NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 25
·12217-12228
·
IF 3.925
Xiaoying Yuan,Yue Leng,Changlong Fang,Kangqi Gao,Chenyu Liu,Jianjun Song,Yingshu Guo
Tetracycline hydrochloride (TC) is a typical refractory organic pollutant, and is frequently detected in different water environments, which will increase microbial drug resistance, destroy ecosystems and threaten human health. It is urgent to develop a simple and effective catalyst for TC removal. In this paper, a facile two-step calcination method was used to prepare a LaCoO3/g-C3N4 composite catalyst with high activity and high stability for PMS activation to degrade TC. Various characterization results confirmed that the LaCoO3/g-C3N4 composite catalyst possessed smaller particle size, higher stability and faster electronic transmission ability. Benefiting from the synergistic effect between LaCoO3 and g-C3N4, the LaCoO3/g-C3N4 catalyst showed high activity for PMS activation to degrade different antibiotics. Furthermore, the results of the quenching experiments and the electron paramagnetic resonance (EPR) tests showed that the generated SO4˙− and 1O2 radicals during the PMS activation process played a key role in pollutant degradation. The effect of different reaction conditions (including pH, temperature, PMS concentration, catalyst dosage and different anions) on the performance of the catalyst was also investigated. The catalyst cycle evaluation experiments showed that the LaCoO3/g-C3N4 composite catalyst has high stability and reusability. The phytotoxicity evaluation based on seed germination experiments indicated that the LaCoO3/g-C3N4 composite catalyst system can effectively reduce the toxicity of antibiotics.
研究领域:
环境科学
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材料科学
·
生物学
✓ 已验证
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·230
·
IF 4
Zhao Wang,Jawad Ali,Ajmal Shahzad,Yanan Chen,Haiqing Ma,Qiao Huang,Lei Xie,Futang Xing
Fe-based heterogeneous catalytic advanced oxidation processes show great potential for treating wastewater. However, catalyst instability often hinders their practical use, mainly due to the slow regeneration of Fe2+sites. Herein, we developed a Fe3S4/WO3catalyst, where the electron-rich Wx and Sx sites promoted efficient electron transfer, enabling continuous regeneration of Fe2+active sites on the catalyst surface. The Fe3S4/WO3catalyst exhibited outstanding degradation efficiency for tetracycline (TC) in the peroxymonosulfate (PMS) system, achieving a 92.5% removal efficiency, significantly higher than its individual components of Fe3S4(52.8%), WO3(43.1%), and WS2(53.2%). Moreover, the Fe3S4/WO3/PMS system demonstrated a broad operational pH range (3.0–9.0), excellent degradation efficiency for various emerging pollutants, minimal interference from background electrolytes and organic matter, and strong stability in real water treatment. Chemical scavenger tests and electron paramagnetic resonance (EPR) analysis confirmed that the oxidative degradation of TC was driven by multiple reactive species, including SO4•−,•OH,•O2−, and1O2. This study provides a novel strategy for regulating active sites in Fe-based catalysts to ensure sustained performance, offering a pathway for the rational design of next-generation Fenton-like catalysts for efficient and sustainable micropollutant removal from wastewater.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Shangyi Li,Jun Huang,Xukai Li,Laisheng Li
Co-Ce as the dominant active sites immobilized MCM-48 (Co-Ce/MCM-48) was fabricated via H-bonding by the hydrothermal and incipient wetness co-impregnation method. The incorporation of Co-Ce/MCM-48 (67.2%) provided higher mineralization of sulfamethazine (SMT) than Co/MCM-48 (62.2%) and Ce/MCM-48 (39.4%) in O 3 /peroxymonosulfate (O 3 /PMS) system at 90 min reaction time. The catalytic efficiency could be further improved owing to enhanced PMS decomposition rate when initial pH increased to 9.4. The electron transfer capacity in Co-Ce/MCM-48/O 3 /PMS was improved according to in-situ electrochemical tests. In situ-Raman characterization implied that PMS was bonded to the Co⋯HO-Si-O-Si-OH⋯Ce to generate the Ce-OH⋯HSO 5 − and Co-OH⋯HSO 5 − complexes, which was decomposed by O 3 and one-electron transfer reaction into reactive oxygen species (ROSs). LC-MS analysis indicated that the breakage of N-S bond, SO 2 extrusion and -CH 3 oxidation on rings were the major degradation pathway during SMT degradation. To uncover the relationship of interface electron transfer with Co-Ce/MCM-48 and PMS activation by O 3 , electron paramagnetic resonance (EPR) spectra was recorded to investigate the variation of ROSs in different processes. Simultaneous PMS reduction and oxidation over the solid-liquid-gas interface occurred for the generation of free and non-free radicals in Co-Ce/MCM-48/O 3 /PMS process.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Xuechang Ren,Suying Ding,Renhua Chen,Ning Fu
