APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 21.1
Qi Zhou,Jiale Wang,Jiaojiao Song,Hao Yan,Ruiyan Wang,Tiantian Luo
A mesoporous N-doped carbon bearing atomically dispersed Fe (Fe 1 -N-Cv) was created that uniquely couples carbon-vacancy and pore engineering to switch the electron spin state of highly accessible Fe sites from low-spin (t 2 g 5 e g 0 ) to high-spin (t 2g 3 e g 2 ), thereby unlocking superior Fenton-like activity. The material was synthesized by pyrolyzing Fe-encapsulated ZIFs under negative pressure, whereby the built-in pressure gradient simultaneously enlarged pores and generated carbon vacancies. Fe 1 -N-Cv degrades pollutants 3.89-fold faster than conventional Fe 1 -N-C, maintains > 99 % tetracycline removal and > 95 % mineralization during 240 min of continuous flow operation, operates over a pH range of 3.0–9.0, and shows stable recyclability and strong resistance to coexisting matrix constituents. Mechanistic analysis identifies a non-radical regime dominated by singlet oxygen, assisted by high-valent Fe-oxo and electron-transfer pathways, while DFT calculations show that carbon defects accelerate interfacial charge transfer and lower the free-energy barrier for PMS activation. Synergistic engineering of carbon vacancies and pores thus emerges as a powerful lever to modulate both the geometric accessibility and electronic spin state of single-atom Fe centers, directly translating into markedly enhanced Fenton-like performance. This strategy offers a promising approach for boosting single-atom-catalyst activity and robustness, advancing their practical deployment in continuous environmental remediation technologies.
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高影响因子
ANALYTICAL CHEMISTRY
·
2017
·
IF 6.32
Hao Hu,Jinyi Zhang,Yu Ding,Xinfeng Zhang,Kailai Xu,Xiandeng Hou,Peng Wu
Singlet oxygen (1O2), generated via photosensitization, has been proved to oxidize chromogenic substrates with neither H2O2 oxidation nor enzyme (horseradish peroxidase, HRP) catalysis. Of the various methods for modulation of the 1O2 generation, DNA-controlled photosensitization received great attention. Therefore, integration of the formation/deformation DNA structures with DNA-controlled photosensitization will be extremely appealing in visual biosensor developments. Here, the stable melamine-thymine complex was explored in combination with DNA-controlled photosensitization for visual detection of melamine. A T-rich single stand DNA was utilized as the recognition unit. Upon the formation of the T-M-T complex, double stand DNA was formed, which was ready for the binding of SYBR Green I and activated the photosensitization. Subsequent oxidation of TMB allowed visual detection of melamine in dairy products, with spike-recoveries ranging from 94% to 106%.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Beizhao Chen,Meng Zhang,Li Wang,Li Li,Qi Han,Xun Liu,Mengxia Wang,Bei Liu,Yi Jiang,Zhongying Wang
The singlet oxygen ( 1 O 2 )-based nonradical AOP process, realized in carbon materials after nitrogen and metal doping, has drawn much attention in recent years. However, the exclusive generation of 1 O 2 in the specialized two-dimensional (2D) catalytic membranes and the associated contaminant degradation mechanisms remain unclear. Herein, a Fe-doped crystalline carbon nitride (Fe-CCN) material without additional nitrogen doping was developed to preferentially initiate 1 O 2 -based nanoconfined oxidation of organic pollutants in the 2D Fe-CCN membrane/PMS system. Density functional theory calculation revealed that the Fe-O-N configuration formed after Fe doping altered the electronic structure of Fe centers, enhancing PMS adsorption and promoting the thermodynamically favorable generation of the –O* intermediate, leading to fast and highly selective 1 O 2 generation. EPR characterization and ROS quenching experiment also confirmed that the Fe-CCN activated PMS, generating nearly 100 % 1 O 2 . The Fe-CCN membrane/PMS system exhibited excellent resistance to natural organic matter (NOM) interference and dramatically increased Bisphenol A (BPA) degradation kinetics, approximately 590 times faster than in conventional batch systems. Enhanced 1 O 2 exposure concentration within the Fe-CCN membrane nanochannels was supported by EPR data and 1 O 2 exposure simulations. Furthermore, The Fe-CCN membrane/PMS system showed wide pH tolerance, excellent pollutant degradation performance, and high stability. This work underscores the practical significance of 1 O 2 -based oxidation reactions in membrane-confined AOPs for the rapid and efficient removal of organic contaminants from water.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Lu Zheng,Yifan Gu,Fengting Li
