JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yi Hu,Dezhi Chen,Rui Zhang,Yuan Ding,Zhong Ren,Maosheng Fu,Xiukun Cao,Guisheng Zeng
Waste-derived biochar has been emerged as promising catalysts to activate peroxymonosulfate (PMS) for the degradation of organic contaminants . Herein, passion fruit shell derived biochar (PFSC) was prepared by a one-pot pyrolysis method and used as a metal-free catalyst to activate PMS for the degradation of tetracycline hydrochloride (TC). The batch experiments indicated that the pyrolysis temperature could influence the efficiency of PFSC for the activation of PMS. In the PFSC-900 (prepared at 900 °C)/PMS system, the degradation rate of TC can reach 90.91%. The quenching test and electron paramagnetic resonance spectra revealed that the high catalytic performance of PFSC-900/PMS system was mainly attributed to the non-free radical reaction pathway containing a carbon bridge, and the TC degradation was controlled primarily by singlet oxygen-mediated oxidation . Moreover, the carboxyl group of ketones and the graphite-N atoms on PFSC-900 are the possible active sites of the non-free radical pathway including direct electron transfer or the formation of O 2 •- / 1 O 2 . This study not only shows a new type of biochar as an efficient catalyst for PMS activation but also provides a way of value-added reuse of passion fruit shell.
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高影响因子
Photodiagnosis and Photodynamic Therapy
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2021
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IF 3.631
Xianglian Liao,Chunxiu Yang,Huiyun Lin,Buhong Li
Background Singlet oxygen ( 1 O 2 ) is highly reactive to biological components such as lipids, proteins and DNA, which induces oxidative damage to cells and tissues. Natural antioxidants may function as 1 O 2 quencher to prevent 1 O 2 involved photosensitized oxidation in biological system. Methods Time-resolved measurement of 1 O 2 luminescence was employed to evaluate the 1 O 2 quenching abilities of natural antioxidants in air-statured phosphate buffered saline (PBS), including (-)-Epigallocatechin gallate (EGCG), Proanthocyanidins, L-carnosine and Vitamin C. The 1 O 2 quenching effects and rate constant of EGCG were investigated by detecting the absorption, fluorescence and 1 H-NMR spectroscopy and 1 O 2 luminescence decay curves, respectively. In addition, the protective activity of EGCG against 1 O 2 oxidative damage caused by Ce6-mediated photodynamic therapy (PDT) was verified in cells. Results EGCG, proanthocyanidins, L-carnosine and Vitamin C efficiently quenched 1 O 2 luminescence at 1270 nm. The triplet-state quenching rate constants of EGCG for Rose Bengal (RB), Chlorin e6, AlPcS and HiPorfin are 2.21 × 10 9 , 4.90 × 10 8 , 3.30 × 10 8 , 1.78 × 10 9 M −1 s −1 , while the 1 O 2 quenching rate constants are 2.80 × 10 8 , 1.50 × 10 8 , 1.30 × 10 8 , 1.70 × 10 8 M −1 s −1 , respectively. Furthermore, EGCG could effectively quench 1 O 2 production to prevent NIH/3T3 cells oxidative damage induced by Ce6-mediated PDT. Conclusions EGCG is an efficient quencher for both triplet-state photosensitizers and 1 O 2 . The quenching ability of EGCG during photosensitization for selected photosensitizers is: RB > HiPorfin > Ce6 > AlPcS. EGCG could be used to protect normal cells and tissue against oxidative damage.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
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IF 14.229
Songxue Wang,Jiayu Tian,Qiao Wang,Feng Xiao,Shanshan Gao,Wenxin Shi,Fuyi Cui
