Sustainability
·
2025
·Vol. 17
·期 21
·9886
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IF 3.3
Chuqiao Sha,Fangkui Cheng,Shen Luo,Chao Zhou,Hong Zhang
CoFe2O4loaded onto red brick powder (CoFe2O4@RBP) was synthesized via coprecipitation followed by post-calcination and employed as a heterogeneous catalyst to activate peroxymonosulfate (PMS) for the degradation of methylene blue (MB), thereby valorizing red brick demolition waste within a circular economy pathway and aligning the study with sustainability-oriented resource recovery. The effects of pH, PMS concentration, catalyst dosage, and coexisting substances on MB removal were systematically investigated. Complete MB removal was achieved within 30 min, and the apparent rate constant for the CoFe2O4@RBP/PMS system was 0.22 min−1—slightly lower than that of CoFe2O4/PMS—while Co leaching was markedly reduced. The process performed well across a broad pH range (3.0–9.0). EPR and radical-quenching experiments indicate that SO4•−and HO• play a minor role, whereas the Co(II)–PMS complex is primarily responsible for MB degradation; accordingly, common coexisting species (SO42−, Cl−, NO3−, humic acid) exert negligible effects. The catalyst also maintained strong durability across numerous repetitions. These results highlight a cost-efficient route to PMS activation by coupling CoFe2O4with construction waste-derived supports.
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ACS ES&T Water
·
2025
·
IF 4.3
Yin Li,Jiahui Hu,Lin Lin,Bing Li,Xiao-yan Li
Transition metal-activated peroxymonosulfate (PMS) processes are extensively studied for pollutant degradation, with phenyl methyl sulfoxide (PMSO) commonly used as a probe for detecting high-valent metal species. However, recent studies have attributed PMSO oxidation to reactive oxygen species generated from PMS self-decomposition, raising concerns about the probe’s specificity. This study systematically evaluated PMSO oxidation under varying pH conditions to reassess its reliability. The results showed that the PMSO degradation and methyl phenyl sulfone (PMSO2) formation increased significantly with rising pH. This pH-dependency, intrinsic to the PMS/PMSO system, indicates potential interference from PMS itself. Multiple analytical approaches indicate that 1O2 and O2•- generated from PMS self-decomposition make negligible contributions, whereas PMS itself is the primary oxidant converting PMSO to PMSO2. Kinetic studies revealed that SO52– primarily drives PMSO oxidation via nucleophilic attack, with a rate constant of 10.44 M–1s–1, far exceeding that of HSO5– (0.037 M–1 s–1). Theoretical calculations further confirmed that PMSO is relatively resistant to nucleophilic attack by SO52–, making it a comparatively reliable sulfoxide probe in acidic and neutral PMS systems. These findings highlight the limitation of PMSO as a high-valent metal probe under alkaline conditions and offer guidance for probe selection in future studies.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2025
·
IF 2.1
Jingli Sun,Xuqiang Li,Lu Chen,Yujie Zhen,Siyu Zheng,Shaolong Dong,Yingmin Yu
In order to reduce the impact of nitrogen-containing compounds in oil products on the environment, this paper selected n-heptane as the oil product model and pyridine as the nitrogen-containing compound. Four inexpensive extractants (furfuryl alcohol, 1,4-butanediol, N,N-dimethylacetamide, and dimethyl sulfoxide) were selected as the extractants to separate pyridine from the oil model at 303.2 K, and the liquid–liquid equilibrium (LLE) data were measured. The partition coefficients (D) and separation coefficients (S) of the extractants were calculated and used to evaluate the extractants. Based on the LLE data, correlations were performed using NRTL and UNIQUAC models, and the interaction parameters of the corresponding optimization models were obtained. The root-mean-square deviation (RMSD) values of the NRTL and UNIQUAC models were 0.98% and 1.09%, respectively. The GUI-MATLAB tool was selected to evaluate the accuracy of the binary interaction parameter regression by a Gibbs energy topology analysis. To probe the underlying mechanism of the extraction process between the extractants and pyridine, the σ-profile was used to analyze the interaction patterns between the extractants and pyridine. Given their high extraction efficiency, the studied extractants can be considered as potential extractants for extractive denitrification processes.