The rational design of transition metal and nitrogen co-doped carbon-based catalysts for the efficient removal of antibiotics through non-radical pathway of peroxymonosulfate (PMS) activation has attracted widespread attention. Herein, a magnetic hierarchical porous Fe-N-C catalyst (FeBDC-NH 2 -800) was successfully constructed by pyrolyzing the hierarchical porous precursor metal–organic framework gel (FeBDC-NH 2 ) consisting of nitrogen-containing ligands. Benefiting from the defective heterojunction structure, the catalyst exhibited effective and efficient degradation towards amoxicillin (AMX) by activating PMS to produce 1 O 2 . The degradation of AMX was up to 97.4 % within 30 min, which was 2.48 and 2.16 times more than that of FeBDC-NH 2 /PMS and nanosized Fe 3 O 4 /PMS respectively. The high degradation performance could be maintained toward low pollutant concentration conditions and cycle experiments, manifesting its possibility for practical application. Combining the data of quenching experiments, electron spin resonance spectra, electrochemical experiments, X-ray photoelectron spectra and density functional theory calculation, the mechanism was revealed that radical pathway contributed little during degradation while singlet oxygen played a significant role. The cleavage of lattice oxygen and defective heterogeneous structure of FeBDC-NH 2 -800 contributed together to promote PMS for 1 O 2 production.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Guizhou Xu,Zunyao Wang,Lin Sun,Aimin Li,Xianchuan Xie,Xueyuan Gu
Metal-free peracetic acid (PAA) activators are urgently required due to their low toxicity. Heteroatom doping is beneficial to improve the catalytic performance of carbon materials, but the activation performance of doped carbon materials on PAA and the underlying mechanism have not been reported. Herein, nitrogen and sulfur co-doped mesoporous carbons (NS-MC-x, with x representing the mass ratio of thiourea:mesoporous carbon) were fabricated and used as efficient PAA activators for 4-chlorophenol (4-CP) degradation. The NS-MC-1.0/PAA system can remove > 95 % of 4-CP within 10 min, far more than the MC/PAA system. Co-existing anions show no effect on the degradation of 4-CP, whereas humic acid has a certain degree of inhibition. Singlet oxygen ( 1 O 2 ) primarily drives the degradation of 4-CP, with a secondary contribution from a direct electron transfer process mediated by reactive surface complexes, while the contribution of radicals is minimal. In addition, NS-MC-1.0 exhibits excellent reusability for PAA activation, which is conductive to its practical application. This study facilitates further research on metal-free catalysts for PAA activation and offers fresh perspectives on the utilization of PAA in degrading emerging pollutants.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 12
·1-8
·
IF 5.479
Wang Xiao-hui,Yu Yin-xiao,Cheng Kun,Yang Wei,Liu Yuan-an,Peng Hong-shang
Conjugated polymer hybrid nanoparticles (NPs) loaded with both indocyanine green (ICG) and 1,3-diphenylisobenzofuran (DPBF) are described. The NPs are dually functional in that ICG acts as the photosensitizer, and DPBF as a probe for singlet oxygen ( 1 O 2 probe). The nanoparticle core consists of the energy donating host poly(9,9-dioctylfluorenyl-2,7-diyl)-co-(2,5-p-xylene) (PFP). The polymer is doped with the energy acceptor DPBF. Ratiometric fluorometric detection of singlet oxygen is accomplished by measurement of fluorescence at wavelengths of 415 and 458 nm. In addition, the shell of the positively charged polymeric nanoparticles was modified, via electrostatic interaction, with negatively charged PDT drugs ICG. The integrated nanoparticles of type ICG-DPBF-PFP display effective photodynamic performance under 808-nm laser irradiation. The 1 O 2 sensing behaviors of samples are evaluated based on the ratiometric fluorescent responses produced by DPBF and PFP. 1 O 2 can be fluorimetically sensed with a detection limit of 28 μM. The multifunctional nanoprobes exhibit effortless cellular uptake, superior photodynamic activity and a rapid ratiometric response to 1 O 2 .
