Journal of Water Process Engineering
·
2026
·
IF 6.6
Li Zeng,Hanbin Wu,Yiyang Xu,J. Paul Chen,Yiqiao Xie,Yang Yu
The efficient treatment of dye-containing wastewater remains a critical environmental issue, primarily due to its biological toxicity to aquatic microorganisms and high chromaticity. In this work, two types of Co₃O₄-functionalized ceramic hollow fiber membranes were designed to activate peroxymonosulfate (PMS) for the efficient removal of dyes from water. Compared to the static-deposited membrane (SCHFM), the dynamic-deposited membrane (DCHFM) demonstrated a higher loading capacity and more uniform distribution of Co 3 O 4 on both the surface and internal pores, leading to a significant enhancement in catalytic performance. Under optimal operating parameters, the DCHFM achieved over 98% removal of rhodamine B (RhB) during the filtration. Radical quenching and electron paramagnetic resonance (EPR) confirmed the involvement of multiple reactive oxygen species, including singlet oxygen ( 1 O 2 ), hydroxyl radical (HO•), sulfate radical (SO 4 •− ) and superoxide radical (•O 2 − ), with 1 O₂ identified as the predominant reactive species. Furthermore, the functionalized membrane exhibited outstanding operational stability and reusability with negligible cobalt leaching. The findings of this study provide a high-performance catalytic membrane system for the advanced purification of industrial wastewater.
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高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Honglin Zhou,Wenxiu Yuan,Jie Dong,Xiang Shao,Jinyun Chen,Fei Chang,Xinyi Cheng,Haoran Bai,Yujie Cheng,Qincheng Ma,Ying Wang,Jun Tang,Qingping Ke,Jianli Wang
The selective oxidation of cyclohexene to high-value cyclohex–2–enone using singlet oxygen holds significant importance in chemical production. However, conventional methods for generating singlet oxygen are often constrained by harsh conditions, typically requiring high-energy input. This study develops a new methodology that leverages the Pickering emulsion droplet interfaces to facilitate the generation of singlet oxygen for the efficient oxidation of cyclohexene. First, an amphiphilic catalyst SiO2/CNx was synthesized by growing hydrophobic nitrogen-doped carbon on the surface of hydrophilic sheet-like silica through a combined surface-polymerization and carbonization process. Such amphiphilic catalyst can then self-assemble at the interfaces of the oil phase (cyclohexene in ethyl acetate) and water phase (tert-butyl hydroperoxide aqueous solution), thereby stabilizing a water–in–oil Pickering emulsion. The graphitic nitrogen sites on the nitrogen-doped carbon promote the cleavage of tert-butyl hydroperoxide to form superoxide radicals, while the pyridinic nitrogen sites can adsorb and enrich the resulting radicals. In addition, the unique proton-rich microenvironment at the Pickering emulsion droplet interfaces promotes the disproportionation of adsorbed superoxide radicals, generating the desired singlet oxygen for the selective oxidation of cyclohexene. As a result, this Pickering emulsion system achieved a cyclohexene conversion of >99.0% with a 95.0% selectivity toward cyclohex–2–enone, significantly outperforming the results reported in prior studies. This strategy of harnessing the Pickering emulsion droplet interfaces to regulate the generation of highly reactive singlet oxygen opens up a promising route for the efficient synthesis of oxygenated fine chemicals.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Yueru Fang,Zhiqiang Guo,Tanveer Hussain,Xiaoyong Lv,Ronghua Li
Organoarsenical contaminants such as roxarsone (ROX) pose a persistent challenge in water treatment because oxidative degradation of the parent compound inevitably generates inorganic arsenic (iAs), whereas adsorption-based processes immobilize iAs without removing the organoarsenical precursor. As a result, arsenic is redistributed among species rather than eliminated, and its overall fate during transformation and immobilization remains poorly quantified. Here, we develop a Co-doped LaOCl catalyst (Co 0.5 LOC) that enables coupled oxidative transformation and arsenic immobilization under peroxymonosulfate (PMS) activation via spatially integrated Co and La sites. Critically, a complete time-resolved arsenic mass balance is achieved throughout the reaction, with total arsenic recovery maintained at 100 ± 2%, thereby directly linking ROX degradation, iAs formation, and final immobilization. The catalyst exhibits a pseudo-first-order ROX degradation rate of 0.2935 min −1 , 2.2-fold higher than pristine LaOCl, with >96% removal across pH 5–9 and >81% activity retention after five cycles. Mechanistic analysis identifies surface-confined singlet oxygen ( 1 O 2 ) as the dominant reactive species, providing strong resistance to chloride ions and natural organic matter. A synergy index of 6.72 quantifies non-additive oxidation–adsorption coupling. Total organic carbon monitoring reveals that structural transformation substantially exceeds mineralization, with approximately 26% of the initial carbon remaining at 120 min; LC-HRMS tentatively identifies four aromatic intermediates in the residual fraction, consistent with the limited ring-opening capability of surface-confined 1 O 2 . Overall, this work establishes a unified strategy for organoarsenic remediation by integrating oxidative destruction with quantitative arsenic sequestration, enabling comprehensive contaminant fate accountability in advanced water treatment systems.