A CuO coated ceramic hollow fiber membrane with dual functionalities of membrane filtration and peroxymonosulfate (PMS) activation was successfully constructed by applying phase-inversion and dip-coating technologies. The CuO coating condition was investigated, and the optimized CuO coated ceramic hollow fiber membranes (CuO@CHFMs) exhibited excellent catalytic activity for PMS activation to depredate bisphenol A (BPA) in the presence of humic acid (HA), chloride ions (Cl − ) and bicarbonate (HCO 3 − ). Based on the scavenger experiments and electron paramagnetic resonance (EPR) analyses, the non-radical reactive oxygen species - singlet oxygen ( 1 O 2 ), rather than sulfate radicals (SO 4 •- ) or hydroxyl radicals ( • OH), was elucidated as the primary reactive species responsible for the oxidation of BPA in the system. The redox circles of Cu(II)/Cu(I) on the CuO surface of the CuO@CHFMs are mainly responsible for PMS activation and a possible degradation pathway of BPA was proposed. Moreover, the CuO@CHFMs exhibited excellent stability and reusability without tedious catalyst separation/recovery processes. This study is meaningful for the development of novel catalytic membrane with PMS activation functionality in water treatment.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Cong He,Xiangjuan Ma,Huajun Feng,Yangcheng Ding,Yijing Xia,Zhiwei Wang
A flow-through peroxymonosulfate (PMS) electro-activation system with a polyacrylonitrile-based carbon fiber (PCF) membrane anode (denoted as E-PCF-PMS system) was developed. The introduction of the PCF membrane anode enabled the flow-through electrocatalytical system to achieve a remarkable tetracycline (TC) removal of 96.0 ± 0.2 % within 15 min, with a degradation rate of 0.273 min −1 . Scavenging investigations revealed that singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen species for TC degradation in the E-PCF-PMS system, and this finding was confirmed by electron paramagnetic resonance tests. Potential degradation pathways of TC were identified according to the detected intermediates and calculations of density functional theory, and a decreasing trend in the toxicity of TC intermediates was discovered. Thanks to the 1 O 2 -dominated pathway, the constructed E-PCF-PMS system could achieve efficient TC degradation under different concentrations of several common anions (Cl − , NO 3 − , HPO 4 2− , and HCO 3 − ) and humic acid (HA). General applicability and reusability tests demonstrated the excellent practicability of the proposed system. The PMS electro-activation system offers a potential technique for high-efficient degradation of contaminants in water and wastewater.
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Environmental Technology & Innovation
·
2025
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IF 7.1
Yang Li,Yuqing Yu,Youming Diao,Yixi Li,Zihan Xie,Man Chen
The contamination of emerging organic contaminants (EOCs) in natural waters poses a serious threat to environmental and public health. Advanced oxidation processes (AOPs) based on non-radical reactive species are considered the mainstream methods for degrading EOCs. However, the catalysts used for oxidant activation often suffer from elaborate synthesis, poor stability and low selectivity. Herein, a one-pot carbonization of chitosan–FeCl 3 complexes was designed to yield Fe/Fe 3 O 4 -embedded graphitic carbon (FC900) catalyst. This catalyst was capable of activating peroxymonosulfate (PMS) for selective degradation of bisphenol A (BPA). The FC900/PMS system removed 97.8 % BPA within 40 min with a rate constant k of 0.09 min −1 , which was nine times faster than that by nano-Fe 3 O 4 /PMS. Singlet oxygen and high-valent iron-oxo species were identified as the primary reactive species with negligible •OH/SO 4 - • contribution, demonstrating a non-radical reactive species-dominated degradation process. The system showed excellent tolerance to interference from common anions and natural organic matter, and could be reused for five cycles. It achieved an oxidant utilization efficiency of 0.33 mg BPA per mg PMS, among the best surveyed PMS activator systems to date. The results provide insight into developing simple, stable and efficient catalysts for the treatment of EOCs in complex environment.
