Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120879
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IF 7.2
Chengzhao Liu,Tao Liu,Suhua Liu,Xiufang Zhang,Guanlong Wang
Recently, it was reported photocatalytic H 2 O 2 generation performed in biphasic system could significantly increase the H 2 O 2 yield. Aiming to further improve the H 2 O 2 yield, hydrophobic heterojunction of α-S and vacancy-rich g-C 3 N 4 (CNN) was constructed. H 2 O 2 production performance tests demonstrated the 0.2α-S/CNN composite achieved H 2 O 2 yields 1.72 and 1.99 times higher than pristine CNN and α-S, respectively. N-(C) 3 bonded nitrogen(N 3 C ) promoted oxygen activation, and heterojunction facilitated the separation of photogenerated holes and electrons. These contributed more effective photocatalytic synthesis of H 2 O 2 . The optimal 0.2α-S/CNN achieved a production rate of 2218 μmol g −1 , with an impressive apparent quantum yield (AQE) of 6.92 % under 455 nm monochromatic light, outperforming the state-of-the-art catalysts. The proposed mechanism suggested that photogenerated electrons migrated from α-S to CNN, reducing adsorbed O 2 to form •O 2 − radicals. These radicals subsequently reacted with water in the aqueous phase to generate H 2 O 2 via 2e − ORR. Due to the strong hydrophobicity of the catalyst, most •O 2 − radicals were generated in benzyl alcohol (BA) phase, while H 2 O 2 predominantly formed in the aqueous phase. This spatial separation delayed H 2 O 2 decomposition, facilitating its accumulation and enhancing overall yield.
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Frontiers of Environmental Science & Engineering
·
2020
·Vol. 15
·期 4
·1-13
·
IF 4.053
Feng Haoran,Liu Min,Zeng Wei,Chen Ying
The present study reports the use of the O 3 /H 2 O 2 process in the pretreatment of the mother liquor of gas field wastewater (ML-GFW), obtained from the multi-effect distillation treatment of the gas field wastewater. The range of optimal operation conditions was obtained by single-factor experiments. Response surface methodology (RSM) based on the central composite design (CCD) was used for the optimization procedure. A regression model with Total organic carbon (TOC) removal efficiency as the response value was established ( R 2 = 0.9865). The three key factors were arranged according to their significance as: pH>H 2 O 2 dosage>ozone flow rate. The model predicted that the best operation conditions could be obtained at a pH of 10.9, an ozone flow rate of 0.8 L/min, and H 2 O 2 dosage of 6.2 mL. The dosing ratio of ozone was calculated to be 9.84 mg O 3 /mg TOC. The maximum removal efficiency predicted was 75.9%, while the measured value was 72.3%. The relative deviation was found to be in an acceptable range. The ozone utilization and free radical quenching experiments showed that the addition of H 2 O 2 promoted the decomposition of ozone to produce hydroxyl radicals (·OH). This also improved the ozone utilization efficiency. Gas chromatography-mass spectrometry (GC-MS) analysis showed that most of the organic matters in ML-GFW were degraded, while some residuals needed further treatment. This study provided the data and the necessary technical supports for further research on the treatment of ML-GFW.