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CARBON
·
2025
·
IF 11.6
Xudong Hu,Xiaolian Zhao,Shuang Li,Mengmeng Zhou,Jun Long,Xinhai Wang,Usman Farooq
Developing advanced photocatalysts with high light utilization and outstanding performance is crucial for the efficient purification of wastewater from organic contaminants. Our groundbreaking photocatalyst, boasting superior efficiency and realizing activation of peroxymonosulfate (PMS) by near-infrared-light (NIR), effectively degrades pollutants such as chlorophenol, bisphenol A, and various antibiotics in wastewater by prediction of theoretical calculation. This is verified by strategically synthesis of metal sulfide-modified graphitic carbon nitride (g-C 3 N 4 ) Z-scheme heterojunctions, which is optimized for photo-Fenton catalysis. CuS/CNNSs degrades 40 ppm 4-CP to undetectable in 20 min with a rate constant of 0.230 min −1 , 10x faster than Carbon-nitrogen nanosheets (CNNSs), showcasing its remarkable efficiency and the degradation efficiency remains above 80 % along with extremely excellent quantum efficiency (3.81 %) under NIR (1000 nm). It has strong catalytic stability and can cope with various complex water bodies with >90 % efficiency retention after 5 cycles. Moreover, we have delved into the intricate details of the degradation efficiency in real water system and various descriptors that affect the activation ability of catalysts by density functional theory (DFT). This strategy provides insight for pollutant degradation mechanisms for advanced photocatalyst R&D for wastewater treatment.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Ping Liang,Jianbin Lin,Xiongcong Guan,Jie Wang,Xinxin Zhang,Xin He,Qi Feng,Chi Zhang
Self-supported nanoporous metal foils with precisely engineered architectures are promising for catalysis, sensing, and environmental remediation, yet their scalable fabrication remains challenging. Here, we present a sequence-controlled liquid gallium (Ga)-assisted alloying/dealloying strategy, integrated with thermal evaporation, to construct Ag-modified nanoporous copper (Cu) foils. By varying the Ag deposition sequence, two distinct architectures were obtained: one features Ag 3 Ga intermetallic decorations, while the other forms a continuous Ag network within the nanoporous Cu. Subsequent electrooxidation generates Cu x O nanoneedles as catalytically active sites. The architecture with dispersed Ag 3 Ga yields exceptional non-enzymatic glucose sensing with high sensitivity, low detection limit, and long-term stability. In contrast, the continuous Ag network promotes outstanding photo‑Fenton degradation of organic dyes within minutes and excellent reusability. This work demonstrates a versatile approach to spatially control noble metal distribution in nanoporous Cu foils, enabling multifunctional catalytic systems for biosensing and environmental purification.
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Journal of Water Process Engineering
·
2026
·
IF 6.6
Chao Lian,Yongli Shi,Liman Zhang,Xiping Chen,Hai Zhu,Kai Zhang
Direct conversion of hazardous spent aluminum ash into an N-doped porous carbon/alumina composite (NPC-2). • NPC-2 activates peroxymonosulfate via both radical and non-radical pathways for rapid tetracycline degradation. • Radical ( HO . , SO 4 . – ) and non-radical ( 1 O 2 , electron-transfer) processes cooperate to enhance performance. • The porous structure ensures robust redox cycling and maintained activity over multiple runs. • Toxicity of degradation intermediates is significantly reduced, confirming environmental safety. Spent aluminum ash (SAA), a hazardous industrial solid waste, is conventionally landfilled or downcycled into low-value materials, presenting environmental risks and resource underutilization. Meanwhile, the removal of refractory antibiotics like tetracycline hydrochloride (TCH) often relies on advanced oxidation processes that face challenges related to cost, efficiency, and catalyst stability. To address these dual issues, we developed a novel method to convert inert SAA into a high-performance N-doped porous carbon/alumina composite catalyst (NPC-2) via an integrated alkali-activation and pyrolysis strategy. The resulting NPC-2 acts as a highly effective peroxymonosulfate (PMS) activator, achieving complete TCH degradation within 100 min with 69.2% COD removal and retained 82% removal efficiency throughout 30 cycles of continuous-flow operation, owing