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高影响因子
ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Xin Zhang,Liping Li,Xinhui Liu,Handan Zhang,Lu Dong,Pengcheng Li,Mengzhu Xue,Linshuai Duan,Xiqin Liu,Bohan Li,Guohui Xia
Extracellular antibiotic resistance gene (eARG) has emerged as a global crisis in recent years, yet commonly used disinfectants have proven ineffective for their elimination. Seeking to enhance the degradation efficiency of eARG, this study explored the potential of carbon nanotubes-activated persulfate (CNTs + PS) system as a novel method for eradicating eARG. Our findings demonstrated that CNTs + PS effectively disrupted the intact structure of eARG, inhibited their genetic replication and horizontal transfer capability, achieving remarkable degradation of eARG contamination. Further experiments revealed that 1 O 2 played a predominant role in eARG degradation, while electron transfer played minor roles in the degradation process. The carbonyl groups served as the primary sites for activating PS to generate 1 O 2 . CNTs can enhance the efficiency of electron transfer from eARG to PS. Moreover, the degradation efficacy of eARG by CNTs + PS was influenced by various factors including the dosage ratio between CNTs and PS, initial concentrations of eARG, pH values, inorganic anions and humic substances and water matrix. Reusability experiment demonstrated that CNTs + PS exhibited stable degradation performance after multiple uses. These findings offer a new perspective for the efficient degradation of eARG in environmental remediation.
研究领域:
环境科学
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化学工程
·
微生物学
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纳米技术
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水处理
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高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Jialin Liang,Yu Zhang,Liang Zhang,Xiao Xiao,Zhihua Mo,Yan Zhou
Conventional hydroxyl radical (•OH)-based treatments ( i.e. , iron-based advanced oxidation technologies (Fe-AOTs) and electrochemical processes) are generally considered efficient approaches for sludge dewatering via destroying the stable extracellular polymeric substances (EPS) structure in sludge. However, extremely acidic conditions ( i.e. , pH 2.8–3.2) in such processes hinder their commercial viability, primarily due to corrosive and environmental issues. Singlet oxygen ( 1 O 2 ), known for its selective oxidation and environmental stability, can break down protein structures even at low levels. 1 O 2 -based processes may enable efficient sludge dewatering under neutral conditions by disrupting complex EPS structures. Therefore, in this study, we for the first time proposed a 1 O 2 -based electrochemical process with a catalytic cathode of pyrite-modified graphite (electro-FeS 2 @graphite) for sludge dewatering under neutral conditions. Results showed that under optimized conditions, the electro-FeS 2 @graphite system achieved superior sludge dewatering (47.9 % water content over ten cycles) compared to existing Fe-AOTs and electrochemical methods. Electron paramagnetic resonance, quenching tests, and reactive oxygen species probes confirmed that the FeS 2 @graphite catalytic cathode mainly generated 1 O 2 species for efficiently eliminating hydrophilic aromatic structures and enhancing sludge dewatering without pH regulation. A three-step mechanism was proposed for the enhanced sludge dewaterability in the electro-FeS 2 @graphite system: (i) in situ high H 2 O 2 yield at FeS 2 @graphite cathode, (ii) considerable 1 O 2 generation within the system, and (iii) selective attack on hydrophilic aromatic structures by 1 O 2 . The operational cost of the proposed system was also substantially lower than that of the above-mentioned treatments. Overall, these findings highlight the effectiveness of 1 O 2 -based electrochemical process in achieving stable and cost-effective sludge dewatering without acidification.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2016
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IF 3.782
Xuefei Zhou,Xiaohong He,Shiliang Wei,Kun Jia,Xiaobo Liu
A novel cyano-terminated zinc phthalocyanine (ZnPc-CN) exhibiting visible near infrared (vis-NIR) emitting around 690 nm in N,N -dimethylformamide (DMF) solvent has been synthesized. Furthermore, the peripheral cyano groups of newly synthesized zinc phthalocyanine were hydrolyzed in strong basic solution, leading to water soluble carboxylated zinc phthalocyanine (ZnPc-COOH) with completely quenched fluorescence in aqueous solution. Interestingly, we found that the NIR fluorescence of aqueous ZnPc-COOH was dramatically recovered in the presence of gold nanorods (Au NR), which was due to the alternation of ZnPc-COOH molecules self-assembling via electrostatic interaction between cetyltrimethylammonium bromide (CTAB) on the surface of Au NR and peripheral carboxyl of ZnPc-COOH. In addition, ZnPc-COOH/Au NR conjugates demonstrated an improved singlet oxygen generation, which could be served as potential bioimaging probe and photosensitizer for photodynamic therapy.