研究领域:
环境科学
·
化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shuai Yang,Dongqi Tian,Xinhao Wang,Peng Zhou,Zhaokun Xiong,Heng Zhang,Yang Liu,Gang Yao,Bo Lai
Fenton-like technology has been widely used in the field of water treatment as an advanced oxidation processes (AOPs), and a multitude of non-homogeneous catalysts have been reported effectively to enhance it. Herein, nitrogen and sulfur co-doped nanocarbon materials (NSC) was designed and synthesized, which formed a unique mesoporous structure and abundant functional groups on the surface. It exhibits superior catalytic performance to enhance the Fe(III)/H 2 O 2 system for sulfamethoxazole (SMX) degradation, k obs is 18 times higher than Fe(III)/H 2 O 2 system after the introduction of NSC under the same experimental conditions. Also, the working pH of Fe(III)/H 2 O 2 system was broadened by NSC. Quenching and probe experiments demonstrate that hydroxyl radical (∙OH) was the dominant active species. Both dissociative and surface-bound iron species were observed, which indicates direct reduction and in-situ binding of Fe(III), respectively. Further investigation found nitrogen and sulfur co-doped attribute to the formation of abundant functional groups, the C O bond and C S C bond on the surface of NSC result in the directly reduce of Fe(III), while –COOH contributes to the in-situ binding. The intermediates and possible degradation pathway of SMX degradation were proposed based on the results of liquid chromatography-quadrupole time of flight-mass spectrometer (LC-QTOF-MS). The results of cycling and co-existing ions experiments demonstrate that NSC has outstanding potential for application. This work provides a novel insight into the sustained removal of micropollutants from the aqueous environment based on the nanocarbon materials enhancing the Fenton-like oxidation.
研究领域:
环境科学
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材料科学
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化学工程
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Feng Cheng,Peng Zhou,Yang Liu,Xiaowei Huo,Jian Zhang,Yue Yuan,Heng Zhang,Bo Lai,Yongli Zhang
Slow reduction of Fe(III) in iron-mediated Fenton-like systems strongly limits the decomposition of H 2 O 2 to produce hydroxyl radicals ( • OH). Here, we report that graphene oxide (GO) possesses excellent reactivity to enhance the Fe(III)/H 2 O 2 Fenton and photo-Fenton oxidation for degrading chloramphenicol (CAP). EPR analysis and quenching tests reveal that • OH is the primary oxidant for CAP degradation. The characterization analysis and iron species transformation experiments demonstrate that Fe(III) can combine with the functional groups on the GO surface to form GO-Fe(III) complexes. The chronopotentiometry and cyclic voltammogram suggest that GO can donate electrons to Fe(III) via intramolecular electron transfer and promote H 2 O 2 induced Fe(III) reduction by increasing the oxidation capability of Fe(III) due to the formation of GO-Fe(III) complexes, resulting in the strong promotion of the Fe(III)/Fe(II) cycle for producing OH. Moreover, the dark- and vis-GO/Fe(III)/H 2 O 2 systems can effectively degrade CAP at initial pH ranging from 2.0 to 4.7. The reusability and stability of GO were evaluated by performing the cyclic degradation experiments of CAP. The OH induced degradation pathway of CAP was proposed involving three stages, based on intermediates analysis of UPLC-QTOF-MS/MS system. Therefore, the GO/Fe(III)/H 2 O 2 system with or without visible light shows high potential for application in environmental remediation.
研究领域:
环境科学
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化学
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高影响因子
Biomaterials Science
·
2022
·Vol. 10
·期 9
·2358-2369
·
IF 7.59
Yao Hu,Song Bai,Xingyu Fan,Fangfang Zhou,Botao Chen,Songwen Tan,Hui Xu,Anqiang Pan,Shuquan Liang,Yongju He
Employing hypoxia-activated prodrugs is an appealing oncotherapy strategy, but limited by insufficient tumor hypoxia. Moreover, a standalone prodrug fails to treat tumors satisfactorily due to tumor complexity. Herein, a nanosystem (TPZ@FeMSN-GOX) was established for triple synergetic cancer starvation therapy, hypoxia-activated chemotherapy and chemodynamic therapy (CDT). TPZ@FeMSN-GOX was prepared by synthesizing iron-doped mesoporous silica nanoparticles (FeMSNs) followed by surface conjugation with glucose oxidase (GOX), and then loading with hypoxia-activated prodrug tirapazamine (TPZ). When TPZ@FeMSN-GOX entered the tumor cells, GOX could not only exhaust glucose to starve cancer cells and concomitantly produce H2O2, but also consume O2 to aggravate the hypoxia environment and amplify TPZ-mediated chemotherapy. Meanwhile, the released Fe3+ was reduced to reactive Fe2+ by endogenous glutathione, which ultimately decomposed the produced H2O2 and endogenous H2O2 into highly toxic ˙OH, guaranteeing highly efficient CDT. Together, TPZ@FeMSN-GOX could effectively kill cancer cells and significantly inhibit tumor growth, providing a good paradigm for effective tumor treatment.
