SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Chenlu Liu,Jingjing Xu,Junfeng Niu,Mindong Chen,Yonghui Zhou
This paper introduces a Z-scheme Ag 3 PO 4 /Bi 4 Ti 3 O 12 heterojunction composite photocatalyst prepared by an in-situ growth method. The photocatalytic properties of the prepared samples under visible light irradiation were studied by degrading sulfamethoxazole (SMX). The results of photocatalytic experiments and cycle experiments showed that Ag 3 PO 4 /Bi 4 Ti 3 O 12 -20% composite exhibited much better photocatalytic activity and stability than pure Ag 3 PO 4 and pure Bi 4 Ti 3 O 12 . The capture experiment results showed that h + is the main active substance in the process of SMX degradation. In addition, we proposed a possible photocatalytic mechanism based on the results of experiment and characterization. The formation of a direct Z-Scheme photocatalytic system promoted the separation of carriers, thereby improving the stability and activity of the composite samples.
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APPLIED SURFACE SCIENCE
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2021
·
IF 6.707
Jinyan Cao,Yue Jing,Zhongxing Du,Wei Chu,Jianjun Li,Wanglai Cen
A novel n-n type WC/BiOCl binary photocatalyst was synthesized, and applied to sulfamethoxazole (SMX) degradation. The physical and photoelectric properties of the WC/BiOCl were characterized by various experimental and calculational methods. An intimate interfacial contact between WC and BiOCl was identified, which help to reduce the aggregation of BiOCl and more importantly, build an internal electrical field between WC and BiOCl. It is interesting to find that the WC layer(s) can help to reduce the interfacial charge transfer resistance and act as electron transfer and storage sites. Subsequently, the holes are engaged in the oxidation of SMX by WC/BiOCl. Additionally, WC/BiOCl photocatalyst has more reactive sites and absorbs more incident photons compared with pure BiOCl. Quenching and electron spin resonance (ESR) experiments indicate that O 2 ·- is the main active species, holes and OH • are also involved. The degradation pathway of SMX and the enhancing mechanism for the photodegradation through the combination of WC and BiOCl were explored. This work provides a novel binary photocatalyst for SMX degradation.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2019
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IF 5.589
Ai-Yue Wang,Kai Sun,Liping Wu,Ping Wu,Wenchao Zeng,Zhongmin Tian,Qun-Xing Huang
Different biomass materials (walnut shell, coconut shell or cottonwood sawdust) were co-pyrolyzed with carbon-enriched oily sludge to produce aqueous phase sulfamethoxazole (SMZ) adsorption materials. The co-pyrolysis char was activated with K 2 CO 3 to modify its micro-structure and functional groups. Results show that ACs prepared from the mixture contained more mesopores than biomass-based ACs, more porous and higher yield than oily sludge-based ACs. One-step activation method was more attractive than two-step activation in larger specific surface area (up to almost 4 times), wider pore size distribution (2–3 nm), stronger SMZ adsorption ability (higher than 2 times). The maximum BET surface area was 1342 m 2 /g for the ACs prepared from the mixture of walnut shell and oily sludge by one-step activation and it had the maximum SMZ adsorption capacity up to 361.9 mg/g, which is higher than previous reported values. The capacity of SMZ adsorption of ACs was mainly attributed to pore size distribution, specific surface area and functional groups. Among them, the appropriate content of C O and C O functional groups, larger specific area and more pores range from 2 to 3 nm lead to higher adsorption capacity.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Shizong Wang,Jianlong Wang
High efficient and stable activator is desired for the sulfate radical-based wastewater treatment. Cobalt sulfide and cobalt oxide have high catalytic activity for peroxymonosulfate (PMS), but poor stability. Here, a novel composite, nano Co 9 S 8 and CoO encapsulated by nitrogen and sulfur co-doped sludge-derived biochar (CoO/Co 9 S 8 @N-S-BC) was synthesized, characterized and applied for activating PMS. The results showed that CoO/Co 9 S 8 @N-S-BC can effectively activate PMS for sulfamethoxazole (SMX) degradation, and 0.08 mM of SMX could be completely degraded within 10 min. The influencing factors, such as pH, temperature, chloridion, carbonate and humic acid were investigated. The SMX degradation conformed to pseudo first-order kinetics with rate constant of 0.379 min −1 . Sulfate radicals (dominant) and hydroxyl radicals contributed to SMX degradation. Carbon defects, pyridinic N, quaternary N, the carbon atoms next to pyridinic N, C O groups, -C-S-C and Co(II), all contributed to PMS activation.