This study addresses the limited Fe 3+ /Fe 2+ conversion in homogeneous Fenton-like systems by introducing reducing MoS₂ as a co-catalyst to the Fe 3+ /PMS system, while simultaneously investigating the effect of MoS₂ crystal structure on reaction kinetics. Hydrothermally synthesized 1 T/2H-MoS₂ (denoted as M-x) significantly enhanced phenol degradation in the Fe 3+ /PMS system. Among the catalysts, M-180 demonstrated optimal performance, achieving 91.14 % phenol degradation within 20 min. XPS analysis revealed a positive correlation between 1 T-phase content and degradation efficiency, confirming that 1 T-MoS₂ facilitates Fe 3+ /Fe 2+ redox cycling to promote efficient PMS activation. Radical quenching experiments and electron paramagnetic resonance (EPR) spectroscopy further identified SO₄· − , 1 O₂, and O₂· − as the primary reactive species.
研究领域:
环境化学
·
催化
·
纳米材料
·
水处理
·
高级氧化工艺
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qingqing Shi,Yaqi Hou,Qiting Zhu,Yongmei Hao
Due to the complex structure of metal–carbon-based catalysts derived from metal-organic frameworks (MOFs), it is difficult to clarify the active sites and catalytic mechanisms. Constructing of structure–activity relationship is conducive for identifying active center, but there is still a gap in the bimetal-carbon-based catalysts/PMS systems. Here, we report a highly efficient and stable CuCo bimetal-nitrogen doped carbon catalyst (CuCo@C-N) for the activation of PMS for efficient degradation of PNP. By manipulating the catalyst structure, establishing the structure–activity relationship and combining with DFT calculation, the non-metallic active centers were determined, including defects, C=O and graphite N. Co was the only metal active center, and the presence of Cu accelerated the redox cycle of the system. The degradation of PNP was dependent on electron transfer and ROS activation. The metal active center was used to generate sulfate radicals (SO 4 •− ), and the non-metal active sites accelerated electron transfer and non-radical pathways to generate 1 O 2 .
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2024
·
IF 6.9
Zhenbo Wu,Jinjuan Xue,Zhaoxia Chen,Yiting Lv,Shuaishuai Ma,Jinku Ma,Mingxin Wang
Membrane technology for wastewater remediation has generated significant interest, however, the single functionality, dull wettability and easy fouling property of the membrane hinder its practical application. Herein, a self-cleaning and multi-use superwetting nanofiber membrane was prepared by electrospinning and subsequent spraying technique. The sulfonated cobalt phthalocyanine/NH 2 -MIL-125 (CoPcS/NMIL) heterojunction was uniformly enrobed over polyethylene terephthalate (PET) electrospun membrane derived from waste PET bottles. The unique CoPcS/NMIL heterojunction exhibited a dual driving effect in photocatalytic activity and membrane wettability. Therefore, the fabricated CoPcS/NMIL@PET composite membrane demonstrated its capability to address complex water pollution issues effectively. The composite membrane exhibited notable flux permeation ability (538–3180 L m −2 h −1 ) and achieved excellent separation efficiency of over 99 % for diverse oil-in-water emulsions under the gravity filtration condition. Notably, the membrane can efficiently deal with stubborn high-viscosity crude oil fouling profiting from the photocatalytic self-cleaning function. A high flux recovery ratio of 93.6 % and a low irreversible fouling resistance ratio of 6.4 % can be obtained after 30 min of visible light irradiation. Impressively, CoPcS/NMIL@PET membrane exhibited enhanced permeation flux, separation efficiency and self-cleaning capacity compared to NMIL@PET membrane. Meanwhile, the CoPcS/NMIL@PET-activated peroxomonosulfate (PMS) system exhibited extremely high degradation performance for RhB under visible light with the degradation efficiency of 98 % within 10 min, suggesting its potential in the rapid purification of water-soluble organic pollutants . In addition, the CoPcS/NMIL@PET membrane has good chemical stability and mechanical properties for potential long-term use. Moreover, the demulsification mechanism in oil-water separation and PMS-photocatalysis synergetic mechanism over the fabricated CoPcS/NMIL@PET membrane were also investigated in detail. The research offers a promising approach for the design and fabrication of novel nanofiber membranes that incorporate photosensitizers and MOFs functional surfaces to address the challenges associated with such wastewater treatment .
