ENVIRONMENTAL RESEARCH
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2023
·
IF 8.3
Zhuangzhuang Zhang,Haiqian Zhao,Zhonghua Wang,Zhipei Hu,Qingshu Wang,Erlin Meng,Shiwei Lai,Jiaxin Ying,Hongguang Li,Chuanyan Wu
The use of the electro-Fenton process to continuously generate H 2 O 2 and efficiently degrade organic pollutants is considered a promising technology . The ratio of generation of H 2 O 2 is usually regarded as the critical step; however, how the H 2 O 2 is utilized is also of particular importance. Herein, activated carbon was activated at different temperatures and used to explore the effect of nitrogen doping on the production and utilization of H 2 O 2 in the electro-Fenton-based degradation of organic pollutants. The experimental results indicate that nitrogen-doped activated carbon simultaneously promotes the generation and utilization of H 2 O 2 , which is attributed to the regulation of the competition between phenol and O 2 adsorption by the doped nitrogen. Nitrogen doping not only improves 2e − ORR selectivity but also aggregates phenol near the cathode to balance the concentrations of phenol and ·OH. Density functional theory (DFT) calculations further confirmed that pyrrole-N as a dopant promoted the adsorption of phenol , while pyridine-N was more favorable for O 2 adsorption. The unique balance of nitrogen types possessed by modified activated carbon NAC-750 permits the efficient synergistic generation and utilization of H 2 O 2 in a balanced manner during the degradation of phenol. This work provides a new direction for the rational nitrogen-doping modification of activated carbon for the electro-Fenton-based degradation of organic pollutants.
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MICROCHEMICAL JOURNAL
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2023
·
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
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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
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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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
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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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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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MOLECULES
·
2023
·Vol. 28
·期 9
·3736
·
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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JOURNAL OF BIOMATERIALS APPLICATIONS
·
2023
·
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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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jianwen Zhou,Tianshang Shan,Hao Luo,Bruno Boury,Xia Xu,Hui Wu,Fengshan Zhang,He Xiao
Designing efficient semiconductors for photocatalytic oxygen reduction reaction (ORR) without sacrificial agent is an urgent challenge for H 2 O 2 production under ambient condition. Graphite carbon nitride (g-C 3 N 4 ) exhibits controllable regulation in band structure and light absorption for photocatalytic process. However, the photocatalytic H 2 O 2 synthesis by pristine g-C 3 N 4 is poor due to the fast recombination of photogenerated carriers and unfavorable selectivity of ORR. To enhance the photocatalytic H 2 O 2 production, different types of carbon can use in combination with g-C 3 N 4 . In the present work, we show how cellulose fiber from bamboo can lead to hybrid C/ g-C 3 N 4 photocatalyst with enhanced photocatalytic activity and H 2 O 2 production rate of 121.75 μmol·L −1 ·h −1 , which is 6.2-fold higher than that of pure g-C 3 N 4 without any sacrificial agent. The experimental results confirmed that TEMPO-cellulose derived hydrophilic carbon can not only accelerate the transfer of photo-generated electrons as well as efficient charge carrier separation, but also promote the sequential two-step single-electron ORR route. Thus, this work provides a pioneering perspective for tuning the electronic interaction between g-C 3 N 4 and cellulosic carbon for enhanced photocatalytic H 2 O 2 synthesis.
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ELECTROCHEMISTRY COMMUNICATIONS
·
2022
·
IF 5.443
Jinge Wang,Wei Zhou,Jiayi Li,Chaowei Yang,Xiaoxiao Meng,Jihui Gao
Pulsed electrocatalysis is emerging as a promising strategy for the improvement of electrocatalytic performance. Herein, the 2-electron oxygen reduction reaction (2eORR) for H 2 O 2 synthesis was taken as a model reaction to explore the effects of pulsed parameters on electrocatalysis. Firstly, the key parameters of a square wave pulse were determined by theoretical analysis and electrochemical testing. Secondly, we found that the pulsed period of the square wave pulse should be neither too short nor too long due to the opposing effects of non-Faradaic and diffusion processes. The lower duty ratio was more favorable for 2eORR. Finally, the effects of the pulsed waveform were explored. We found that the enhanced effects on 2eORR under the rapid sweep potential of a triangular or sine wave were similar to those for a square wave with a short period. Under a sine wave pulse with a frequency of 0.2 Hz, the H 2 O 2 production rate and Faradaic efficiency of 2eORR were increased by 1.4 times and 3.62 times, respectively, compared with the results obtained under constant potential, and the energy consumption was reduced by 75 %. The enhanced effects described above could be attributed to the diffusion layer becoming thinner while the pulsed potential was applied. The reaction rate was increased by the diffusion of reactants (i.e., O 2 , H + ) to the electrode surface and the intrinsic selectivity of 2eORR was increased by the oxygen-rich environment. In addition, the ineffective electroreduction of H 2 O 2 was also reduced by the diffusion of H 2 O 2 toward the bulk solution. This work provides new insights into the determination of parameters, waveform effects and the mechanism of pulsed electrocatalysis.
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MOLECULES
·
2022
·Vol. 27
·期 24
·9028
·
IF 4.927
Ling Zhang,Zhenkuan Ma,Yun Fan,Songlin Jiao,Zhan Yu,Xuwei Chen
In this work, ionic liquid (IL) of 1-propyl-3-methyl imidazolium chloride-functionalized silica-mesostructured cellular foam (MCF) was prepared. The obtained MCF-IL was used to construct the Fe(CN)63−-confined electrode (MCF-IL-Fe(CN)63−/PVA) and H2O2electrochemical behavior on the electrode was investigated. It was found that H2O2was oxidized on the freshly prepared electrode while catalytically electro-reduced on the acid pretreated one. Cyclic voltametric results revealed that the real catalyst for catalytic reduction of H2O2was Prussian blue (PB) rather than Fe(CN)63−. The electrocatalytic ability of the acid-pretreated MCF-IL-Fe(CN)63−/PVA electrode offered a wide linear range for H2O2detection. The present study on H2O2electrochemical behavior on an MCF-IL-Fe(CN)63−/PVA electrode might provide useful information for further developing integrated Fe(CN)63−-mediated biosensors as H2O2is extensively involved in the classic reaction containing oxidase enzymes.Keywords:silica mesostructured cellular foam;hydrogen peroxide;ferricyanide;reduction;Prussian blue;ionic liquid
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