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International Journal of Environmental Research and Public Health
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2020
·Vol. 17
·期 2
·473
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IF 2.849
Jian Yu,Hao Shen,Bin Liu
In this paper, attapulgite purified by acid heat was employed, and millimeter polyethersulfone-modified attapulgite hybrid microspheres were prepared. The effects of mixed bisphenol A (BPA) and sulfamethoxazole (SMX) solution on the modified attapulgite doping ratio, initial solution pH, adsorbent dosage, contaminant concentration, and temperature were studied. The experimental results showed that BPA and SMX compete in the adsorption process, and the hybrid microspheres preferentially select the BPA molecules (anionic endocrine disruptors) compared to the SMX. The adsorption process in the mixed solution conforms to the quasi-secondary-order kinetic model. The adsorption of BPA and SMX by hybrid microspheres is more consistent with the extended Langmuir adsorption thermodynamic model, and the adsorption of BPA + SMX is more in line with the Langmuir adsorption thermodynamic model. At 25 °C, the maximum adsorption capacity of hybrid microspheres for BPA and SMX was 102.04 and 12.80 μmol·g−1, respectively, and the maximum adsorption of BPA + SMX was 112.36 μmol·g−1. After five regenerations, the removal effect of the hybrid microspheres on the endocrine disruptors remained above 95%.Keywords:endocrine disruptor;bisphenol A;sulfamethoxazole;attapulgite;adsorption
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ENVIRONMENTAL POLLUTION
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2014
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IF 3.902
Chi Wang,Hao Li,Shaohua Liao,Di Zhang,Min Wu,Bo Pan,Baoshan Xing
The K d of sulfamethoxazole (SMX) on activated carbon (AC) was larger than that of SMX on single-walled carbon nanotubes (SC), but the competition of SMX with carbamazepine (CBZ) for adsorption sites was weaker on AC than SC. Thus, a large K d value does not necessarily reflect a high affinity. The analysis of the apparent sorption , competition, desorption hysteresis, and the sorption thermodynamics for SMX and CBZ did not provide sufficient information to distinguish their sorption affinities. The release of the adsorbed CBZ was not altered with SMX as the competitor, but SMX release increased significantly after CBZ addition. The higher sorption affinity of CBZ may be explained by the interactions of the CBZ benzene rings with the aromatic structures of the adsorbents. Although the thermodynamic meaning cannot be described, the release ratio of the adsorbed pollutants provides useful information for understanding pollutant sorption strength and associated risks.
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RSC Advances
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2017
·Vol. 7
·期 77
·48670-48677
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IF 3.108
Shizong Wang,Jianlong Wang
Pharmaceuticals and personal care products (PPCPs) are emerging contaminants, which are ubiquitous and pose the potential risk to ecosystem and human health. It is necessary to remove PPCPs from water and wastewater. In this study, sulfamethoxazole, a widely used antibiotic, was chosen as targeted pollutant. Fenton process and persulfate process were employed to remove sulfamethoxazole from aqueous solution. The results showed that Fenton process required less amount of Fe(II) and oxidant than persulfate process to achieve 100% removal of sulfamethoxazole in the water sample prepared with de-ionized water. The maximal mineralization reached 83% when hydrogen peroxide concentration was 1 mM and Fe(II) was 0.05 mM for Fenton process. The maximal mineralization for persulfate process was 60% with 4 mM of persulfate and 4 mM of Fe(II). The increase of Fe(II) concentration could increase the decomposition of hydrogen peroxide and persulfate, but did not increase the mineralization of sulfamethoxazole, indicating that the decomposition of hydrogen peroxide and persulfate was not positive correlation with the removal and mineralization of sulfamethoxazole. Five intermediate compounds were detected in Fenton process while eight intermediate compounds in persulfate process, suggesting that different degradation pathway occurred in the two processes. The wastewater components had negative effect on the degradation of sulfamethoxazole for both Fenton and persulfate processes. The removal efficiency of sulfamethoxazole was 52.5% and 52.3%, respectively, for Fenton and persulfate processes. Persulfate process could be an alternative for treating the real wastewater containing PPCPs.