to the redox-active platform induced by its porous architecture. Mechanistic investigations reveal that the porous architecture creates a redox-active platform, while nitrogen doping modulates the electronic structure to facilitate electron transfer. This combination drives PMS activation through potential coupled radical ( HO . / SO 4 . – ) and non-radical ( 1 O 2 /electron transfer) pathways. This work demonstrates the sustainable conversion of solid waste into a green and highly effective detoxification material, presenting a dual-purpose strategy for environmental remediation and value-added waste utilization. Download: Download high-res image (200KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yujia Yang,Huiyi Shen,Lejin Xu
This work is dedicated to achieving the high mineralization efficiency of oxytetracycline (OTC) in a dissolved oxygen (DO) activated Fenton-like system by constructing a catalyst with unique catalytic performance. Three-dimensional graphene anchored nZVI hybrid MnO 2 (3D-rGO@nZVI/MnO 2 ) with layered and porous structures was synthesized and characterized by field emission scanning electron microscopy coupled with an energy dispersive spectrometer (SEM-EDS), Brunner-Emmet-Teller (BET) analysis, X-ray diffraction (XRD) measurement and Raman spectroscopy. The experimental results showed that the removal efficiency of OTC could reach 100.0% with outstanding TOC decrease of 84.0% at natural pH in the 3D-rGO@nZVI/MnO 2 -DO system. Moreover, negligible harmful intermediates were detected by ultra-performance liquid chromatography-mass spectrometry (UPLC-MS) after the reaction in the 3D-rGO@nZVI/MnO 2 -DO system. Reactive oxygen species (ROSs) detection, electrochemical measurements and X-ray photoelectron spectroscopy (XPS) analysis confirmed that the elimination mechanism of OTC was the unique catalytic degradation caused by the synergism of •OH and 1 O 2 . The unprecedented synchronous generation of •OH and 1 O 2 by DO activation provides an innovative strategy for further exploration of Fenton-like system toward more effective degradation of organic pollutants.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Wenrui Jia,Huazhe Wang,Qinglian Wu,Lushi Sun,Qishi Si,Qi Zhao,Yaohua Wu,Nanqi Ren,Wanqian Guo
The synergistic activation of persulfate by multiple factors could degrade pollutants more efficiently. However, the co-activation method based on metal ions has the risk of leakage . The non-metallic coupling method could achieve the same efficiency as the metal activation and meanwhile release environmental stress. In this study, the original biochar (BC) was prepared through using Chinese medicinal residue of Acanthopanax senticosus as the precursor. Compared with other biochar, the pore size structure was higher and toxicity risk was lower. The ultrasonic (US)/ Acanthopanax senticosus biochar (ASBC)/persulfate oxidation system was established for Atrazine (ATZ). Results showed that 45KHz in middle and low frequency band cooperated with ASBC600 to degrade nearly 70 % of ATZ within 50 min, and US promoted the formation of SO 4 − and OH. Meanwhile, the synergy index of US and ASBC was calculated to be 1.18, which showed positive synergistic effect. Finally, the potential toxicity was examined by using Toxicity Characteristic Leaching Procedure (TCLP) and luminescent bacteria. This study provides a promising way for the activation of persulfate, which is expected to bring a new idea for the win-win situation of pollutant degradation and solid waste resource utilization.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Yingpeng Gu,Yue Sun,Weisheng Zheng
Cupric (Cu(II)) complexes in industrial wastewater are responsible for the failure of conventional alkaline precipitation, but the properties of cuprous (Cu(I)) complexes at alkaline circumstance have not been focused. This report proposed a novel strategy for the remediation of Cu(II)-complexed wastewater by coupling alkaline precipitation with green benign reductant, namely, hydroxylamine hydrochloride (HA). This remediation process (HA-OH) exhibits superior Cu removal efficiency that cannot be achieved with the same dosage of oxidants (3 mM). The possibility of Cu(I) activated O 2 catalysis and self-decomplexation precipitation were investigated, and the results identified that 1 O 2 was generated from Cu(II)/Cu(I) cycle, but it was insufficient to annihilate organic ligands. Cu(I) self-decomplexation was the dominate mechanism of Cu removal. For real industrial wastewater, HA-OH process can realize the efficient Cu 2 O precipitation and Cu recovery. This novel strategy utilized intrinsic pollutant in wastewater without introducing other metals, complicated materials, and expensive equipment, broadening the insight for the remediation of Cu(II)-complexed wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yinxu Wang,Andac Armutlulu,Wenyuan Hu,Ruzhen Xie