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Song Cheng,Yutao Liu,Xinyi Liu,Changqing Zhu,Jingyang Luo,Jiashun Cao,Fuqiang Liu
Electro-assisted activation of peroxymonosulfate (EA-PMS) by transition metals oxides (TMOs) has been extensively studied for the removal of organic pollutants. Despite TMOs possess considerable activity and affinity to PMS, their poor bulk conductivity still limits the electron exchange during the TM δ/δ+1 redox cycle, especially the efficient reduction of TM δ+1 via cathodic process. In this study, carbon felt loaded with modified Co 3 O 4 nanosheets (Co@FCF) was fabricated and applied as the flow-through electrode of EA-PMS process, where the Co 3 O 4 nanosheets were embedded with numerous metallic Ni particles encapsulated within carbon layers (Ni@C). Driven by weak electric current, continuous electrons can be supplied to the bulk Co 3 O 4 from the electron-rich Ni@C nanoparticles, resulting in accelerated Co 3+ /Co 2+ cycle, enhanced production of SO 4 ·− and improved energy utilization efficiency. Electrochemical tests along with density functional theory calculations indicate that the unique structure of Co@FCF played essential role in the enhanced performance.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
·
2025
·
IF 5.1
Liu Ouyang,Huihu Wang,Lizhong Duan,Jingle Zhang,Shenghao Jiang,Yu Xiong,Chenhuinan Wei,Xing Xiang,Yun Zhao,Qianyu Wang
Tetracycline (TC), a widely detected aquatic pollutant, poses significant ecological risks, necessitating the development of effective remediation strategies. Photocatalytic degradation, which converts TC into harmless CO 2 and H 2 O, offers a promising eco-friendly solution. This study successfully synthesized a novel 2D/3D g-C 3 N 5 /BiVO 4 (N-CN/BiVO 4 ) S-scheme heterojunction via a hydrothermal method. The optimized 5 % N-CN/BiVO 4 exhibited exceptional performance in activating the Fe 2+ /PMS system under visible light, achieving a 96.8 % TC removal efficiency with an apparent rate constant 4.4 times higher than that of BiVO 4 . Mechanistic studies, including ultraviolet photoelectron spectroscopy (UPS) and valence band X-ray photoelectron spectroscopy (VB-XPS), confirmed the S-scheme interfacial charge transfer pathway. Furthermore, radical quenching experiments revealed that the enhanced photocatalytic activity originated from the synergistic contribution of multiple reactive species ( OH, SO 4 − , O 2 − , h + , and 1 O 2 ), validating both the efficient activation of Fe 2+ /PMS and the proposed S-scheme charge transfer mechanism. This work presents an innovative approach for high-performance pollutant degradation by coupling an S-scheme heterojunction with the Fe 2+ /PMS activation system.
研究领域:
环境科学
·
光催化
·
水污染修复
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 5
·1284-1296
·
IF 7.3
Yuxuan Lin,Weihua Qin,Yuwei Lu,Mingye Ren,Pan Gao,Feng Xiao,Shaoxia Yang
Improving the performance of single-atom catalysts (SACs) is still challenging in Fenton-like reactions for degrading refractory organic pollutants. Here, we designed P and N co-doped Fe SACs to regulate the electronic structure of Fe active sites and enhance the reaction kinetics of peroxymonosulfate (PMS) activation. The obtained heteroatom-doped Fe SACs for the first time exhibited an ultra-low activation energy (ca. 3.7 kJ mol−1) and excellent degradation efficiency for bisphenol A (BPA) in a wide pH range (4.3–9.2). The superior reaction kinetics of the Fe SACs were attributed to enriching the electron density of atomic Fe and then forming dual electron-rich/-deficient sites, which accelerated the electron transformation to generate reactive oxygen species (ROS). In this study the heteroatom-doped Fe SACs with rapid reaction kinetics are achieved, and provides an idea to design SACs with superior performance in heterogeneous Fenton-like reactions.