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Desalination and Water Treatment
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2024
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IF 1
Chao Wang,Su Xu,WenChao Liao,TsingHai Wang
Manganese oxide-based catalysts have been frequently adopted to activate peroxymonosulfate (PMS) for the degradation of refractory contaminants such as sulfamethoxazole (SMX). In this study, the Co-doped ɑ-MnO 2 catalyst was prepared to validate the concept that the introduction of additional oxidation states and structural defects due to the doping process would significantly enhance the efficiency of PMS activation. Among all Co@ ɑ-MnO 2 catalysts prepared, the activator with the mole ratio of Co/Mn 0.05:1 exhibited the highest SMX degradation. A near 100% removal of SMX (1000 μ g / L ) was achieved within 1 min in a condition with 10.0 mmol/L PMS and 0.5 g/L Co 0.05 @ ɑ - MnO 2 at 25 ℃ . The effects of catalyst dose, PMS concentration, initial SMX concentration, solution pH, temperature, and coexisting cations, anions, and humic acid (HA) on SMX degradation were studied. The impressive sustainability of the Co 0.05 @ ɑ-MnO 2 /PMS system was confirmed by its capability of operating over a wide pH range, its stability after multiple cycles, and its insensitivity to the coexisting of cations. The presence of high electrophilic anions, such as NO 2 ¯ and HCO 3 ¯ , on the other hand, would compromise the SMX degradation. Furthermore, reactive oxygen species (ROS) generated in the Co@ ɑ-MnO 2 /PMS system were identified by scavenger tests and electron paramagnetic resonance (EPR). Singlet oxygen ( 1 O 2 ) was verified to be the major route contributing to the degradation of SMX. In addition, sulfate radicals ( SO4 •¯ ), superoxide radicals (O 2 •¯ ), and hydroxyl radicals (ּ • OH) were also generated in the Co@ ɑ-MnO 2 /PMS system and participated in SMX degradation. Therefore, the Co@ ɑ-MnO 2 is a promising catalyst for PMS activation in the degradation of SMX.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Xiaohui Lu,Yanjun Li,Hongyu Zhou,Siyu Li,Wei Wei,Guochun Lv,Gang Yang,Shihuai Deng,Bo Lai,Jiali Peng
Recently, many reagents have been introduced to accelerate the formation of highly reactive intermediate Mn species from permanganate (KMnO 4 ), thereby improving the oxidation activity of KMnO 4 towards pollutants. However, most studies have mainly focused on sulfur-containing reducing agents (e.g., bisulfite and sodium sulfite), with little attention paid to nitrogen-containing reducing agents. This study found that hydroxylamine (HA) and hydroxylamine derivatives (HAs) can facilitate KMnO 4 in pollutant removal. Taking sulfamethoxazole (SMX) as a target contaminant, the effect of pH, SMX concentration, KMnO 4 and HA dosages, and the molar ratio of HA and KMnO 4 on the degradation of SMX in the KMnO 4 /HA process was systematically investigated. Quenching experiments and probe analysis revealed MnO 2 -catalyzed KMnO 4 oxidation, Mn(III) and reactive nitrogen species as the primary active species responsible for SMX oxidation in the KMnO 4 /HA system. Proposed transformation pathways of SMX in the KMnO 4 /HA system mainly involve hydroxylation and cleavage reactions. The KMnO 4 /HA system was more conducive to selective oxidation of SMX, 2,4-dichlorophenol, and several other pollutants, but reluctant to bisphenol S (BPS). Overall, this study proposed an effective system for eliminating pollutants, while providing mechanistic insight into HA-driven KMnO 4 activation for environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Haoran Song,Linxia Yan,Jin Jiang,Jun Ma,Suyan Pang,Xuedong Zhai,Wei Zhang,Dong Li
In this study, electrochemical activation of peroxydisulfate (PDS) using carbon anodes including multi-walled carbon nannotube (MWCNT), graphite (GR), black carbon (BC) and granular activated carbon (GAC) for degradation of antibiotic sulfamethoxazole (SMX) was investigated for the first time. The degradation of SMX by electrochemical activation of PDS using carbon anodes showed dual kinetics: an induction stage followed by a quick decay stage. In the latter stage, the degradation rate of SMX by electrochemical activation of PDS using MWCNT, GR, BC and GAC anodes increased about 15–35 times of that by electrolysis alone and 30–130 times of that by carbon/PDS (without applying current). The results of degradation of radical probes (atrazine (ATZ) and nitrobenzene (NB)) and radical scavenging effect manifest that nonradical oxidation, hydroxyl radical (HO ) and sulfate radical (SO 4 − ) jointly contributed to the degradation of SMX in electrochemical activation of PDS. The formation of transition state structure of PDS (activated PDS, PDS ∗ ) between PDS molecule and carbon anodes by applying current was proposed to be responsible for nonradical oxidation, and its further decomposition resulted in the generation of HO and SO 4 − . Increasing PDS concentration (0.1–5 mM) or current density (10–200 A m −2 ) considerably promoted the degradation of SMX. Additionally, electrochemical activation of PDS using carbon anodes exhibited good resistance to water matrices.