The sluggish kinetics of Fe(II) regeneration and inactive Fe(III) sludge accumulation strongly hampers the scientific progress of Fenton-related reactions toward practical application. Herein, we developed a durable zero-valent iron super dispersed sodalite-graphene oxide hybrid (Z@GO-SOD) via reactive oxidation species (ROSs) route using industrial waste lithium silicon fume (LSF) as raw material, and first applied it as a visible-light-driven photocatalyst to initiate Fenton-like reaction for effective ciprofloxacin (CIP) remediation. The Z@GO-SOD featured a mesoporous structure with iron strongly interaction with GO hybrid zeolite, the GO hybrid zeolite acted as an efficient mediator, facilitating charge separation and transportation to expedite the iron redox cycle. The presence of persulfate could further act as an electron acceptor to boost photogenerated e − /h + separation, resulting in more OH for fast CIP removal. Over 90 % of CIP was removed within 30 min in the Z@GO-SOD/Vis/PS system with the usage of merely 0.4 g/L catalyst, and as high as 71% CIP was completely mineralized, which outperformed most of the state-of-the-art photo-Fenton catalysts. Meanwhile, Z@GO-SOD also demonstrated excellent reusability and stability. This work indicated the feasibility of utilizing solar energy for both preparation of catalyst and remediation of wastewater, paying the way for a sustainable solution for environmental solid waste pollution and water scarcity issue.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 17
·50815-50828
·
IF 5.8
Chen Chen,Sun Hao,Zhang Shengyu,Su Xiaosi
In this study, stalk biochar (BC) was prepared by a high-temperature pyrolysis process and used as a non-metallic catalyst to activate peroxydisulfate (PDS) to degrade tetracycline hydrochloride (TCH). Various characterization results showed that BC had a hollow tubular structure, irregular folds, and important active sites such as oxygen-containing functional groups. Under the optimal reaction conditions, the degradation rate of TCH reached 98.1% within 120 min. In addition, the degradation performance was satisfactory and similar under acidic and near neutral pH, and higher temperature promoted the degradation of TCH. The SO 4 · − , ·OH, and 1 O 2 generated by PDS activation were reactive oxygen species (ROS), which degraded TCH through free radical/non-radical synergistic pathways. Quenching experiments proved that the generated SO 4 · − and ·OH might be the dominant reactive oxygen species (ROS) during the oxidative reaction. The research results will provide a theoretical basis for the application of PDS activated by non-metallic catalysts in the remediation of tetracycline antibiotics pollution.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xiaoyue Zhou,Renli Yin,Jieqiong Kang,Zhenjie Li,Yanan Pan,Jieyun Bai,Adela Jing Li,Rongliang Qiu
The formation of high-valent active species during peroxymonosulfate (PMS) activation has attracted great interest. However, how to rapidly generate high-valent active species during PMS activation process remains ambiguous. Herein, iron vacancy anchored layered double hydroxides activated PMS process were designed to enhance the removal rate of sulfamethoxazole (SMX) by 30.0 times to PMS alone, which even showed much superiority to the homogeneous Fe 2+ /PMS system. Due to the cooperation of Fe vacancies, PMS favored to be adsorbed on Fe2 sites (adjacent to iron vacancy) and combined with Fe2 sites to form Fe(II)-O-SO 3 -OH complex. Then, the accepted electrons led to the cleavage of S-O bond in Fe(II)-O-SO 3 -OH complex, resulting in the spontaneous generation of Fe (IV) =O/Fe (V) =O species. Finally, PMS activation pathways were proposed from radical oxidation to nonradical oxidation via high-valent iron-oxo species. This study provides a new perspective on generation of high-valent iron-oxo species for excellent performance and resistance with real wastewater .
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