Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124603
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IF 7.5
Qian Sun,Xiaoyun Ma,Yan Meng,Lijun Yang,Kaile Li,Mengyuan Xu,Jing Deng,Jie Zhu
The persistent occurrence of antibiotics in aquatic environments, along with the induced antibiotic-resistant bacteria (ARB) and resistance genes (ARGs), constitute a complex environmental issue encompassing both chemical contamination and biological risks. This study investigates the performance and mechanism of UV-LED/PDS and UV-LED/PMS systems for treating sulfachloropyridazine (SCP), a typical sulfonamide antibiotic, as well as ARB and ARGs. Results showed that both systems significantly enhanced SCP degradation, with UV-LED/PDS showing higher degradation efficiency under the tested conditions. The degradation rate increased with oxidant concentration over the range of 0.5–1.5 mM. Alkaline conditions favored SCP degradation in both systems. Quenching and probe experiments demonstrated that SO 4 ∙ - was the dominant reactive species for SCP removal, with HO· playing an auxiliary role, and the contribution of HO· increased slightly with increasing pH. The proposed degradation pathway was elucidated based on eleven intermediates identified by HPLC-MS, and acute toxicity changes were evaluated using ECOSAR. Furthermore, both systems effectively controlled ARB and ARGs, with UV-LED/PMS outperforming UV-LED/PDS, through the dominant contribution of SO 4 ∙ - , alongside a secondary role of HO·. Flow cytometry, SEM, and enzymatic assays confirmed that both systems compromised membrane integrity, induced morphological damage (roughening, shrinkage, collapse), and overwhelmed antioxidant defenses via oxidative stress, ultimately leading to cell damage. Weakly alkaline conditions resulted in slightly better inactivation performance than acidic conditions.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Youwei Yang,Jianxing Wang,Yan Gao,Xuekun Tang,Chunying Wang,Xianping Luo
ZnFe 2 O 4 catalysts synthesized via hydrothermal (ZFO-H) and sol-gel (ZFO-S) methods were employed to activate peroxodisulfate (PDS) under UV light for the efficient conversion of low-concentration NH 4 + -N into environmentally benign N 2 , offering a promising solution for advanced wastewater treatment. Characterization revealed that the sol-gel-derived ZFO-S exhibited uniform agglomeration, smooth surfaces, and an 80% reduction in surface hydroxyl density (as indicated by the FTIR peak area at 3320 cm -1 ), outperforming both hydrothermally prepared and commercial ZnFe₂O₄ (ZFO-H and ZFO-M, respectively). This study addresses the critical challenge of ammonia nitrogen removal in wastewater, where conventional methods often struggle with low efficiency or secondary pollution. Mechanistic studies demonstrated that ZnFe 2 O 4 facilitated electron transfer at Zn sites to activate PDS, generating reactive species dominated by singlet oxygen ( 1 O 2 ), which drove NH 4 + -N oxidation. Density functional theory (DFT) calculations further elucidated the reaction pathway, highlighting preferential adsorption of NH 3 at oxygen sites on the ZnFe 2 O 4 (311) surface, followed by sequential dehydrogenation and coupling to form N 2 . Under optimal conditions (pH >9.25, 10 mM PDS, 25°C, 3 h), 97.40% of initial 50 mg/L NH₄ + -N was converted to N₂, with negligible NO 3 − byproduct formation (< 6%), demonstrating high feasibility for practical wastewater remediation. The reduced surface hydroxyl groups and lower work function of ZFO-S enhanced electron transfer, underscoring its superior catalytic activity. This work provides a novel strategy for designing hydroxyl-regulated photocatalysts tailored for wastewater treatment and advances the mechanistic understanding of persulfate-based ammonia nitrogen remediation in engineered water systems.