Schematic of a dual-functional nanoplatform for photodynamic therapy (PDT) and singlet oxygen ( 1 O 2 ) feedback. It offers a new strategy for self-monitoring photodynamic ablation. FRET: fluorescence resonance energy transfer. Indocyanine green is attached in the shell of nanoparticles, and 1,3-diphenylisobenzofuran is doped into the energy donating host conjugated polymer.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wangman Yin,Xinman Tu,Xinding Lv,Li Zhang,Tingting Li,Xiaojun Wang,Jianping Zou
The photocatalytic fuel cell (PFC) can treat the increasingly severe pollution from flotation wastewater in the mining industry by simultaneously converting the chemical energy of pollutants into electricity. The inherent thermodynamic and kinetic differences in degradation pathways are crucial for governing pollutant mineralization and electricity generation in the PFC system. However, achieving simultaneous contaminant elimination and maximum energy recovery through rational pathway modulation remains challenging. Herein, oxygen vacancy-enriched heterostructured BiPO 4 /Bi 2 MoO 6 photoanode by B/P co-doping, denoted as BPO/BP-BMO, is constructed via a one-step acid-mediated solvothermal method. The in-situ heterojunction and oxygen vacancies induced by heteroatom doping effectively modulate electronic/band structures, optimize interfacial charge transfer, and enhance electron-hole pair separation efficiency. The optimal BPO/BP-BMO photoanode exhibits enhanced production of singlet oxygen ( 1 O 2 ) under visible-light irradiation, which is critical for regulating the degradation pathways of sodium isopropyl xanthate (SIPX). Experimental and theoretical studies have shown that 1 O 2 preferentially targets the -O-CSS- bond in SIPX, leading to the rapid formation of isopropanol, a compound that mineralizes quickly, while minimizing the buildup of unreactive intermediates such as ROCS₂O − . The isopropanol-oriented degradation pathway endows the BPO/BP-BMO-PFC system with 92 % degradation efficiency within 90 min and a power density of 9.7 μW cm −2 , with the latter being 1.8 times that of the Bi 2 MoO 6 -PFC system. This study demonstrates an advanced photoanode, progressing from rational defect/heterojunction design to degradation pathways regulation, thereby establishing a more effective PFC system for sustainable wastewater-to-energy conversion processes.
研究领域:
环境科学
·
光催化
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能源材料
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水污染控制
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电化学
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材料化学
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可持续能源
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ying Wu,Chi Song,Xinyan Yu,Xianbao Shen,Lijie Xu,Ying Zhang,Han Gong,Changlei Xia,Lu Gan
In this study, waste polyethylene (PP) obtained from obsoleting water purifier filter was mixed with ferric chloride hexahydrate (FeCl 3 ·6H 2 O) to prepare a series of single crystal phased iron compound incorporated carbon composites (Fe/PP-C). The prepared Fe/PP-Cx catalysts were then utilized to degrade sulfamethoxazole (SMX) in water by activating peroxymonosulfate (PMS). The results showed that with the assistance of pyrolysis temperature regulation, waste PP filter could control the crystalline phase of the iron compound in the prepared Fe/PP-Cx through releasing distinct gaseous atmospheres at respective pyrolysis temperature. When the pyrolysis temperature was set at 600 °C and 900 °C, pure phase ferric oxide (Fe 3 O 4 ) and zero-valent iron (ZVI) incorporated carbon catalysts were obtained, respectively. 0.2 g/L of Fe/PP-Cx could completely degrade 0.02 mM of SMX within 20 min, in which the toxicity of the reaction solution was also effectively reduced. In both Fe/PP-Cx/PMS systems, non-radical mechanisms dominated the SMX degradation, in which singlet oxygen played the dominant role in the Fe/PP-C600/PMS system, whereas electron transfer process was primarily responsible for SMX degradation in the Fe/PP-C900/PMS system. High-valent iron-oxo species was also involved in SMX degradation in the Fe/PP-C900/PMS system. Since Fe/PP-C600 and Fe/PP-C900 respectively activated PMS via heterogeneous and homogeneous routes, Fe/PP-C600 maintained higher longtime use stability. This study aims to present a simple approach to manipulate the nonradical organic pollutant degradation mechanisms in PMS activated system, which also provides a new strategy of utilizing waste polymer.
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RSC Advances
·
2022
·Vol. 12
·期 31
·20251-20258
·
IF 4.036
Ying Yang,Jianbo Yin,Fangsheng Tao,Yunshan Zhou,Lijuan Zhang,Yuxu Zhong,Yong'an Wang