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Engineering
·
2025
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IF 11.6
Qian Hu,Shanli Wang,Kaixing Fu,Guangpeng Yang,Licong Xu,Wenbin Jiang,Minghua Wu,Wangyang Lu,Xiaomin Zhu,Jinming Luo
The singlet oxygen ( 1 O 2 )-driven nonradical oxidation pathway has shown great promise for the degradation of organic pollutants with high ionization potentials (IPs) in complex water matrices because of its longer half-life and stronger resistance to environmental interference. However, the symmetric configuration of the active sites (e.g., Fe–O–Fe) in heterogeneous catalysts largely restricts the efficacy of 1 O 2 generation during ozone activation. In this study, we constructed an asymmetric Co–O–Fe dual-site in bimetallic metal‒organic frameworks (MOFs) with enhanced electron delocalization to switch the ozone activation pathway from radical-dominant to nonradical-dominant. By combining experimental and theoretical analyses, we revealed that breaking the symmetry of iron sites with Co incorporation optimizes the local electronic structure, thereby facilitating ozone adsorption and reducing the O‒O bond scission energy barrier to produce 1 O 2 . As a result, the constructed asymmetric Co–O–Fe dual-site demonstrates impressive 6.6 and 2.0 fold increases in 1 O 2 selectivity and phenol degradation efficiency, surpassing the performance of the state-of-the-art ozonation catalysts. Furthermore, the Co–O–Fe dual-site/O 3 system could efficiently and stably remove diverse high-IP organic pollutants in complex water matrices, following a positive linear correlation ( R 2 > 0.97) between the kinetic rate constants and theoretical IP values, which further highlights the unique and critical role of 1 O 2 . This work advances the understanding and design of efficient dual-site catalysts for selective 1 O 2 generation and sustainable high-IP pollutant degradation.
研究领域:
环境化学
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催化科学
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材料科学
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水污染控制
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物理化学
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DESALINATION
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2026
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IF 9.9
Xiao Zhang,Sihan Zheng,Kai Feng,Shengtao Xu,Yulu Gao,Yongjun Sun
Functionalized carbon nitride membrane was designed within the interlayer nanochannels. • Pseudo-first-order kinetics constant for Co@2D CN membrane/PMS system reached 0.24 ms −1 . • Interlayer confinement modulated PMS activation promote generation of SO 5 ●– and produce 1 O 2 . • Membrane-based interlayer confinement addressed reaction selectivity in Fenton-like catalysis. Heterogeneous Fenton-like catalysis is a promising approach for wastewater treatment but is constrained by mass transport limitations and poor reaction selectivity. To address these challenges, an in-situ functionalized membrane with active cobalt modification on a two-dimensional carbon nitride (2D CN) substrate (Co@2D CN membrane) was designed and applied to activate peroxymonosulfate (PMS) and remove emerging organic contaminants under continuous-flow conditions. The in-situ functionalization strategy preserved the interlayer nanochannels of the 2D membrane and ensured uniform cobalt dispersion, thereby providing an efficient platform for non-radical Fenton-like catalysis under interlayer confinement. Mechanistic analysis revealed that interlayer confinement enhanced singlet oxygen ( 1 O 2 ) production by promoting electron transfer between cobalt sites and PMS to form SO 5 ●– precursors. Furthermore, density functional theory (DFT) calculations demonstrated that interlayer confinement tailored PMS adsorption and molecular configuration, facilitated electron transfer between Co sites and PMS, and lowered thermodynamic barriers of PMS activation, which accelerated the self-reaction of SO 5 ●– precursors and boosted 1 O 2 evolution. With distinctive unoccupied π* orbitals, long lifespan and selective oxidation properties, 1 O 2 greatly mitigated the interference of coexisting anions and natural organic matter (NOM). This work demonstrates that interlayer confinement efficiently promotes selective 1 O 2 production, offering a promising strategy for membrane-based nonradical Fenton-like catalysis toward practical wastewater remediation. Download: Download high-res image (312KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jin Liu,Zhirui Fan,Wenzhe Zhao,Peipei Song
