Small
·
2025
·
IF 12.1
Fukang Feng,Xiaoyu Zhang,Xinrui Han,Guangyu Wu,Weinan Xing
The efficiency of peroxymonosulfate (PMS) activation in photocatalytic processes critically depends on the regulation of electron transfer from generation to utilization. Herein, a holistic electron transfer pathway is constructed within a metal–organic frameworks (MOFs)-derived Cu-Cu x O/TiO 2 composite to achieve superior PMS activation. The incorporated Cu species serve as dynamic redox mediators, enabling an efficient non-photoinduced electron transfer pathway via Cu 0 &Cu n+ cycling. Simultaneously, the Cu-induced bandgap narrowing and abundant oxygen vacancies significantly enhance visible-light absorption and facilitate the rapid trapping of photogenerated electrons. This synergy establishes a continuous and highly efficient electron transfer from photoexcitation to catalytic reaction. The optimized catalyst Cu-Cu x O/TiO 2 -2 delivers an exceptional tetracycline hydrochloride (TC) degradation rate constant of 38.26 × 10 −3 min −1 , representing a 2.04-fold enhancement over pristine TiO 2 (18.74 × 10 −3 min −1 ). Mechanistic studies confirm that the radical ( • OH/ • SO 4 − ) and non-radical (h⁺) pathways function synergistically in the Cu-Cu x O/TiO 2 -2/PMS system, collectively enabling highly efficient TC degradation. Three plausible degradation routes are proposed based on intermediates identification and density functional theory (DFT) calculations. Furthermore, economic analysis is conducted to transition from mechanistic insight to practical value, assessing the commercial potential of the Cu-Cu x O/TiO 2 -2/PMS photodegradation system. This work provides valuable insights into the design of efficient composite catalysts through regulated electron transfer via dynamic redox cycling coupled with oxygen vacancy engineering.
研究领域:
环境科学
·
材料化学
·
光催化
·
废水处理
·
纳米材料
·
氧化还原化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Shengwen Zhou,Rui Yang,He Yan,Guixian Zhu,Xingwu Lu,Xiuwen Cheng
The development of a low-cost catalytic system using waste copper slag to activate peroxymonosulfate (PMS) for tetracycline (TC) degradation in water represents a green and efficient pathway. In this study, magnetic FeOOH@Fe₃O₄ nanoparticles were synthesized from copper slag and applied in a material/PMS system to degrade TC. Experimental results demonstrated a remarkable 99 % TC removal efficiency within 30 min. Characterization analysis revealed that the amorphous structure of FeOOH promotes the formation of amorphous zones and multiphase interfaces, thereby exposing more active sites and enhancing catalytic activity. This effect, combined with the large specific surface area of Fe₃O₄, significantly accelerated the degradation rate. Notably, the material maintained an 80 % degradation efficiency even after five reuse cycles. The reaction mechanism involves multiple pathways, including free radical and non-free radical mechanisms, as well as adsorption and electron transfer, with the non-radical singlet oxygen ( 1 O₂) being the predominant reactive species. Furthermore, the study proposes potential degradation intermediates and outlines possible degradation pathways for TC, while also predicting associated toxicity changes. This research provides a novel methodology for developing environmental functional materials from solid waste, offering valuable insights for addressing the dual challenges of waste disposal and the degradation of emerging pollutants.