By combining the anionic salt meso-tetra(4-carboxyphenyl)porphyrin (TCPP4−) and the Keggin polyoxometalate cation cluster [Al13O4(OH)24(H2O)12]7+ via a simple ion-exchange method, a hybrid (C48H26N4O8)[Al13O4(OH)24(H2O)12]2(OH)10·18H2O (Al13–TCPP) was prepared and thoroughly characterized as a prototype of polyoxometalate–porphyrin hybrids for the photocatalytic degradation of the mustard gas simulant 2-chloroethyl ethyl sulfide (CEES). The experimental results showed that the catalytic degradation rate of CEES in the presence of Al13–TCPP reached 96.16 and 99.01% in 180 and 90 min in methanol and methanol–water solvent mixture (v/v = 1 : 1), respectively. The reaction followed first-order reaction kinetics, and the half-life and kinetic constant in methanol and solvent mixture were 39.8 min, −0.017 min−1 and 14.7 min, −0.047 min−1. Mechanism analysis indicated that under visible light irradiation in air, CEES was degraded through a combination of oxidation and alcoholysis/hydrolysis in methanol and the methanol–water solvent mixture. The superoxide radical (O2˙−) and singlet molecular oxygen (1O2) generated by Al13–TCPP selectively oxidized CEES into a non-toxic sulfoxide. The singlet oxygen capture experiments showed that Al13–TCPP (Φ = 0.236) had a higher quantum yield of singlet oxygen generation than H4TCPP (Φ = 0.135) under visible light irradiation in air. The material Al13–TCPP has good reusability, and the degradation rate of CEES can still reach 98.37% after being recycled five times.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Shuang Liu,Chao Liu,Hejiao Zhang,Weizhen Zhang,Wei Ding,Huaili Zheng,Hong Li
The sulfite (S(IV))-based advanced oxidation process (AOP) has emerged as an appealing alternative to the traditional persulfate-based AOP for the elimination of organic contaminants from diverse water matrices. In this work, a silica reinforced ZIF-67(Co) catalyst (CZS) is fabricated, characterized and tested in the activation of S(IV) for the sulfamethoxazole (SMX) degradation. The prepared CZS demonstrates superior stability and catalytic ability for the degradation of SMX compared to ZIF-67(Co) across a broad pH range. Unlike the conventional radical-dominated oxidation systems, the CZS/S(IV) system for SMX degradation operates through a non-radical mechanism, featuring high-valent Co(IV) and singlet oxygen ( 1 O 2 ) as the predominated reactive species. The hydroxylated Co species exposed on the CZS surface is identified as the pivotal active site, realizing the S(IV) activation through a complexation-electron transfer process, resulting in the production of various reactive intermediates. Co(II) undergoes the conversion to Co(IV) by generated HSO 5 − , and 1 O 2 predominantly originates from the intermediate SO 4 •− . Profiting from the highly selective oxidation capacities of Co(IV) and 1 O 2 , the established oxidative system demonstrates a remarkable interference resistance and exhibits an exceptional decontamination performance under real-world water conditions. In short, this work provides a sustainable S(IV)-based oxidation strategy for environmental remediation via non-radical mechanism.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xiupeng Yue,Yongping Shan,Wentao Jiao,Kai Shen,Yaping Zhang
Electrokinetic (EK) delivery followed by thermal activated peroxydisulfate (PS) has turned out to be a potential in situ chemical oxidation technology for soil remediation , but the activation behavior of PS in an electrical coupled thermal environment and the effect of direct current (DC) intervention on PS in heating soil has not been explored. In this paper, a DC coupled thermal activated PS (DC-heat/PS) system was constructed to degrade Phenanthrene (Phe) in soil. The results indicated that DC could force PS to migrate in soil, changing the degradation rate-limiting step in heat/PS system from PS diffusion to PS decomposition, which greatly accelerated the degradation rate. In DC/PS system, 1 O 2 was the only reactive species directly detected at platinum (Pt)-anode, confirming that S 2 O 8 2- could not directly obtain electrons at the Pt-cathode to decompose into SO 4 •- . By comparing DC/PS and DC-heat/PS system, it was found that DC could significantly promote the conversion of SO 4 •- and •OH generated by thermal activation of PS to 1 O 2 , which was attributed to the hydrogen evolution caused by DC that destroys the reaction balance in system. It was also the fundamental reason that DC leaded to the reduction of oxidation capacity of DC-heat/PS system. Finally, the possible degradation pathways of phenanthrene were proposed on the basis of seven detected intermediates.
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高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Jialiang Liang,Jingke Wu,Pengfei Gan,Yudan Liu,Peng Zhen,Yunyi Li,Zhiwei Zhao,Wen Liu,Meiping Tong
Organophosphorus pesticides are extensively utilized worldwide, but their incomplete dephosphorization poses significant environmental risks. This study investigates the dephosphorization of dimethoate (DMT), a representative organophosphorus pesticide, using a vacuum ultraviolet system. Surprisingly, in addition to hydroxyl radicals ( • OH), non-radical processes such as photoexcitation and singlet oxygen atoms (O( 1 D)) exert more significant effects on DMT dephosphorization. The degradation kinetics of DMT demonstrate a perfect linear correlation with the radical yield in both UV-based and VUV-based advanced oxidation processes (AOPs), with greater efficacy of radical attack observed in the VUV system. This heightened efficiency is attributed to the excitation of DMT to a high-energy excited state induced by UV 185 radiation. Additionally, • OH alone is inadequate for achieving complete dephosphorization of DMT. The Fukui index and singly occupied orbital (SOMO) analysis reveal that the O( 1 D) generated by UV 185 -induced photolysis of O 2 exhibits exceptional selectivity towards P=S bonds, thereby playing an indispensable role in the dephosphorization process of DMT. This study highlights the significant contribution of non-radical pathways in DMT dephosphorization by VUV, which holds great implications for the advancement of photochemical-based AOPs.
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