JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Huiwang Dai,Wenjun Zhou,Wei Wang,Zhiqi Liu
In this study, three Co/N-C catalysts were prepared by pyrolysis of bimetallic zeolitic imidazole frameworks with different Co/Zn ratio, and the critical active Co species in peroxymonosulfate (PMS) activation was investigated. The three catalysts had distinct cobalt species but similar N configuration and graphitization degree. The Co species were distributed as single atoms (Co SAs) at a Co/Zn molar ratio of 1:8, while Co nanoclusters (Co NCs) and Co nanoparticles (NPs) would be formed with further increase in Co content. The degradation efficiency of BPA did not show correlation with the increasing of Co content in catalyst. Based on the catalytic performance comparison and reactive species detection, Co SAs was identified as active sites, which could interact with PMS to generate 1 O 2 via path of PMS→HOO*→O*→ 1 O 2 . However, the role of NCs and NPs in directly activating PMS was negligible. In addition, the increase of Co content in Co/N-C catalyst would result in mass cobalt leaching, which enhanced the BPA degradation via homogeneous catalytic reactions with Co IV as reactive species. It is an effective way to design the Co/N-C catalyst with high catalytic activity and stability via regulating the formation of Co SAs.
研究领域:
环境化学
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催化
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材料科学
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Mingyang Dai,Shaobo Liu,Xiaofei Tan,Qiang Chen,Jian Ye,Ang Sun,Ni Liu
The recycling and utilization of waste biomass resources have attracted widespread attention due to their enormous potential economic value. In this study, a magnetic zero-valent iron nanoflake-modified graphitic mesoporous carbon composite (Fe@SBCx) was prepared using ultrasound-assisted impregnation and pyrolysis strategies, and employed as an efficient peroxydisulfate (PDS) activator for the removal of the antibiotic norfloxacin (NOR) from water. The Fe@SBC 1.13 /PDS system exhibited excellent oxidation performance, achieving nearly complete removal (>99 %) of 10 mg/L NOR within 25 min. Singlet oxygen ( 1 O 2 ) and ferryl iron species (Fe(IV)) were identified as the major oxidative reactive species in the system. The formation of electron donor–acceptor complexes during the reaction facilitated the decomposition of PDS and the generation of oxidative species. Fe@SBC 1.13 demonstrated satisfactory recyclability and catalytic stability. Based on density functional theory (DFT) calculations and intermediate product analysis, the degradation pathways of NOR were proposed. Moreover, the toxicity evaluation results revealed a lower bacterial cytotoxicity in the treated drainage. Overall, this study not only enriches the theoretical research on the degradation mechanisms of fluoroquinolone antibiotics in the environment but also provides a viable approach for developing highly efficient and carbon–neutral catalysts.
研究领域:
环境科学
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材料科学
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化学工程
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高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Renchan Han,Xiangyu Wang,Min Jiang,Ping Ning,Iseult Lynch
The surface passivation deactivation and limited supply of Fe 2+ on nano zero-valent iron (nZVI, Fe 0 ) restrict activation of persulfate. Herein, L-cysteine modified cobalt-based ZIF derivative anchored Fe 0 (Fe 0 @ZIF-CoNS2) containing luxuriant oxygen vacancy (O v ) defects and bimetals was fabricated. The sintered bulk ZIF-CoNS2 and chain-shaped Fe 0 were disaggregated into rough and dispersed nanospheres, meanwhile, the loading of Fe 0 increased the specific surface area of ZIF-CoNS2 by 11 times. The peroxydisulfate (PDS) consumption efficiency of 96.11 % and the metronidazole (MNZ) removal efficiency of 96 % were achieved by the catalytic action of 0.18 g/L Fe 0 @ZIF-CoNS2. Compared than the unmodified system, the leaching concentrations of Fe and Co ions were reduced by 7.33 mg/L and 4.44 mg/L, respectively. The regulation of L-cysteine elevated the relative ratio of O v from 0.46 to 6.26 and augmented the electron transfer ability of precursor. Fe, Co and O v were identified as the main active sites, where O v played an important role as a medium in inducing sustainable generation of Fe 2+ /Co 2+ and 1 O 2 . The modified system fulfills the degradation of MNZ through plentiful 1 O 2 and scant free radical. This research offers insights into the formation of O v and enhancement of nZVI reactivity during advanced oxidation processes.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Shishu Zhu,Chao Jin,Xiaoguang Duan,Shaobin Wang,Shih-Hsin Ho
Nonradical reactions induced by nanocarbon-driven peroxydisulfate (PDS) activation recently emerge a promising strategy of groundwater remediation or wastewater treatment, whereas the involved reaction pathways remain controversial. We here investigate and differentiate the two representative nonradical mechanisms of PDS activation on graphene-like nanosheets (GNS). The template-induced GNS exhibited a high porosity of over 1200 m 2 g −1 and a few-layered turbostratic structure with graphitic microcrystals. The nonradical oxidation system (aqueous 1 O 2 and nonaqueous electron transfer) of GNS/PDS was highly-reactive, and outperformed graphene- or metal-based activators. Although singlet oxygen ( 1 O 2 ) was detected in the bulk solution, the contribution of 1 O 2 to the entire oxidation were limited (0.004–0.43% and ~6% at neutral and alkaline pH, respectively), determined by chemical probes and steady-state kinetics. Different to the reference product (benzoquinone) of phenol oxidation by photosensitive singlet oxygenation, intermediate product in GNS/PDS was benzoic acid which barely resulted from 1 O 2 oxidation. Furthermore, surface-confined electron transfer was the major oxidation pathway verified by electronic measurement. Surface adsorption rather than hydrophobic effect of organic substrates on GNS accelerated a two-electron transfer. The nonradical oxidation exhibited a dissociation constant ( p Ka)-dependent mechanism because of competitive adsorption with S 2 O 8 2− anions. The findings facilitate a thorough understanding of carbon-catalyzed persulfate activation during in situ chemical oxidation (ISCO) and provide novel insights for the selective removal of aqueous organic contaminants in a nonradical manner.