研究领域:
纳米技术
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癌症治疗
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药学
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生物医学工程
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2022
·Vol. 36
·期 12
·e6888
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IF 4.072
Tiedong Sun,Zhengya Yue,Yan Song,Jiatong Ni,Wenxin Wang,Junge Zhao,Jialun Li,Yuan Sun,Bin Li
Chemodynamic therapy (CDT) is a highly effective clinical treatment strategy based on the Fenton or Fenton-like responses. However, its efficacy has been greatly limited by the complex tumor microenvironment, TME, such as the low levels of H 2 O 2 and the overexpression of the glutathione (GSH). Polyoxometalates (POMs) are compounds that consist of anionic transition metal oxide clusters, such as tungsten (W) and molybdenum (Mo), and notably, these compounds have excellent redox properties in biological systems that can be utilized therapeutically. Therefore, POM-CaO 2 @ZIF-8 nanoparticles (NPs) have been synthesized and used as a mediator to develop an electrically enhanced CDT strategy. It is hoped that the simultaneous modulation of endogenous (the H 2 O 2 generated by CaO 2 NPs and GSH depletion by POM) and exogenous (Electric, E) stimulation enhanced Fenton-like responses will lead to better therapeutic results. Such a treatment strategy has shown excellent tumor cell killing effects in both in vitro and in vivo studies.
研究领域:
纳米医学
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癌症治疗
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材料科学
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生物医学工程
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CARBOHYDRATE POLYMERS
·
2020
·
IF 7.182
Xin Ye He,Ao Sun,Tao Li,Yong Jun Qian,Hong Qian,Yun Fei Ling,Ling Hong Zhang,Qing Ya Liu,Tao Peng,Zhiyong Qian
The development of minimally invasive surgery has created a demand for ideal medical adhesives exhibiting biocompatibility, biodegradability, antimicrobial activity, and strong adhesion to tissues in wet environments. However, as clinically approved surgical tissue glues suffer from poor adhesion activation, limited adhesion strength, and toxicity, novel tissue glues are highly sought after. Herein, a mussel-inspired injectable hydrogel was prepared from catechol- and methacrylate-modified chitosan/gelatin and shown to exhibit biocompatibility, inherent antimicrobial activity, and good adhesion to wet tissues. Moreover, as this gel could be applied onto tissue surfaces and cured in situ within seconds of body contact by a biocompatible and multifunctional redox initiator (H 2 O 2 -ascorbic acid), it was concluded to be a promising surgical sealant and wound dressing (even for infected wounds) accelerating wound healing .
研究领域:
生物材料学
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医学
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药学
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BIOSENSORS & BIOELECTRONICS
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2021
·
IF 10.618
Li-Ping Zong,Ling-Yu Ruan,Junji Li,Robert S. Marks,Jun-Song Wang,Serge Cosnier,Xue-Ji Zhang,Dan Shan
Enzyme mimetics have attracted wide interest due to their inherent enzyme-like activity and unique physicochemical properties , as well as promising applications in disease diagnosis, treatment and monitoring. Inspired by the attributes of nonheme iron enzymes , synthetic models were designed to mimic their capability and investigate the catalytic mechanisms . Herein, metal-organic gels (Fe-MOGs) with horseradish peroxidase (HRP) like Fe-N X structure were successfully synthesized though the coordination between iron and 1,10-phenanthroline-2,9-dicarboxylic acid (PDA) and exhibited excellent peroxidase-like activity. Its structure-activity relationship and the in-situ electrochemiluminescence (ECL) detection of H 2 O 2 secreted by Hela cells were further investigated. The highly dispersed Fe-N X active sites inside Fe-MOGs were able to catalyze the decomposition of H 2 O 2 into large amounts of reactive oxygen species (ROS) via a Fenton-like reaction under a low overpotential. Due to the accumulation of ROS free radicals , the luminol ECL emission was significantly amplified. A proof-of-concept biosensor was constructed with a detection limit as low as 2.2 nM and a wide linear range from 0.01 to 40 μM. As a novel metal organic gels based enzyme mimetic, Fe-MOGs show great promises in early cancer detection and pathological process monitoring.