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2021
·
IF 5.876
Fan Nie,Wenyue Xu,Di Zhang,Baizhi Jiang,Qi Sun,Junwei Wang
The N-doped two-dimensional (2D) carbon-based catalysts play a crucial role in the PMS catalytic activity of advanced oxidation processes (AOPs). However, their activation mechanism still lacks a reasonable explanation. A low-cost and one-step synthesis of N-doped graphite-2H nanoplatelets (N-GNPs) were prepared through the calcination under 600°C. N-GNPs 0.5 -600 was applied to activate permonosulfate (PMS) 19.4 times faster than that of pure PMS system under visible light to degrade bis(monochloro-s-triazine) reactive dye. We first demonstrate that electron arrangement in N-GNPs samples can effectively activate PMS and generate 1 O 2 as much as S O 4 · − and HO · as the main reactive species. The EPR test results were consistent with the quenching test. Density functional theory (DFT) calculations showed the graphite N adjacent C atoms (Eb= -8.9 eV) were promoted to produce more active sites. Bidirectional regulation of graphite N bonded C atoms form a local electron state, making the C most active electron donation. The 2P Z orbital of carbon atoms becomes occupied with the free electrons. The localized orbitals lead to the stronger Columbic repulsion of π electrons and enlarged interlayer distance, making it easier for the electrons to give out and accelerate the free-radical process.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Yang Zhou,Jin Jiang,Yuan Gao,Su-Yan Pang,Jun Ma,Jiebin Duan,Qin Guo,Juan Li,Yue Yang
Recently, in situ chemical oxidation (ISCO) using peroxymonosulfate (PMS) for environmental decontamination has received increasing interest. In this study, oxidation kinetics and products of four steroid estrogens (i.e., estrone, 17β-estradiol, estriol, and 17α-ethinylestradiol) by PMS under various conditions were investigated. PMS could fairly degrade steroid estrogens over the pH range of 7–10, and the degradation rate increased with the increase of solution pH. This pH-dependence was well described by parallel reactions between individual acid-base species of steroid estrogens (E and E − ) and PMS (HSO 5 − and SO 5 2− ), where specific second-order rate constants for E − with HSO 5 − and SO 5 2− were in the range of 2.11–5.58 M −1 s −1 and 0.77–1.25 M −1 s −1 , respectively. Identification of oxidation products by liquid chromatography/electrospray ionization quadrupole time-of-flight mass spectrometer showed that PMS readily oxidized the phenolic group of steroid estrogens, leading to the generation of hydroxylated and ring-opening products. The presence of bromide and chloride ions (Br − and Cl − ) at environmentally relevant levels could greatly accelerate the degradation of steroid estrogens by PMS with the formation of halogenated aromatic products. This effect was quantitatively estimated by a kinetic model, where the formation of free bromine and chorine and their rapid electrophilic substitution with steroid estrogens were taken into consideration. Eco-toxicity of transformation products of 17α-ethinylestradiol by PMS treatment in the absence and presence of bromide and chloride was estimated by quantitative structure–activity relationship analysis using ECOSAR. These findings advance the understanding of ISCO using PMS.
✓ 已验证
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2026
·
IF 6.6
Limin Chen,Jinfang Hu,Yulai He,Juncang Wang,Ye Hong,Wenjin Chen
The advancement of cost-effective, non-metal-doped catalysts is essential for the effective degradation of aquatic contaminants. In this study, hollow carbon spheres (HCS) were synthesized from glucose using the soft stencil method. These HCS were subsequently co-doped with nitrogen and phosphorus using ammonium dihydrogen phosphate ((NH 4 ) 2 HPO 4 ) as the doping source, resulting in N, P co-doped hollow carbon spheres (NPHCS). These NPHCS served as a mediator for peroxymonosulfate (PMS) activation, applied in the degradation of tetracycline hydrochloride (TC). The unique architecture of NPHCS, characterized by hollow 3D cavities and mesoporous channels, established a spatially confined environment that markedly increased total surface exposure and number of reactive centers. This structure facilitated rapid adsorption and activation of PMS on the catalyst surface, generating reactive oxygen species more efficiently compared to unrestricted nitrogen and phosphorus-doped carbon nanosheets (NPCN) and carbon black (NPCB). The confined nano-environment of the hollow cavities shortened mass transfer pathways, substantially improving the contact and catalytic efficiency between active oxygen species and pollutants. Consequently, over 90% of TC was degraded within 20 min. This research offers a novel insight into the design of low-cost, N, P co-doped catalytic nanoreactors for improving the catalytic efficiency in non-metal-based systems.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 50
·108538-108552
·
IF 5.8
Wang Yongqiang,Bai Yibo,Han Che,Li Zaimei,Lun Xiaowen,Zhang Conglu
Graphite-like carbon nitride (g-C 3 N 4 ) is favored for its excellent physicochemical properties. However, the high complexation rate of photogenerated carriers greatly limits its practical applications. Based on this, a novel CQDs-doped carbon nitride nanosheets composite (CNS/CQDs) was prepared and applied to the visible light–induced activation of peroxymonosulfate (PMS) for meloxicam (Mel) and tetracycline (TC) degradation. The photocatalytic degradation of Mel and TC were remarkably promoted in the CNS/CQDs+PMS+vis system. Mel photodegradation of 99.90% was achieved over 30 min with 20 mg CNS/CQDs and 20 mg PMS at pH11. And TC photodegradation of 95.97% was achieved over 45 min with 20 mg CNS/CQDs and 20 mg PMS at nature pH6.5. The TOC mineralization rates of Mel and TC were 75.49% and 52.00%, respectively. The transient photocurrent response and electrochemical impedance measurements (EIS) results indicated that the doping of CQDs could improve the charge transfer efficiency of pure g-C 3 N 4 , and CNS/CQDs had a low charge transfer resistance. Capture experiments and EPR tests explored the effective actives in the CNS/CQDs+PMS+vis system. Possible degradation pathways of Mel were also analyzed. This study provides valid residual drugs degradation under the dual conditions of visible light catalytic oxidation and persulfate oxidation, which will be a novel perspective for advanced oxidation technology to effectively remove organic pollutants from water.