研究领域:
环境科学
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化学工程
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水处理技术
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高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Shuang Liu,Hong Wu,Huaili Zheng,Weizhen Zhang,Wei Ding,Hong Li,Chao Liu
Sulfite (S(IV))-based advanced oxidation process has attracted widespread attention due to the generation of strongly oxidizing sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) for contaminants remediation. However, the contaminant degradation by singlet oxygen ( 1 O 2 ) through a nonradical pathway was still unclear in the S(IV) activation system. Herein, a magnetic Fe 3 O 4 /g-C 3 N 4 (MCN) composite was synthesized for the utilization as a visible-light catalyst to activate S(IV) under visible-LED (Vis-LED) for the organic degradation . The incorporation of Fe 3 O 4 in g-C 3 N 4 up-regulated the photocatalytic performance in the S(IV) activation for X-3B degradation, and > 98% of X-3B (20 mg L −1 ) was degraded with the degradation rate constant ( k obs ) of 0.110 min −1 within 30 min. The SO 4 •− and 1 O 2 produced in the MCN/S(IV)/Vis-LED system were identified as the primary reactive species through the quenching experiments and electron spin resonance. Interestingly, the light-induced generation of superoxide radical (O 2 •− ) played a negligible role in the formation of 1 O 2 , and most of 1 O 2 was corroborated to be originated from SO 4 •− besides SO 5 •− , which was rarely reported in other S(IV) activation processes. The catalysts before and after utilization were characterized to further elucidate the mechanisms for the S(IV) activation. There were two possible pathways for the S(IV) activation: the electron transfer from S(IV) to the photo-generated holes and the ligand-to-metal charge-transfer (LMCT) within the surface Fe(III)−S(IV) complexes. Furthermore, the MCN/S(IV)/Vis-LED system was of high resistance to complex water matrixes (pH, inorganic anions, etc.), demonstrating its application perspective in the purification of wastewater containing organic pollutants .
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
CATALYSIS LETTERS
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2024
·Vol. 155
·期 1
·1-16
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IF 2.3
Huang Yeqiong,Song Zhi,Liu Boxia,Zhang Xiayan,Liu Jialu,Li Cheng,Han Dongxu,Xing Chuhan
After the outbreak of COVID-19, the severe threat to the entire biological environment caused by the extensive use of chloroquine phosphate (CQ) continues. In this paper, a new sol–gel method was used to inject highly active Co into the PrSmMnO 3 matrix structure to prepare a novel perovskite composite catalyst PrSmCo 0.8 Mn 0.2 O 3 with stable properties, and was used to efficiently activate monopersulfate (PMS) to produce high concentration of 1 O 2 and degrade CQ. The CQ degradation rate of 40 mg L −1 within 80 min was 97.3%, and excellent performance was maintained after 5 cycles. The fixed variable method found that the PrSmCo 0.8 Mn 0.2 O 3 /PMS system still has high efficiency and adaptability in complex water bodies. Through quenching experiments and electron paramagnetic resonance spectroscopy (EPR), we explored the PrSmCo 0.8 Mn 0.2 O 3 /PMS system. PMS is efficiently adsorbed on highly active Co, forming a high-entropy mixed interface, which promotes the decomposition of PMS and generates a large amount of ⋅O 2 − radicals. At the same time, Co–Mn synergistically and efficiently utilizes excess electrons and ⋅O 2 − radicals in the solution to produce high concentrations of 1 O 2 through disproportionation reactions, promoting the degradation of CQ. It provides new insights into the application of perovskite oxides in medical wastewater treatment. Graphical
研究领域:
环境科学
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材料科学
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医学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Yingying Zhang,Qiang Huang,Ruoting Wang,Xinjie Du,Yu Yu,Zhe Chen
Modulating the coordination environment of single-atom catalysts (SACs) and designing architectures to maximize the exposure of active sites are pivotal strategies for enhancing peroxymonosulfate (PMS) activation. The fabrication of single-atom‑iron catalysts on support with particular coordination is essential but still remains challenge. Herein, we proposed the construction of single-atom‑iron embedded in graphitic carbon nitride nanosheets (SA-Fe@C 3 N 4 ) catalyst. The layer-confined synthesis strategy realized the loading of single-atom irons and ultrathin C 3 N 4 nanosheet formation in the interlayer of layered template RUB-15. XANES analysis corroborated that the isolated iron atoms are coordinated with three