研究领域:
生物化学
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生物技术
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分析化学
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材料科学
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癌症研究
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ding-Ming Xue,Yi-Jun Zhang,Jing-Wen Chen,Hao Yang,Rui-Jie Xie,Shi-Chao Qi,Yuan-Qing Bu,Fei Liu,Hou-Hu Zhang,Jacques Lalevée
Covalent organic frameworks (COFs), as a newly emerging kind of porous and crystalline materials, serve as an ideal template for hydrogen peroxide (H 2 O 2 ) photosynthesis. However, the vision of achieving high efficiency and selectivity in H 2 O 2 photosynthesis is greatly hindered by the large exciton binding energy and limited charge separation efficiency influenced by the molecular structure of the building blocks. Herein, we developed three newly designed COFs with a donor–acceptor (D-A) structure and incorporated regulatory units (fluorine, F, and methoxyl, OCH 3 ) in the D-A pathway through molecular engineering to optimize electronic structure, the availability of activate sites, charge kinetics and O 2 activation capacity. Due to electron-donating effect, OCH 3 -functionalization (NIES-COF-3) can strengthen the intramolecular electron transfer and interaction with O 2 . This results in a reduction of the energy barrier of the rate-determining step (*O 2 → *OOH) and excellent O 2 -to-H 2 O 2 photocatalytic activity under visible light irradiation, delivering an H 2 O 2 production rate of 3238.4 μmol g −1 h −1 and a high apparent quantum yield of 3.17 %. In addition, F-functionalization (NIES-COF-2) primarily reduces the band-gap energy and improve the O 2 adsorption capacity compared to unfunctionalized NIES-COF-1. This work unveils insight into the catalytic activity-optimization mechanism of molecular engineering in the D-A structure and provides important references for photocatalysts.
研究领域:
材料科学
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化学工程
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环境科学
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Xiang Gao,Huanhuan Chen,Huimin Qiu,Yang Zhang,Jie Cheng,Yizhong Shen
Due to the typical volatility of gaseous pollutant methyl mercaptan (CH 3 SH), the development of a facile, reliable, and accurate onsite environmental surveillance of highly toxic CH 3 SH faces many challenges, but it is critical to environmental atmosphere assessment and safeguarding public health. Here, we prepared a novel bimetallic carbon dots (Fe&Cu@CDs) nanozyme with high peroxidase-mimicking activity to design a portable hydrogel kit for onsite visual H 2 O 2 -self-supplying enzymatic cascade catalytic colorimetric and photothermal signal synergistic amplification dual-modal monitoring of CH 3 SH in atmospheric environment. Assisted by alcohol oxidase (AOX), CH 3 SH could be specifically converted into H 2 O 2 for oxidizing chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) catalyzed by Fe&Cu@CDs to produce dark blue ox-TMB with absorption at 652 nm and photothermal characters. Consequently, a CH 3 SH concentration-dependent change both in naked-eye color and photothermal effect-triggered temperature were observed. By hybridizing AOX-assisted Fe&Cu@CDs + TMB with agarose, a H 2 O 2 -self-supplying colorimetric and photothermal signal synergistic amplification sensory hydrogel kit integrated with Color Picker APP-installed smartphone and 660 nm laser-equipped handheld thermal imager for CH 3 SH was proposed with acceptable results in atmospheric environment around wastepile ( e.g. , solid waste and food waste piles), which exhibited great potentials to further develop commercial onsite monitoring platforms in warning-early abnormal atmospheric CH 3 SH for safeguarding environmental health.
