 h reaction has the highest content of anthraquinone moieties and the best performance for H 2 O 2 production (420 μmol h −1 g −1 ) in the absence of organic sacrificial agents. These findings bring insights to incorporate anthraquinone chemistry into photocatalysts at molecular levels for efficient H 2 O 2 production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Qiao Yang,Chuanhai Xia,Shuai Chen,Xuezhi Cao,Jingcheng Hao
Hypothesis Despite that the development of Cu 2 SnS 3 (CTS) catalyst has attracted increasing interests, few study has reported to investigate its heterogeneous catalytic degradation of organic pollutants in a Fenton-like process. Furthermore, the influence of Sn components towards Cu (II)/Cu (I) redox cycling in CTS catalytic systems remains a fascinating research. Experiments In this work, a series of CTS catalysts with controlled crystalline phases were prepared via a microwave-assisted pathway and applied in the H 2 O 2 activation for phenol degradation. The efficiency of phenol degradation in CTS-1/H 2 O 2 system (CTS-1: the molar ratio of Sn (copper acetate) and Cu (tin dichloride) is determined to be Sn:Cu = 1:1) was systematically investigated by controlling various reaction parameters including H 2 O 2 dosage, initial pH and reaction temperature. We discovered that Cu 2 SnS 3 exhibited superior catalytic activity to the contrast monometallic Cu or Sn sulfides and Cu (I) acted as the dominant active sites. The higher Cu (I) proportions conduce to the higher catalytic activities of CTS catalysts. Quenching experiments and electron paramagnetic resonance (EPR) further proved that the activation of H 2 O 2 by CTS catalyst produces reactive oxygen species (ROS) and subsequently leads to degradation of the contaminants. A reasonable mechanism of enhanced H 2 O 2 activation in Fenton-like reaction of CTS/H 2 O 2 system was proposed for phenol degradation by investigating the roles of copper, tin and sulfur species. Findings The developed CTS acted as a promising catalyst in Fenton-like oxidation progress for phenol degradation. Importantly, the copper and tin species contribute to a synergetic effect for the promotion of Cu (II)/Cu (I) redox cycle, which thus enhanced the activation of H 2 O 2 . Our work may offer new insight on the facilitation of Cu (II)/Cu (I) redox cycle in Cu-based Fenton-like catalytic systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Junpeng Yue,Hanpei Yang,Chen Liu,Qiang Zhang,Yanhui Ao
A new strategy to realize efficient removal of organics from water through photo-self-Fenton was investigated. Characterizations and calculations demonstrated that a novel twin carbon nitride with abundant surficial N-defects and compressed π-π layer stacking can be constructed by thermal polymerization of urea under suitable basicity. Synergistically, the twins exhibited an in-situ H 2 O 2 producing at a rate as high as 26.36 mM h −1 g −1 at 420 nm that exceeded most reported C 3 N 4 , and their mineralization rates for Tetracycline Hydrochloride, Bisphenol A , Ciprofloxacin, and Rhodamine B reached 8.8, 15.2, 9.1, and 13 times higher than that of pristine C 3 N 4 . It is concluded that enriching both of photogenerated electrons and molecular oxygens on specific sites plays a crucial role during photocatalysis-self-Fenton process. Particular attentions have to be paid to build structures achieving one and two-electron reduction of O 2 , and activation of H 2 O 2 to •OH simultaneously.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Guiyang Yu,Ke Gong,Chuanwang Xing,Lan Hu,Haibin Huang,Lejie Gao,Debao Wang,Xiyou Li
Organic semiconductor under photoexcitation could generate abundant strong-binding Frenkel excitons and inevitably suffer from low dissociation efficiency (<1%) and poor mobility ability, which severely suppresses the efficient utilization of photogenerated charges and corresponding activity. Herein, a dual P-doping strategy is proposed in bay and corner sites implanted polymeric carbon nitride (PCN-D) for visible-driven H 2 O 2 production. The dual P doping breaks localized electron state around original symmetric heptazine units and weakens the binding energy between electrons and holes, increasing dissociation efficiency to reach 11.9% with 20-fold improvement. In addition, the conductivity ability of PCN-D, including formed carrier charge concentration and mobility, achieves 13-fold and 7-fold improvement, which facilitates the charge transfer and separation. The proposed dual doped-P-site strategy, with the blessing of porous structure, provides plentiful active center for effective adsorption and activation of O 2 molecule, further accelerating reaction progress and achieving six-times increase of photocatalytic H 2 O 2 production rate. This work provides in-depth insight into the importance of dual P-doping to optimize kinetic behavior of photogenerated charges and opens an avenue to the multiscale doping-modulation of semiconductor with high efficiency solar energy conversion.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 9
·2716-2730
·
IF 7