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MARINE POLLUTION BULLETIN
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2024
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IF 5.3
Jianxin Fan,Jiaxin Yang,Fulong Cheng,Shikuo Zhang,Jiaoxia Sun
The extensive use of antibiotics has led to significant antibiotic pollution in water bodies, and suspended particulate matter (SPM) is known to be a key carrier of antibiotics in rivers. In this work, the adsorption characteristics of sulfamethoxazole (SMX) on SPM was investigated through batch adsorption and annular flume experiments, and the MIKE 21 model was employed to simulate the migration of SMX and SPM. Results revealed that most SMX adsorption occurred rapidly within 20 min, and 80 % of the equilibrium adsorption capacity was reached. Multilayer adsorption was confirmed by Freundlich model, and adsorption process was found to be spontaneous, endothermic, disordered, and the equilibrium adsorption amounts of SMX on SPM increased with salinity and organic matter increase. SMX desorption from SPM occurred upon the sudden changes of hydrodynamic states, nearly reaching the one-fifth of the SMX equilibrium adsorption amounts within 30 min and the re-adsorption of SMX on SPM would occur with water remained stationary or the re-disturbance time prolonged. The dynamic adsorption process of SMX related with the physicochemical property changes of SPM, which was contributed to the hydrogen bonds, π–π interactions, surface complexation, significantly influenced by the pore filling at the macropore and mesopore scales. The MIKE 21 simulations confirmed hydrodynamic states as the primary factors affecting the migration of SMX and SPM. SMX concentrations in the water would decrease in the presence of SPM, leading to the slower downstream migration of SMX.
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Water
·
2024
·Vol. 16
·期 2
·218
·
IF 3
Xiaohu Lin,Haifeng Fang,Libing Wang,Danyan Sun,Gang Zhao,Jingcheng Xu
Photocatalysis has emerged as a promising technology for the removal of emerging contaminants such as antibiotics from water. Fixing photocatalytic materials on polymers to prepare applicable membranes is a feasible method for applying photocatalysis. This study explored the preparation of composite PAN-TiO2and PAN-TiO2-rGO (PAN-rGTi) photocatalytic membranes by combining TiO2, TiO2-reduced graphene oxide (rGO) and polyacrylonitrile (PAN) using electrospinning. Characterization through SEM and EDS analysis confirms the composite membrane’s microstructure and elemental composition. The electrospun PAN-TiO2and PAN-rGTi composite membranes exhibit a stable and efficient photocatalytic performance in degrading sulfamethoxazole (SMX) and enrofloxacin (ENR), two typical antibiotics commonly found in water bodies. Photocatalytic degradation experiments under simulated solar light reveal the superior performance of the composite photocatalytic membranes compared to PAN alone, with a notable increase in the reaction rate constants of PAN-TiO2(1.8 to 2.2 times for SMX and 3.2 to 4.0 times for ENR) and even higher enhancements for PAN-rGTi (2.8 to 3.0 times for SMX and 5.4 to 6.5 times for ENR) compared to PAN alone. Despite minor decreases (from 97.6% to 90.4%) in activity over five cycles, the photocatalytic composite membranes remain effective, showcasing their stability and recyclability. This study highlights the potential application of PAN-TiO2and PAN-rGTi composite membranes as sustainable and effective materials for removing emerging contaminants from water. Further exploration should focus on optimizing materials for specific emerging contaminants and improving their application feasibility for wastewater and water treatment and water purification in water bodies.
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