研究领域:
环境科学
·
分析化学
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纳米技术
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材料科学
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PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2025
·
IF 6.3
Xinyang He,Ying Tian,Weiwei Lu,Fangfen Jing,Mingzhu Jin,Jiahui Zhu,Qi Fong,Rongtai Yu
Background The widespread presence of antibiotics in aquatic environments poses severe ecological risks due to inadequate removal in conventional wastewater treatment. This study investigates morphology-controlled concave polymer nanospheres for simultaneous tetracycline (TC) degradation and photocatalytic H 2 O 2 production. Methods Synthesis of aminophenol-formaldehyde resins (APF) using 3-aminophenol (3-AP), ammonia water, and formaldehyde. Through precise acetone-mediated etching, three concave resin catalysts with distinct concavities (70–78 nm) and wall thicknesses (47–54 nm) were synthesized. Significant findings Systematic characterization revealed that increased wall thickness enhanced visible-light absorption (up to 700 nm), while higher concavity improved light reflection efficiency. The catalyst synthesized with 38 mL acetone demonstrated optimal H 2 O 2 yield (168.5 mg g⁻¹), whereas the maximum TC degradation efficiency (106.57 % at 180 min) was achieved using the 32 mL acetone-etched catalyst with the deepest concavity. Mechanistic studies identified synergistic effects between light scattering geometry and charge carrier dynamics, where concave structures facilitated multi-directional photon utilization while thickened walls suppressed electron-hole recombination. This work provides new insights into morphology engineering for dual-functional photocatalytic systems in environmental remediation.
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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Weikang Wang,Yadong Wu,Shahid Khan,Haopeng Jiang,Muhammad Adnan Qaiser,Xianzhi Chai,Chengzhang Zhu,Lele Wang,Qinqin Liu
Solar-driven hydrogen (H 2 ) and hydrogen peroxide (H 2 O 2 ) generation over visible-light responsive carbon nitride (CN) photocatalysts for in situ efficient sterilization is a promising and eco-friendly strategy. Herein, a colloidal potassium-ion (K + ) intercalated crystalline CN nanosheets (KCCN) photocatalyst was constructed for boosting synergetic H 2 O 2 synthesis with isopropanol (IPA) oxidation and in situ antibacterial effect . The surface hydroxyl (−OH) and cyano (−C N) groups induced by molten salt (KCl)-assisted thermal treatments contributed to the colloidal nature of CN, facilitating for high wettability of KCCN in aqueous solution to gain active hydrogen (H + ) from water sustainably. Meaningfully, the enhanced high-energy singlet oxygen species ( 1 O 2 ) produced by KCNN-2 were verified by electron paramagnetic resonance (EPR) and 9,10-anthracenediyl-bis(methylene)-dimalonic acid (ABDA)-fluorescent probe, significantly contributing to H 2 O 2 production and antibacterial effect. Consequently, the optimal KCCN-2 exhibited a much enhanced H 2 generation of 4.11 mmol g −1 h −1 , and H 2 O 2 production activity of 1.82 mmol L −1 h −1 with acetone yield rate of 47.3 mmol g −1 h −1 under visible-light (λ > 420 nm) irradiation in 10 vol% IPA solution. The in-situ generated H 2 O 2 can be activated to produce reactive oxygen species (ROS), especially 1 O 2 , to effectively kill the Escherichia coli , reaching an improved an antibacterial rate of 89.7% under stimulated sunlight irradiation in 1 h. This work could offer a new insight into the photoinduced ROS for aqueous H 2 O 2 photosynthesis and antibacterial application.
研究领域:
环境科学
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生物学
·
材料科学
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危险品化学品经营许可证（带存储）