研究领域:
环境科学
·
催化
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
iScience
·
2023
·
IF 5.8
Xiai Zhang,Wenquan Zhang,Xinwei Zhang,Jun Li,Tong Wang,Qikui Fan,Hao Zhu,Zhimao Yang,Chuncai Kong
Peroxymonosulfate (PMS)-based advanced oxidation processes in liquid phase systems can actively degrade toluene. In this work, the catechol structural surfactant was introduced to synthesize the dispersed and homogeneous CoFe 2 O 4 nanospheres and embedded into MoS 2 nanoflowers to form magnetically separable heterojunction catalysts. The innovative approach effectively mitigated the traditionally low reduction efficiency of transition metal ions during the heterogeneous activation process. In CoFe 2 O 4 /MoS 2 /PMS system, the toluene removal efficiency remained 95% within 2 h. The contribution of SO 4 ⋅- , ·O 2 - , ·OH, and 1 O 2 was revealed by radical quenching experiment and electron paramagnetic resonance spectroscopy. The results illustrated that MoS 2 offers ample reduction sites for facilitating PMS activation via Fe 3+ /Fe 2+ redox interactions. Furthermore, an investigation into the toluene degradation pathway within the CoFe 2 O 4 /MoS 2 /PMS system revealed its capability to suppress the formation of toxic byproducts. This ambient-temperature liquid-phase method presented promising route for the removal of industrial volatile organic pollutants.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Mingjun Xie,Yuying Han,Na Wang,Zixuan Huang,Congting Sun
The efficient elimination of recalcitrant synthetic dyes from complex waters remains a pressing challenge for advanced oxidation processes (AOPs). Herein, an Fe-MOFs-derives@BC composite was fabricated by anchoring MIL-101(Fe) crystals onto rice-straw biochar followed by high-temperature carbonization. XRD, SEM and XPS confirm the formation of a crystal–amorphous hybrid in which residual MIL-101(Fe) nanocrystallites are embedded within a conductive carbon matrix rich in oxygen vacancies. The composite rapidly activates PMS via a synergistic Fe(II)/Fe(III) redox cycle and carbon-facilitated electron transfer, generating SO₄• − , •OH, and 1 O₂ to driving Rhodamine B (RhB) and Malachite Green (MG) degradation. Under optimal conditions (0.1 g L −1 catalyst, 0.1 g L −1 PMS), >90% RhB and MG were removed within 15 min across deionised, groundwater, lake and river matrices; even in the most complex river water, 90% removal is achieved in 10 min. When Fe-MOFs-derives@BC is immobilised in a poly (vinylidene fluoride) membrane, a continuous-flow micro-reactor maintains >90% removal over 600 min with negligible flux decline and undetectable Fe leaching. This hybrid radical/non-radical pathway, broad matrix tolerance and long-term membrane stability position Fe MOFs-derives@BC/PMS as a robust, scalable platform for advanced wastewater treatment.
研究领域:
环境工程
·
材料科学
·
化学工程
·
水处理技术
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2021
·
IF 6.291
Guomin Geng,Yanhui Gao,Zhitong Zhang,Kangqi Gao,Wenyu Zhang,Jianjun Song
Developing monolithic carbon-based catalyst with low cost, easy separation and high performance to degrade pollutants via PMS activation is crucial. In this work, a series of novel monolithic Me-CA catalysts based on biomass derived carbon aerogel were prepared by hydrothermal method using waste watermelon peel as raw material. Co-CA catalyst showed excellent performance to activate PMS for 2, 4-DCP degradation in different temperature and different water matrices. Different pollutants, such as ciprofloxacin (CIP), bisphenol A (BPA), and 2, 4-dichlorophenoxyacetic acid (2, 4-D) could also be removed in the Co-CA/PMS system. As expected, Co-CA could be easily separated from degraded solution, and show high stability and reusability for PMS activation with a lower cobalt leaching. Based on the results of the quenching tests, electron paramagnetic resonance (EPR) spectra, Chronoamperometric test (i-t curves) and electro-chemical impedance spectroscopy (EIS), the PMS activation mechanism was proposed. The phytotoxicity assessment determined by germination situation of mung bean indicated that PMS activation could eliminate the hazards of 2, 4-D. Therefore, this study provides a low cost, efficient and environmental-friendly monolithic biomass carbon aerogel catalyst for different pollutants degradation , which further advances monolithic catalyst for practical wastewater treatment .
研究领域:
环境科学
·
材料科学
·
化学工程
·
废水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）