研究领域:
环境科学
·
光催化化学
·
水处理技术
·
纳米材料
·
高级氧化工艺
·
药物代谢
·
环境污染物降解
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2026
·Vol. 156
·期 6
·169
·
IF 2.5
Wang Mei,Wu Tong,Song Xianghai,Bu Quan,Zhou Bingliang
This study presents a high-performance cobalt catalyst supported on microwave-pyrolyzed biochar (Co/MPC) for efficient peroxymonosulfate (PMS) activation to degrade atrazine (ATZ). The microwave-assisted pyrolysis (MWP) technique yielded biochar (MPC) with superior textural properties—specifically, a significantly higher specific surface area (214.18 m 2 /g) and pore volume (0.46 cm 3 /g)—compared to conventionally pyrolyzed biochar (BC). This enhanced porous structure facilitated the uniform dispersion of ~5 nm cobalt nanoparticles, resulting in the highly active Co/MPC catalyst. The Co/MPC+PMS system achieved over 99% ATZ degradation within just 4 min, outperforming its conventionally prepared counterpart (Co/BC) (77%). The catalyst demonstrated robust performance across a range of PMS dosages and pollutant concentrations, with minimal interference from coexisting inorganic ions (Cl − , SO 4 2− , NO 3 − , H 2 PO 4 − , HCO 3 − ) and organic humic acid in the Co/MPC+PMS system. Radical quenching experiments and electron paramagnetic resonance (EPR) analysis identified hydroxyl radicals (⋅OH) and sulfate radicals (SO₄⋅⁻) as the dominant reactive species responsible for the rapid degradation. This work highlights the significant advantage of microwave-assisted synthesis in creating advanced carbon-metal catalysts and offers a highly efficient, stable, and practical solution for the remediation of persistent organic pollutants like ATZ without requiring additional energy input. Graphical The alternative text for this image may have been generated using AI. Microwave-assisted preparation of Co/MPC for efficient PMS activation towards atrazine degradation.