Siyuan Gao,Fangmian Wei,Johannes Karges,Yukun Zhao,Liangnian Ji,Hui Chao
Melanoma is one of the most aggressive and deadliest forms of skin cancer. Besides traditional medicinal techniques, the use of photodynamic therapy is receiving increasing attention as a complementary method. Despite recent advances in the field, the majority of compounds unselectively localize inside the organism and are excited with blue or ultraviolet light, limiting the application of this method to superficial tumors. To overcome these drawbacks, herein, the encapsulation of cyclometalated iridium(III) prodrugs into selenium nanoparticles, which were further camouflaged with cancer cell membranes, is reported. The nanocomposite readily dissociated upon exposure to hydrogen peroxide, triggering the release of the iridium complex, which acts as a photosensitizer, as well as methylquinone and selenium nanoparticles, which act as glutathione scavengers and chemotherapeutic reagents. The reduced intracellular glutathione levels enhance the sensitivity of the cancer cells for anticancer treatment. The cancer cell membrane-camouflaged nanoparticles showed improved selectivity, membrane permeability, and pharmacokinetic effect for cancerous cells. Upon two-photon excitation at 730 nm, the nanoparticles were able to identify as well as nearly fully eradicate a melanoma tumor inside a mouse model by synergistic chemotherapy and near-infrared photodynamic therapy.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Yanmei Li,Jing Wang,Ziyang Xiang,Junhui Yang,Jinglin Yin,Xin Guo,Wenlei Wang
In this study, a carbonized aerogel (CA) decorated with Mn-FeOOH hybrid nanoparticles was prepared and has been used as a better heterogeneous photo-Fenton catalyst. Mn doping accelerated the regeneration of Fe 2+ and promoted the decomposition of H 2 O 2 while producing many hydroxyl radicals (·OH), which solved the mass transfer problem in the traditional heterogeneous Fenton system. The amount of·OH in the Mn-FeOOH@CA/H 2 O 2 system within 40 min was 2.4 times higher than that in the FeOOH@CA/H 2 O 2 system, which further indicates that·OH was the main active species. High-porosity CA has been designed as an electron transport channel. During photocatalysis , electron transfer occurred between the Mn-FeOOH composite material and CA. The Fe 2+ could be used as reaction sites to promote the activation of H 2 O 2 on the surface of 1-Mn/FeOOH, and achieved 100 % As(III) degradation efficiency within 25 min. The catalyst maintained more than 80 % of its original oxidation capacity after five cycles of experiments, which indicates that it has good durability. This work is expected to provide rational design of heterometallic doped materials with oxygen vacancies to treat arsenic pollution.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2023
·
IF 7.8
Peng Xu,Zhuoyu Yang,Xin Liu,Pengfei Zhu
Zero-valent copper (ZVC) coupled with oxygen gas (O 2 ) was extensively studied to degrade refractory contaminant, while the active dismutation reaction and low reactivity of Cu(I) refrained the performance at acid condition. In this study, ferrous ion (Fe(II)) was added to the ZVC/O 2 system (ZVC/Fe(II)/O 2 system) to enhance the degradation ability, the degradation rate of acid orange 7 in the ZVC/Fe(II)/O 2 system was enhanced by 34.8% compared to the ZVC/O 2 system, and the corresponding apparent rate constant was almost three times higher than that of the ZVC/O 2 system. In the reactive species identification experiments, by electron spin resonance experiments and quenching experiments of nitrobenzene , tert butyl alcohol and methanol, hydroxyl radical was proven as primary reactive oxygen species rather than high-valent metal-Cu(III). In addition, the optimum ZVC dosage, Fe(II) concentration, pH and stirring rate were derived based on optimization experiments combined with economic applicability. In the ZVC/Fe(II)/O 2 system, the mechanism was analyzed by detecting the variation of the concentration of H 2 O 2 , Cu(I) and total dissolved copper in the solution. In the degradation process , ZVC was corroded to form Cu(I) by H + , then Cu(I) reacted with O 2 to generate hydrogen peroxide, the generated hydrogen peroxide was induced by Fe(II) and Cu(I) to produce hydroxyl radical, at the same time, ZVC and Cu(I) could reduce Fe(III) to Fe(II). The coexisting substances like carbonate ion , nitrate ion, sulfate ion and phosphate ion did not affect the demineralization of acid orange 7 in the ZVC/Fe(II)/O 2 system, chloride ion remarkably accelerated the degradation rate of acid orange 7, while fulvic acid limited the acid orange 7 removal. The ZVC/Fe(II)/O 2 system also showed excellent degradability in well water, lake water and tap water . Total dissolved copper concentration was controlled within 1 mg/L by the alkali precipitation method, which was within II-level environmental quality criteria in China. These facts suggested that Fe(II)-enhanced ZVC system had great development potential in water treatment .
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