Recently, escalating antibiotics contamination in aquatic environments has become a critical global threat to public health. In this study, a novel cathode catalyst (NH 2 -MIL-101(Fe)@Mel-MoPc/BC) was fabricated via hydrothermal method for efficient degradation of ofloxacin (OFX) through an electro-activated peroxymonosulfate (PMS) system. The incorporation of Mo-C and Fe/Mo-N substantially enhanced the electrocatalytic performance. The influence of various parameters, including the internal mass ratio of the catalyst, current, PMS concentration, OFX concentration, pH, as well as electrolyte concentration and type on OFX degradation were systematically evaluated. Under optimal conditions, OFX degradation reached 92.6 %, with 84.2 % total organic carbon removal, outperforming previous studies. The free radical quenching experiment and electron paramagnetic resonance analysis identified singlet oxygen ( 1 O 2 ) as the dominant active species. In situ Raman spectroscopy, high performance liquid chromatography-mass spectrometry and density functional theory calculation elucidated the degradation mechanism and pathways of OFX, including demethylation, decarboxylation, hydroxylation, and dehydrogenation, ultimately forming water, carbon dioxide, and inorganic ions. Furthermore, computational toxicology and seed germination tests confirmed significantly reduced wastewater toxicity after treatment by electro-activated PMS system based on NH 2 -MIL-101(Fe)@Mel-MoPc/BC cathode. Additionally, it also exhibited superior cyclic stability and excellent performance in various real water matrices and for other organic pollutants such as Rhodamine B, phenol, tetracycline, and dimethyl phthalate, demonstrating great application potential. This work provides valuable insights into cathode catalyst design and establishes a sustainable technology for antibiotic wastewater treatment.
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Reaction Kinetics Mechanisms and Catalysis
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2026
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IF 2.1
Sun Bai,Zhang Zhilong,Zhou Taoyou,Hong Guiyun,Wang Yun,Pan Fakang,Huang Hao,Bao Lining,Yi Mingjian,Zhu Shuguang
Zeolitic imidazolate framework-L (ZIF-L)-derived cobalt–nickel layered double hydroxide (CoNi-LDH) nanosheets are developed as a heterogeneous activator of peroxymonosulfate (PMS) for Rhodamine B (RhB) degradation. The optimized CoNi-LDH/PMS system achieves 99% RhB removal within 12 min along with an apparent rate constant ( k obs ) of 0.55 min −1 , while total organic carbon removal reaches approximately 34% at 12 min. The catalyst also retains activity toward several representative organic contaminants, during five reuse cycles, and in tap and lake water matrices. Quenching experiments, electron paramagnetic resonance, nitroblue tetrazolium probing, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy collectively indicate that PMS activation is dominated by a singlet oxygen ( 1 O 2 )-mediated non-radical pathway, with radical species making minor contributions. The results further suggest that Co/Ni redox cycling promotes PMS activation, while lattice-oxygen-related surface changes would participate in interfacial electron transfer. This study highlights a ZIF-L-derived bimetallic LDH architecture that couples rapid PMS activation with preferential 1 O 2 generation, and provides a basis for further evaluation in complex water matrices.
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Small Methods
·
2021
·Vol. 5
·期 7
·2100423
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IF 14.188
Mingzhe Shao,Dapeng Liu,Baolin Yan,Xilan Feng,Xiaojuan Zhang,Yu Zhang
Inorganic nanomaterials have attracted much attention as enzyme mimics because of simple and stable spatial conformation of those artificially synthesized nanocatalysts. Cu 2 O, as an important kind of narrow band gap semiconductor, is identified as effective as visible-light-driven photocatalysts, which can catalyze decomposition of H 2 O 2 into reactive oxygen species. Moreover, after forming Cu x O/CeO 2 hybrids, the strongly coupled interface between the two components will further improve their catalytic performance. In this paper, the authors try to construct FTO/TiO 2 /Cu x O/CeO 2 (1 < x < 2) nanohybrids with such a kind of active interface via a layer-by-layer electrodeposition strategy by aid of the following surface etching process. It is found that FTO/TiO 2 /Cu x O/CeO 2 exhibits good peroxidase mimic activity in the dark but much better performance under visible light irradiation (λ ≥ 420 nm) during catalytic oxidation of 3,3′,5,5′-tetramethylbenzidine substrates in the presence of H 2 O 2 . Detailed characterizations disclose that the construction of TiO 2 /Cu 2 O pn-heterojunctions do effectively accelerate separation of photogenerated carriers, and the formation of a highly active Cu x O/CeO 2 interface is synergistically favorable for selectively generating singlet oxygen to boost the catalytic performance of FTO/TiO 2 /Cu x O/CeO 2 .