✓ 已验证
DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2026
·
IF 5.2
Huan Song,Le Song,Fangzhou Wu,Yonglei Xing,Xiaoyong Jin,Gang Ni
Nitrogen-doped carbon materials are efficient metal-free catalysts for activating peroxymonosulfate (PMS) in advanced oxidation processes (AOPs). Herein, a honeycomb-like N-doped porous carbon catalyst (CG2N2) was synthesized via pyrolysis using trisodium citrate, glucose, and 3-amino-1,2,4-triazole (3-AT). This catalyst has a large specific surface area, rich active sites (pyrrolic N, C=O) and excellent electron-transfer ability, and outstanding PMS activation performance for organic pollutant degradation. A striking novelty lies in the unprecedented synergistic effect of naturally ubiquitous carbonate (CO 3 2− ) and CG2N2 for PMS activation, which not only accelerates reaction kinetics but also stabilizes catalytic active sites and reshapes the degradation pathway. Experimental results show that CG2N2 completely degrades 20 mg L −1 phenol within 10 min, and the addition of 10 mM CO 3 2− boosts degradation to 100% removal in only 2 min, with the apparent reaction rate constant soaring from 0.853 to 3.426 min −1 . Meanwhile, CO 3 2− significantly enhances the stability of the catalytic system. Systematic characterization reveals that CO 3 2− accelerates PMS decomposition and reactive oxygen species (ROS) generation, while preserving active sites to stabilize the catalyst. Density functional theory (DFT) calculations verify that CO 3 2− strengthens PMS adsorption on the catalyst surface (adsorption energy reduced from −1.52 eV to −1.67 eV) and weakens the O–O bond, theoretically supporting accelerated reaction kinetics. Another innovative finding is that CO 3 2− drives the system from a radical-dominated pathway to a non-radical electron-transfer pathway dominated by the surface-bound CG2N2/PMS∗ intermediate, reducing matrix interference and enabling selective degradation of phenolic pollutants. CG2N2 also shows broad-spectrum degradation ability toward various phenolic pollutants, with CO 3 2− further enhancing efficiency for most targets. This study breaks through the limitation of conventional metal-free PMS activation systems by utilizing naturally abundant carbonate as a synergistic accelerator, providing a highly efficient, sustainable, and matrix-adaptive strategy for organic pollutant removal in complex water matrices.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Zhenzhou Wang,Qing Zuo,Fang Deng,Zhengrong Zhao,Lei Wu,Longshuai Zhang,Wei Ren,Yongcai Zhang,Xubiao Luo,Jianping Zou
A novel “pollutant-triggered catalysis” paradigm is proposed, using pre-adsorbed pollutants as electronic modulators to optimize peroxymonosulfate (PMS) activation over mono-disperse iron single atoms anchored on porous carbon nitride (Fe SAC /CN) for water remediation, unlike conventional strategies treating contaminants as passive targets. Catalytic tests, spectroscopic analyses, and density functional theory calculations were integrated to clarify the effect of pre-adsorbed electron-rich 4-chlorophenol on the electronic configuration of Fe sites and the PMS activation mechanism. The pre-adsorbed pollutant enhanced Fe-site Bader charge transfer and upshifted the Fe 3d-band center, thereby strengthening PMS adsorption, lowering the activation barrier, shifting the dominant pathway toward Fe(IV)=O and 1 O 2 rather than radicals, enabling 100% 4-chlorophenol removal within 15 min, and yielding a 5.34-fold rate enhancement over pristine Fe SAC /CN. The results reveal that substrate-induced electronic modulation of single-atom Fe sites is a viable route to regulate reactive species generation and improve catalytic performance. By redefining contaminants as active electronic modulators, this work offers a scalable paradigm for sustainable water remediation that simultaneously enhances oxidation capacity and environmental applicability.
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2026
·
IF 6
Shuai He,Yan Zhu,Ran Lei,Feng Qin,Guicheng Jiang,Bin Yang,Wenwu Cao
With the fast progress of ultrasonic transducer applications, higher and higher requirements have been put forward to the performance of the piezoelectric ceramics applied in this field. For power-type ceramics, not only high Q m is needed to reduce the heat and improve the power capacity, but also high d 33 is needed to provide the stronger driving force. In this work, a conventional ternary solid-solution ceramic system (0.05 Pb(Mn 1/3 Sb 2/3 )O 3 -0.47PbZrO 3 -0.48PbTiO 3 ) modified by ZnO and Li 2 CO 3 ( x wt % ZnO + y wt % Li 2 CO 3 ) (designated as: 0.05PMS-0.95PZT + x wt % ZnO + y wt % Li 2 CO 3 ) ( x , y = 0-0.3) was fabricated and researched. The combination of A-site doping of Li 2 CO 3 and B-site doping of ZnO was discovered to be able to enhance the piezoelectric coefficient ( d 33 ) effectively over 500 pC/N and maintain the mechanical quality factor ( Q m ) above 1000 simultaneously. The ZnO act as acceptor dopant to enhance the content of oxygen vacancies but facilitate the motion of domain walls to improve the piezoelectricity. Meanwhile, the A-site substitution of Li + construct an internal biased field to stabilize the domain structure leading to the relatively high Q m . Additionally, The Li 2 CO 3 also worked as sintering aid to form liquid transition phase to improve the densification process. The phase composition, microstructures of natural surfaces and fractured surfaces, electrical properties of ceramics were characterized systematically. The excellent comprehensive piezoelectric properties ( d 33 = 525 pC/N, Q m = 1064, k p = 0.63, T c = 320 °C, tan δ = 0.3% (at 25 °C), ε r = 1344) were achieved in the 0.2 wt % ZnO and 0.2 wt % Li 2 CO 3 co-doped 0.05PMS-0.95PZT ceramic sintered at 1075 °C. These advantages make 0.05PMS-0.95PZT + 0.2 wt% (ZnO and Li 2 CO 3 ) a promising alternative for the improvement and production of high-performance ultrasonic transducers applied in power-type applications.