研究领域:
环境科学
·
催化化学
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Surfaces and Interfaces
·
2025
·
IF 6.3
Dengping Zhang,XiangYu Zhang,Jing Hu,Wen Wang,Yuqing Lv,Xiao li Qian
Recent years, persulfate (PS) activation has mainly relied on metal ion activation, carbon materials, and their doped counterparts. However, traditional methods exhibit numerous limitations. Ionic liquids (ILs), due to their customizable nature, offer new potential for targeted non-radical catalysis. In this study, 1-butyl-3-methyl-1H-imidazol-3-ium bis((trifluoromethyl)sulfonyl) amide ([Bmim][Tf 2 N]) was used to enhance peroxydisulfate (PDS) activation for degrading oxytetracycline (OTC), achieving almost complete degradation in just 20 minutes. The mechanism revealed that the imidazole ring in the [Bmim][Tf 2 N] cation acts as an electron donor, promoting the cleavage of the O-O bond in the PDS and generating 1 O 2 . And, the iminium nitrogen in the anion acts as an electron acceptor, facilitating the breaking of the S-O bond in the PDS twice in succession, further producing 1 O 2 . This represents a successful application of ILs for PDS activation, providing new insights into designing efficient, targeted catalytic methods.
研究领域:
环境化学
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催化科学
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绿色化学
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高级氧化工艺
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离子液体应用
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ning Deng,Huichao Zhu,Zhiheng Fan,Changjin Guo,Jie Hu,Xin Huang
Phosphate recovery presents an effective solution to address the conflicting problems of phosphorus pollution and scarcity. However, recovering organic phosphates, such as 1-hydroxyethane 1,1-diphosphonic acid (HEDP), is comparatively complex, which involves multiple processes. Herein, we developed an innovative all-in-one solution to simplify these processes by combining NiFe-layered double hydroxides (NiFe-LDH) and peroxydisulfate (PDS). This combination achieved approximately 90 % conversion of HEDP to orthophosphate, with 100 % of the resulting orthophosphate recovered in 120 min. The exceptional performance in simultaneous HEDP degradation and recovery can be attributed to dual roles of Ni and Fe in NiFe-LDH/PDS. The polyvalent Ni functions as an electron shutter (Ni 2+ ⇋ Ni 3+ ⇋ Ni 2+ ) in the redox cycles between PDS and HEDP, accounting for effective HEDP degradation. The high complexation stability between Fe(Ⅲ) and orthophosphate (log K = 9.92) allows Fe(Ⅲ) to serve as binding sites for orthophosphate recovery. Moreover, NiFe-LDH/PDS effectively treats HEDP across wide pH ranges (3–––10), which can be ascribed to pH buffers originating from protonation/deprotonation in NiFe-LDH layers. The recovered phosphorus with NiFe-LDH exhibited a slow-release property under soil water solution without notable Ni release, which highlighted its potential usage as a slow-release fertilizer. These features—catalytic and binding sites, and high compatibility—allow NiFe-LDH to achieve concurrent degradation and recovery of organic phosphate in a single solution.
研究领域:
环境科学
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化学工程
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WATER SCIENCE AND TECHNOLOGY
·
2022
·Vol. 86
·期 10
·2718-2731
·
IF 2.43
Wang Bo,Cao Xuan,Li Shifeng,Yao Shuhua,Wang Haibo
Nickle-copper ferrite (Ni 0.5 Cu 0.5 Fe 2 O 4 ) supported on activated carbon (AC) (AC@Ni 0.5 Cu 0.5 Fe 2 O 4 ) was synthesized and used as adsorbent, photocatalyst, and activator of peroxydisulfate (PDS) to realize the removal of ciprofloxacin (CIP). AC@Ni 0.5 Cu 0.5 Fe 2 O 4 properties were characterized by scanning electron microscope equipped with energy-dispersive X-ray (SEM-EDX), X-ray diffraction (XRD), N 2 adsorption-desorption isotherm plot of Brunauer-Emmett-Teller (BET) and Barrett-Joyner-Halenda (BJH), vibrating sample magnetometer (VSM). A rapid removal rate (94.30%) of CIP was achieved on AC@Ni 0.5 Cu 0.5 Fe 2 O 4 /PDS/UV system with the condition of catalyst dosage 0.30 g/L, initial pH 7.3, PDS addition 0.20 mM, CIP concentration 10 mg/L (200 mL), UV 28 W, in 30 min. Free radical quenching experiments indicate that reactive species of superoxide (·O 2 − ), holes (h + ), sulfate radicals (SO 4 − ·) and hydroxyl radicals (·OH) were produced and all worked. The reusability test demonstrated that AC@Ni 0.5 Cu 0.5 Fe 2 O 4 could be recycled five times with minimal performance reduction for the removal of CIP. The XRD and SEM of the after used AC@Ni 0.5 Cu 0.5 Fe 2 O 4 did not change significantly, which further showed its stability and recyclability. This work might provide new insight into the application of AC@Ni 0.5 Cu 0.5 Fe 2 O 4 in photocatalysis coupled with adsorption in peroxydisulfate assisted system and has high potential in CIP removal. AC@Ni 0.5 Cu 0.5 Fe 2 O 4 was synthesized by a simple co-precipitation method. AC@Ni 0.5 Cu 0.5 Fe 2 O 4 has a large specific surface area and thus can provide more reaction sites. AC@Ni 0.5 Cu 0.5 Fe 2 O 4 can be used as adsorbent, photocatalyst, and activator of peroxydisulfate. AC@Ni 0.5 Cu 0.5 Fe 2 O 4 displayed an excellent recyclability.