研究领域:
材料科学
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催化化学
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纳米技术
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Kaizhi Yang,Bo Yang,Yining Su,Yang Wang,Feilong Gao,Jungang Tang,Yabin Zhang,Kezhou Yan,Yanxia Guo
FJH technology could effectively synthesize carbon-vacancy-anchored Fe 0 catalysts. • Fe 0 and carbon vacancies could synergistically activate PAA to generate 1 O 2 . • DFT calculations indicate that dual active sites enhance the adsorption of PAA. • The FJH-Fe/CGS-1600/PAA system can selectively degrade electron-rich pollutants. Singlet oxygen ( 1 O 2 ) exhibits strong resistance to interference and high selectivity toward electron-rich pollutants, making it highly promising for practical wastewater treatment. However, it remains challenging to generate 1 O 2 from activated peracetic acid (PAA) selectively. Herein, a dual-site synergistic catalyst was constructed by anchoring zero-valent iron (Fe 0 ) onto the residual carbon matrix of coal gasification slag (FJH-Fe/CGS-1600) via flash joule heating (FJH) induced transient thermal shock. Carbon vacancies act as electron traps to enhance PAA adsorption, while Fe 0 efficiently activates PAA and optimize the reaction pathway spatially, thereby promoting the generation of 1 O 2 . Consequently, the FJH-Fe/CGS-1600 achieved 95.7% degradation of bisphenol A within 60 min and demonstrated stable degradation performance across a wide pH range (5–8) and in chemical wastewater. Furthermore, it exhibited strong resistance to common anions found in chemical wastewater, high selectivity toward electron-rich pollutants, and extremely low metal leaching (< 0.1 mg L −1 ). Density functional theory (DFT) calculations reveal that carbon vacancies enhance the adsorption of the terminal oxygen in PAA (adsorption energy from −1.98 to −3.20 eV) and modulate the Fe 3d electronic structure. This research establishes a strategy for regulating non-radical species by utilizing joule heating to construct dual active sites, thereby providing a sustainable pathway for the co-treatment of coal-based solid waste and wastewater. Download: Download high-res image (134KB) Download: Download full-size image
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
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IF 24.319
Peizhen Yang,Yuhan Long,Wenli Huang,Dongfang Liu
Singlet oxygen ( 1 O 2 )-dominated advanced oxidation processes has drawn widespread attention for selective oxidation of organic pollutants in complex water environments. However, the high efficiency and selectivity of 1 O 2 generation remains challenging. Herein, we develop single-atom copper anchored on Ti 3 C 2 T x MXene nanosheets (Cu-SA/MXene) by molten salt etching for the generation of 1 O 2 via peroxymonosulfate (PMS) activation. Particularly, it exhibits a high selectivity of 99.71% toward 1 O 2 generation by activating PMS, which shows outstanding catalytic activity for multiple pollutants, and strong resistance to inorganic anions. Experimental and theoretical results reveal that the Cu single atoms with three oxygen coordination environments (Cu-O 3 ) are more favorable for PMS absorption and selectively adsorb the terminal oxygen of PMS to promote the generation of SO 5 .- , resulting in the generation of 1 O 2 . A continuous-flow wastewater system by dispersing catalysts on poly (vinylidene fluoride) membrane exhibit stable catalytic activity for polycarbonate plant wastewater treatment over 8 h.
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