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Haidong Zeng,Yingxin Zhang,Tianyu Zhou,Chunbo Liu,Dongshu Sun
In-situ preparing robust CoFe 2 O 4 /PCN PMS activator for multi-pollutant degradation. • Complete degradation TC within 3 min with the rate constant 24-fold higher than CN • Degradation intermediates, routes and toxicity were explored • Wide light absorption, exposed active sites, and charge behavior boost photocatalysis Facing the urgent environmental crisis, it is imperative to create an efficient and robust technology for treating diverse pollutants in aquatic environments. Herein, a CoFe 2 O 4 /PCN composite was designed via a facile in-situ growth method, in which CoFe 2 O 4 uniformly grows on carbon nitride. This architecture not only forms a close interface that facilitates efficient charge separation and migration, but also introduces abundant mixed-valence metal sites, that serve as superior active centers for peroxymonosulfate (PMS) activation and subsequent organic pollutant removal. Specifically, under visible light, the optimized catalyst can 100% degrade TC within 3 min (complete degrade rhodamine B within 20 s, methyl orange within 40 s, and methylene blue within 3 min), and the rate constant was 24-fold higher than pristine CN, surpassing most reported catalysts. The catalyst also demonstrates excellent recyclability and broad pH adaptability. The mechanism behind the performance enhancement stems from the significantly broadened light absorption (supported by UV–vis DRS), fully exposed active sites (evidenced by SEM/TEM/AFM and N₂ adsorption), and enhanced charge behaviors (supported by PCR, EIS, PL/TRPL and KPFM), especially caused by strong internal electric field. At last, the active species, degradation intermediates and their toxicity were investigated using TC degradation as a model, coupled with DFT theoretical calculations. This work proposes a rational design strategy toward constructing efficient and robust photocatalysts, revealing significant promise for water remediation. Download: Download high-res image (269KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2026
·
IF 6
Naxiang Wang,Pengxin Li,Yuntian Wan,Zhi Zhu,Yan Yan,Xu Yan,Wei Peng,Yan Guo
Accelerating the M n+ /M n+1 redox cycling and enhancing electron‐transfer efficiency during peroxymonosulfate (PMS) activation remain major challenges in advanced oxidation processes. In this work, a trimetallic nickel-cobalt-iron Prussian blue analogue (NiCoFe-PBA) precursor was synthesized via a co-precipitation method, followed by calcination and subsequent hydrothermal sulphuration, yielding a catalyst capable of photo-synergistic PMS activation for the degradation of levofloxacin (LEV). Oxygen vacancies were generated through the partial removal of lattice oxygen during air calcination and were further enriched by sulfur ion incorporation via hydrothermal sulfidation, which induces anion exchange and lattice distortion. Structural characterizations and catalytic experiments consistently confirm that NiCoFe-PBA-O-S possesses a markedly increased oxygen-vacancy density. Notably, the combined effects of sulfur species, Ni incorporation, and visible-light excitation markedly facilitated Fe 3+ /Fe 2+ and Co 3+ /Co 2+ redox cycling by enhancing interfacial electron transfer, enabling efficient photo-synergistic PMS activation. Consequently, 100% LEV removal was achieved within 30 min, with a high degradation rate constant of 0.46 min −1 , surpassing most reported catalysts. More importantly, the catalyst retained over 80% LEV removal efficiency within 30 min after eight reuse cycles, and after sulfur regeneration, the 30 min removal efficiency recovered to above 90%. Mechanistic investigations demonstrated that the degradation process was predominantly governed by reactive species in the order O 2 • - > 1 O 2 > SO 4 • - > •OH. This work provides a generalizable strategy for designing recyclable, high-efficiency heterogeneous catalysts for wastewater treatment applications.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）