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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水处理技术
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BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Wenye Li,Binghan Xie,Zhipeng Li,Guoyu Zhang,Zhiying Lv,Qinghao Li,Shuyu Zhao,Mu Tong,Yuanyuan Gao,Langming Bai
The effective dewatering of waste activated sludge (WAS) and the utilization of resources are crucial for the sustainable development of wastewater treatment plants. Ultrasonic (US) collaborative iron-carbon (Fe-C) activated peroxydisulfate (PDS) coupling system was constructed to investigate the transformation of physicochemical properties and explore the mechanisms during the cracking and oxidation of WAS. The ultrasonic enhanced Fe-C/PDS system, which exhibited excellent oxidation capacity under the conditions of PDS, Fe-C, and ultrasonic power levels at 0.12 g/g TS, 0.3 g/g TS, and 0.3 W/mL. The water content of the sludge cake was reduced to 61.71 %, while the specific resistance to filtration was lowered to 1.12 × 10 12 m/kg (decreased by 88.2 %). Furthermore, ultrasonic improved the WAS cracking capacity with a satisfying SCOD production (630.64 mg/L) and a dramatic reduction of 9.16 % in volatile solids. Compared to Fe-C/PDS, the addition of ultrasonic enhanced the leaching of Fe, released carbon source and promoted the formation of various reactive oxidative species to degrade bound EPS. The contribution of O 2 − and 1 O 2 was 37.00 % and 43.17 %, indicating the oxidation process of free radicals and non-free radicals in Fe-C/PDS/US system. Additionally, the concentration of short-chain fatty acids was increased by 96.7 %, which significantly accelerating the quality of carbon source suitable for recycling. The positive improvement of sludge physicochemical properties revealed the disintegration-degradation synergistic effect of the Fe-C/PDS/US systems. These findings provide a novel strategy for effective disposal and reduction in WAS while also offering valuable insights into resource utilization.
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PubMed
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Caiyi Jiang,Ming Hou,Li Yang,Shenghui Guo,Guo Yang,Bo Xing,Yi Wang,Dongzheng Wang,Xiaolin Shi
Fe–N co-doped carbon catalyst has received increasing attention in the field of organic wastewater treatment because of its unique structure and outstanding activity. However, the reusability, catalytic activity, and pH working range are still a great challenge for future application. Herein, a novel αFe-HM@C-T catalyst was prepared by pyrolyzing a mixture of starch and heme and was analyzed by TEM, H2-TPR, XRD, BET, XPS, FTIR, and Raman spectrum. Meanwhile, αFe-HM@C-T catalysts show the highest catalytic performance due to abundant porous structure, higher redox property, and unique Fe–Nx configuration. The rhodamine B (RhB) could be almost completely degraded within 30 min on the 5Fe-HM@C-850, and recovery rates of catalytic activity of 96% and 91.8% were achieved in peroxydisulfate (PDS) and H2O2 systems with an extensive buffer pH range. Furthermore, mechanistic insights by quenching experiments and EPR verified the high removal efficiency of RhB mainly attributed to indirect oxidation of SO4•–, •OH, and 1O2 in both systems, and the potential mechanism was proposed.