研究领域:
生物医学工程
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材料科学
·
化学
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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Dezhi Kong,Yafei Fan,Feifei Wang,Fangyu Zhang,Qi Zhao,Zhaoli Sun,Jianfei Yao,Menghui Chu,Guo Wang,Guanyun Zhang,Zhaoyong Guan,Hua Sheng,Yifeng Wang
Singlet oxygen (1O2) plays a critical role in oxidation reactions, yet improving its reactivity with substrates remains a significant challenge. This study reports an enzyme-like bifunctional catalyst, Co–N2O2/NC, which can efficiently activate peroxymonosulfate (PMS) with high selectivity and nearly quantitatively generates 1O2 without producing other reactive oxygen species to achieve high reactivity. Notably, it significantly increases the bimolecular reaction rate constant between 1O2 and waterborne micropollutants, as demonstrated by the over 1400-fold enhancement in 4-chlorophenol (4-CP) oxidation compared to that in the bulk solution. Enzyme-like catalytic kinetics were observed, with N-sites of the N-doped carbon support serving for activating 4-CP via interfacial electronic interactions, while Co activates PMS to generate 1O2. The interfacial charge transfer lowers the energy barrier for 1O2 to approach the aromatic ring of 4-CP, which is the rate-limiting step in the oxygenation reaction. Our findings lay the foundation and offer guidance for designing catalysts that facilitate the efficient generation and use of 1O2, expanding its application to a broader range of oxidation processes.
研究领域:
环境科学
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催化化学
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材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ruonan Guo,Zenghui Bi,Beidou Xi,Changsheng Guo,Heng Zhang,Ningqing Lv,Guangzhi Hu,Jian Xu
The function of heterogeneous catalyst in singlet oxygen ( 1 O 2 ) generation under acidic and neutral conditions and the effect of sulfate radical on the generation of 1 O 2 is still unclear. This study provided a novel generation pathway of 1 O 2 in the heterogeneous Mn single − atom catalyst (Mn SAC)/peroxymonosulfate (PMS) system. The MnN4 site with the ideal binding strength promoted the activation of PMS to generate sulfate radical (SO 4 •– ), which would be adsorbed on the carbon/nitrogen sites forming SO 4 •– (s) , reacting spontaneously to produce 1 O 2 . The presence of MnN4 and carbon/nitrogen structure sites could shift the oxidation process from a bulk–phase oxidation to a surface oxidation. This shift has important implications in terms of reaction rate and product distribution, as the dual reaction sites decrease the required migration distance for the active species to form 1 O 2 , avoiding the pointless consumption of active substances.
研究领域:
环境科学
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催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Yang Liu,Hongguang Guo,Yongli Zhang,Weihong Tang,Xin Cheng,Wei Li
Sillenite bismuth ferrite (S-BFO) Bi 25 FeO 40 was synthesized by a hydrothermal process and firstly adopted for the activation of peroxymonosulfate (PMS). Multiple characterization was conducted for the morphology and physicochemical features of S-BFO. Degradation of aquatic levofloxacin (LVF) was thoroughly evaluated by using a coupled process for the decontamination of the typical emerging organics. Some crucial parameters for the activation kinetics as well as economic recyclability were examined with the detailed mechanism proposed. For the first time, singlet oxygen ( 1 O 2 ) was identified as the main reactive oxygen species through radical scavenging experiments, electron paramagnetic resonance spectroscopy (EPR) and HPLC-MS determination. Based on the XPS and EPR results, a catalytic mechanism is proposed concerning the parallel generations of 1 O 2 : (i) Bi 5+ is replaced by Bi 3+ , resulting in the formation of an oxygen vacancy in the lattice and an active oxygen (O ∗ ), which could produce 1 O 2 through the reactions with PMS; (ii) direct formation of 1 O 2 from radSO-5 generated by the interaction between Bi 5+ and PMS. This study demonstrates a novel catalyst for heterogeneous activation of PMS via a non-radical mechanism, which could be alternatively adopted in the decontamination in surface/ground water.