nitrogen and one oxygen atoms (Fe-N 3 O 1 ). Notably, the single iron atoms within the SA-Fe@C 3 N 4 matrix serve as the predominant active sites for PMS activation. The catalyst exhibited exceptional activity for the degradation of sulfamethoxazole (SMX), achieving a mass-normalized rate constant ( k Fe ) of 1.54 × 10 5 min −1 mol −1 with high selectivity toward 1 O 2 /•O 2 − .Theoretical calculations revealed that the Fe-N 3 O 1 moiety accelerated the PMS adsorption and reduced energy barriers for the activation of PMS, thus produce key *O intermediate SO 5 •- and form 1 O 2 /•O 2 − with nearly 100% selectivity. This study supplied a simple avenue to fabricate single-atom‑iron on C 3 N 4 with regulated coordination for wastewater treatment.
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Journal of Water Process Engineering
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2026
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IF 6.7
Xiao Liu,Runze He,Jiachen Song,Xinyu Hou,Fei Wang
With the growing severity of environmental pollution, the treatment of organic wastewater and waste plastic bottles has become global concerns. This study explored the feasibility of synthesizing metal-organic composite catalysts using waste PET plastic by a microwave one-step synthesis process with only 4 h. Comprehensive characterizations confirmed that the bimetallic Cu/Mn-PET catalyst outperformed monometallic counterparts and pure BDC-derived catalysts, featuring a more regular polyhedral morphology, good crystallinity and excellent stability. XPS valence state analysis uncovered pronounced synergistic interactions between Cu and Mn. Notably, despite a relatively low specific surface area (11.75 m 2 /g), Cu/Mn-PET featured the highest active site density and exhibited minimal interfacial charge transfer resistance in electrochemical measurements. When combined with PMS-AOPs technology, Cu/Mn-PET achieved nearly 100% degradation efficiency for various pollutants (dyes, antibiotics, phenolic compounds) under optimized conditions, accompanied by substantial mineralization (TOC removal rates above 56.36%). Additionally, the Cu/Mn-PET catalyst also showed strong recyclability with low metal leaching concentrations, as well as good salt tolerance. Furthermore, it was proved that the catalytic mechanism of Cu/Mn-PET involved the combined action of free radical reactions and non-free radical reactions, but the non-free radical based 1 O 2 played a dominant role. Thus, a green and efficient PET microwave one-step conversion technology has been developed to prepare a bimetallic organic composite catalyst with high catalytic activity and stability successfully, which hold significant implications for environmental protection and resource utilization.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Liyuan Wu,Chenjing Hou,Xin Wang,Pengpeng Guo,Xiaoran Zhang,Yi Jin,Yongwei Gong,Xudan Chen,Haiyan Li
The presence of chloride ions (Cl − ) in dye wastewater can hinder the peroxymonosulfate (PMS) oxidation and lead to the abundant production of toxic adsorbable organic halogens (AOX). In this study, we investigate the detailed influence of Cl − on Rhodamine B (RhB) removal and its mechanism, and propose a potential pathway for 1 O 2 -dominated systems to inhibit AOX formation. The concentration of Cl − has a dual effect on the degradation of RhB, with low concentrations inhibiting and high concentrations promoting. Further studies have revealed that Cl − significantly impact the generation and transformation of reactive oxygen species (ROSs). EPR capturing, quenching tests, and molecular probe experiments indicate that as the Cl − concentration increases, the concentration of SO 4 − , OH and their contribution to the degradation of RhB gradually decrease, 1 O 2 slightly increase and then decrease, while HClO and chlorine radicals increase linearly. Additionally, the catalyst plays a crucial role in inhibiting AOX formation and improving the mineralization of RhB. On the one hand, introducing catalysts can alter the proportion of ROSs production. On the other hand, the in-situ generation of H 2 O 2 on the catalyst surface, through O 2 adsorption at sulfur vacancies sites, consumes the produced HClO, thereby inhibiting the formation of AOX. This study proposed a new insight into the mechanism for effective reduction of AOX content for 1 O 2 dominated non-radical PMS activation under saline 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
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Peng Chen,Yejing Gou,Jiaming Ni,Yumeng Liang,Bingqiao Yang,Feifei Jia,Shaoxian Song