研究领域:
环境科学
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催化材料科学
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Water
·
2024
·Vol. 16
·期 3
·505
·
IF 3
Yuting He,Jiantao Lin,Yuchuan Yang,Minghua Liu,Yifan Liu
Modified sludge biochar, recognized for its notable economic and environmental benefits, demonstrates potential as an effective catalyst for peroxydisulfate (PDS) activation. Nevertheless, the specific mechanisms underlying its catalytic performance require more comprehensive investigation. In this study, a modified biochar (TSBC) doped with oxygen (O) and nitrogen (N) atoms was synthesized from sewage sludge and tannin extract, which significantly enhanced the activation of PDS for the degradation of sulfamethoxazole (SMX). The TSBC/PDS system demonstrated robust performance for SMX degradation, achieving over 90% efficiency over a wide pH range (3–10). Subsequent quenching experiments demonstrated that TSBC predominantly catalyzed PDS to generateO21, which effectively degraded SMX via a non-radical pathway. The O- and N-containing functional groups in TSBC were identified as the primary catalytic sites. Besides, density functional theory (DFT) calculations revealed that the incorporation of graphitic N significantly improved the adsorption capacity of PDS on the TSBC surface. Furthermore, based on the identification of intermediates and theoretical calculations, SMX was degraded mainly by two different pathways: S-N cleavage andO21oxidation. This study offers a foundational framework for the targeted modification of sludge biochar, thereby expanding its applications.
研究领域:
环境科学
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催化材料
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JOURNAL OF HAZARDOUS MATERIALS
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2018
·
IF 6.434
Ailin Li,Zihao Wu,Tingting Wang,Shaodong Hou,Bangjie Huang,Xiujuan Kong,Xuchun Li,Yinghong Guan,Rongliang Qiu,Jingyun Fang
The abatement of pharmaceuticals and personal care products (PPCPs), including carbamazepine (CBZ), acetaminophen (ACP) and sulfamethoxazole (SMX), by zero-valent iron (Fe°) activated peroxydisulfate (PDS) system (Fe°/PDS) in pure water and groundwater was investigated. The removal rates of CBZ, ACP and SMX were 85.4%, 100% and 73.1%, respectively, within 10 min by Fe°/PDS in pure water. SO 4 •− , • OH and O 2 •− were identified in the Fe°/PDS system, and O 2 •− was indicated to play an important role in the ACP degradation. The degradation of PPCPs increased with increasing dosages of Fe° and PDS or with decreasing pH and initial PPCP concentrations. Interestingly, the degradation of PPCPs by Fe°/PDS was significantly enhanced in groundwater compared with that in pure water, which was partially attributed to SO 4 2− and Cl − . The first-order constants of CBZ, ACP and SMX increased from 0.021, 0.242 and 0.013 min− 1 to 0.239, 2.536 and 0.259 min −1 , and to 0.172, 1.516 and 0.197 min −1 , respectively, with increasing the concentrations of SO 4 2− and Cl − to 100 mg/L and 10 mg/L, respectively. This study firstly reports the unexpected enhancement of groundwater matrix on the degradation of micropollutants by Fe°/PDS, demonstrating that Fe°/PDS can be an efficient technology for groundwater remediation.
研究领域:
环境科学
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化学工程
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PubMed
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Lindong Liu,Ying Wang,Qian Liu,Wenju Wang,Lian Duan,Xiao Yang,Shixiong Yi,Xuting Xue,Jiangwei Zhang
Understanding how the morphology of a nanocatalyst tailors its catalytic performance is a crucial issue for the rational design and fabrication of active heterogeneous catalysts at the nanometer level. Herein, we demonstrate novel findings of peroxydisulfate (S 2 O 8 2− ; PDS) activation catalyzed by nickel oxide (NiO) nanocatalysts of different morphologies, in which oxygen vacancies ( V O ) were the defective sites that facilitated the chemical bonding with PDS molecules and promoted the reactivity of V O -connected nickel ions for PDS activation, thus elucidating the structural origin of its catalytic activities. The morphologically tunable NiO with various V O concentrations exhibited different catalytic performance for the removal of phenol (a model organic pollutant). Based on an electron paramagnetic resonance (EPR) study, radical competition reactions, and quenching tests, the main reactive species was revealed to be the non-radical PDS-NiO complex, which can effectively attack C 6 H 5 O − to yield intermediates attached to NiO surface. This work not only improves the fundamental understanding of active sites in morphologically tunable transition metal oxides, but also provides valuable guidelines for the rational design and synthesis of high-performance, morphology-dependent nanocatalysts.