研究领域:
环境科学
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化学工程
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高影响因子
Optical Materials Express
·
2017
·Vol. 7
·期 2
·409-414
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IF 2.591
Junliang Lv,Gongqing Wu,Yang He,Lijuan Zhang,Yunhong Yi
Plasmonic nanoparticles hold great potential in photodynamic therapy (PDT). Herein, a nanoplatform of methylene blue (MB) loaded gold nanobipyramids@SiO2 (GBPs@SiO2-MB) was designed to optimize the generation rate of singlet oxygen (1O2), which was based on the plasmonic effect. The surface plasmon resonance (SPR) of GBPs was finely overlapped with the excitation absorption of MB, a wildly applied organic PDT drug prone to enzymatic degradation. This mesoporous silica coating nanoplatform protects MB molecules against degradation, and this overlap greatly enhances the 1O2 yield of MB by the SPR electron from the GBPs. The GBPs@SiO2-MB nanoparticles exhibit a synergistic effect of PDT and photothermal therapies (PTT) of cancer cells under laser irradiation. This study provides a alternative strategy to improve the classic MB treatment for phototherapy application.
研究领域:
生物医学工程
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肿瘤学
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纳米医学
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高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Zhendong Li,Dongfang Liu,Yingxin Zhao,Songrong Li,Xiaocheng Wei,Fansheng Meng,Wenli Huang,Zhongfang Lei
In this study, CuO-CeO 2 was synthesized via an easy hydrothermal-calcination method and innovatively applied to peroxymonosulfate (PMS) activation for pollutants degradation under a non-radical oxidation pathway. Singlet oxygen ( 1 O 2 ) was the dominated reactive oxygen species in the CuO-CeO 2 /PMS system, leading to a dramatical degradation efficiency with Rhodamine B (RhB) as model compounds. The observed rate constant of the CuO-CeO 2 /PMS system was 7–11 times higher than that of only PMS , CeO 2 /PMS and CuO/PMS systems. Also, under the reaction conditions of 1.6 mM PMS, 0.4 g/L catalyst and initial pH 7, the degradation efficiencies of RhB, Methylene Blue , Reactive Blue 19 and atrazine were respectively up to 100%, 85.39%, 72.84% and 98.44% in 60 min. X-ray photoelectron microscopy analysis indicated that the electrons transfer between CuO and CeO 2 and the formation of oxygen vacancy in CeO 2 should be responsible for the enhanced 1 O 2 production, which involved a new non-radical oxidation pathway for PMS activation by CuO-CeO 2 catalyst. Moreover, the combination of CuO and CeO 2 increased reusability and stability of catalyst, allowing it remove more than 92% of RhB over a wide pH range (pH = 3–9). This study not only proved that CuO-CeO 2 is an efficient and stable PMS activator but also provided a new insight into PMS activation through a non-radical oxidation pathway for organic contaminants removal from wastewater.
研究领域:
环境科学
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化学工程
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催化
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水处理
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高影响因子
ANALYTICAL CHEMISTRY
·
2016
·
IF 5.886
Fengjuan Zou,Wenjuan Zhou,Weijiang Guan,Chao Lu,Ben Zhong Tang
Finding an efficient photosensitizer is crucial in ensuring a therapeutic effect of photodynamic treatment. Currently, screening of photosensitizers during photodynamic therapy is achieved by evaluating the total yield of singlet oxygen (1O2), rather than monitoring the formation dynamics of 1O2. 1O2-based chemiluminescence (CL) is a suitable method to directly monitor the generated amount of 1O2. Herein, the tetraphenylethene-sodium dodecyl sulfonate surfactant with aggregation-induced emission characteristics can remarkably amplify the intrinsic CL emission from 1O2 by integrating its micellar microenvironment with a CL energy acceptor effect in a cage-like structure. We present a new luminescence platform for the rapid screening of photosensitizers by monitoring the formation dynamics of 1O2 during photodynamic therapy. This study will not only be critical in optimizing the irradiation time during photodynamic therapy but also open a new door to the discovery of efficient photosensitizers.
研究领域:
光动力治疗
·
化学发光
·
药物化学
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生物医学工程
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PubMed
高影响因子
危险品化学品经营许可证（带存储）