Base on the strong activation activity and affinity of transition metal ions and MoS 2 for peroxymonosulfate (PMS), respectively, Co(Ⅱ)-doped MoS 2 nano-flowers (Co-MoS 2 NFs) with a great photo-response property was facilely synthesized to achieve a more efficient PMS activation for ofloxacian (OFX) degradation. It was found that Co-MoS 2 NFs exhibits superior catalytic activity for OFX degradation under visible-light irradiation, which was attributed to the synergetic effect of doped Co(Ⅱ) and photo-generated carriers to PMS activation. Besides, Co-MoS 2 NFs was able to efficiently degrade OFX within 4 cycles in the presence of PMS while leaked minute amount of Mo and Co ions, implying the excellent cycle stability of Co-MoS 2 NFs. Furthermore, SO 4 •− and 1 O 2 were detected as the primary reactive radicals for OFX degradation in the Co-MoS 2 NFs-PMS system through EPR and quenching tests. This new strategy of coupling doped Co(Ⅱ) and photo-generated carriers for more efficient PMS activation, which will greatly benefit the development of SO 4 •− -based AOPs as well as cater to the demand for environmental remediation in the future.
研究领域:
环境科学
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材料科学
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化学工程
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2026
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IF 9.2
Siyuan Zheng,Bolin Li,Jun Wang,Shanshan Huang,Simiao Wu,Zihang Wang,Guoliang Bai
Levofloxacin (LEV) residues in water are refractory and ecotoxic, while heterogeneous catalytic ozonation (HCO) systems suffer from limited efficiency and insufficient anti-interference ability. To address this, a composite catalyst, Co–Mn/CTS@NZ, was fabricated by loading Co–Mn bimetallic oxides onto chitosan-modified natural zeolite through wet impregnation–calcination to target non-radical reactive oxygen species (ROS) regulation in HCO for enhanced LEV degradation and anti-interference. Under the optimized conditions (LEV 30 mg/L, O 3 5 mg/L, catalyst 5 g, pH 6.5), the system achieved 99.55% LEV removal and 55.52% mineralization in 60 min, outperforming single ozonation significantly. The catalyst exhibited excellent anti-interference performance and operated efficiently across various real water matrices, with negligible metal leaching. Quenching experiments and electron paramagnetic resonance confirmed that 1 O 2 was the primary ROS, with ·O 2 − and ·OH acting as supplementary radicals. Characterization revealed that abundant oxygen vacancies, metal valence cycles, and surface hydroxyl groups synergistically promoted ozone activation and targeted ROS generation. This study provides a low-cost, high-efficiency catalyst for LEV-contaminated water treatment and offers a theoretical basis for targeted ROS regulation in HCO technology—breaking the reliance of traditional HCO on ·OH and advancing the practical application of advanced oxidation in antibiotic pollution control.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Jinyuan Zhang,Long Cao,Jianxin Liu,Yawen Wang,Rui Li,Xiaochao Zhang,Yunfang Wang,Caimei Fan
In general, sulfite activation systems follow a radical generation pathway and non-radical pathways are rare. Different from previous sulfite activation through reactive oxygen species (ROS) pathways, CuCo 2 O 4 -O v rich in oxygen vacancies prepared by simple NaBH 4 treatment can removal ciprofloxacin (CIP) by singlet oxygen ( 1 O 2 ) non-radical pathway and its dominant role proved by the quenching experiments, showing outstanding catalytic performance over a wide pH range. In addition, 1 O 2 has been identified to originate from: SO 5 •- , SO 4 •- , and O 2 •- . The interaction of the presence of O v on the sulfite activation of CuCo 2 O 4 was investigated through a density functional theory (DFT) calculation, electrochemical analysis and XPS. The results indicate that O v can regulate the charge distribution, facilitating electron transfer between the catalyst and sulfite, and enhancing the adsorption and activation of sulfite. Notably, the selectivity of 1 O 2 generation is influenced by O v . The possible degradation pathways of CuCo 2 O 4 -O v were analyzed using liquid chromatography-mass spectrometry (LC-MS), and the toxicity of CIP and its intermediates was assessed using ECOSAR software. Finally, experiments confirmed that CuCo 2 O 4 -O v exhibits good universality and reusability. It is the synergistic activation of sulfite and degradation CIP by singlet oxygen non-free radical pathway by CuCo 2 O 4 catalyst and oxygen vacancy that will provide a new perspective for the activation of sulfite and has good reference value.
研究领域:
环境科学
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材料科学
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催化化学
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高影响因子
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