研究领域:
催化
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环境科学
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材料科学
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Sustainable Materials and Technologies
·
2026
·
IF 9.7
Haize Jin,Ziyuan Wang,Kaiqiang Hong,Xiaoxia Huang,Qikun Wang
The construction of a synergistic adsorption-photocatalysis-peroxydisulfate (PDS) activation system holds great promise for efficient organic pollutants degradation. Herein, cetyltrimethylammonium bromide (CTAB)-modified geopolymer/Ag 9 (SiO 4 ) 2 NO 3 /g-C 3 N 4 (GACC) adsorbent-photocatalyst powder and porous membranes were rationally designed by combining geopolymerization and co-precipitation reactions. The CTAB was successfully introduced to endow the material with positively charged active sites via electrostatic anchoring and hydrophobic assembly. This enabled GACC to effectively capture of both negatively charged PDS and positively charged or zwitterionic moxifloxacin (MOX) species within a wide range of pH values. And the outstanding adsorption response capability of GACC exhibited rapid adsorption-degradation kinetic matching without pre-adsorption. The introduction of CTAB increased the specific surface area, and broadened the visible-light absorption range and reduced the band gap, thereby enhancing charge separation efficiency and facilitating PDS activation. Additionally, the fluorescence lifetime of GACC was found to be prolonged, and the electric double-layer capacitance (C dl ) results confirmed that CTAB facilitated the increase of available active sites. Under simulated sunlight, the GACC powder achieved a MOX removal efficiency of 93.67% within 10 min. Moreover, the GACC porous membranes prepared via H 2 O 2 foaming exhibited comparable degradation performance to powder counterpart (94.10% at 30 min). Furthermore, under dynamic conditions, these membranes exhibited excellent recyclability, highlighting their potential for practical applications. Mechanistic studies revealed that photogenerated electrons dominated PDS activation, while h + , ·OH, ·O 2 − , ·SO 4 − , and 1 O 2 collectively contributed to MOX degradation. This work provides a promising strategy for designing high-performance monolithic adsorbent-photocatalyst systems with synergistic adsorption-photocatalysis-PDS activation for efficient and sustainable wastewater treatment.
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SENSORS AND ACTUATORS B-CHEMICAL
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2026
·
IF 8.3
Yongjing Guo,Hangshuo Feng,Qiuni Zhao,Juntao Mu,Qi Ran,Dongyang Li,Jian Luo,Yi Xia,Ming Hou,Li Yang,Shenghui Guo
Two-dimensional tin sulfide (SnS 2 ) shows great promise as a NO 2 gas-sensing material due to its large specific surface area and suitable band structure, yet its selectivity and detection limit remain inadequate. Herein, PdS/SnS 2 composite with PdS nanoparticle inlaid in lettuce-like structure SnS 2 was synthesized via a facile microwave-assisted method for room-temperature NO 2 detection. The optimized PdS/SnS 2 composite exhibits that the response value to 5 ppm NO 2 reached 2560% at room temperature under 50% relative humidity, which is approximately 10.7 times that of pristine SnS 2 (238%). Importantly, its experimental limit of detection (LOD) for NO 2 is as low as 800 ppt, while the theoretical LOD is below 164 ppt. Furthermore, it also shows outstanding reversibility and repeatability (RSD < 5%), and high selectivity (response ratio > 40) against interfering gases. The enhanced sensing performance is attributed to the synergistic effect of the PdS/SnS 2 heterojunction and sulfur vacancies, which promotes NO 2 gas adsorption on the material surface and electron transport inside the material. This study provides a feasible strategy for designing high-precision and ultra-trace NO 2 sensors with ppt-level detection capabilities at room temperature.
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