CHEMOSPHERE
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2022
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IF 8.943
Zhibin Liu,Xiuping Sun,Zhirong Sun
Developing highly efficient, stable, recyclable, and application value heterogeneous catalysts in advanced oxidation processes has essential application value in the degradation of refractory pollutants. In this paper, the CoNi alloy anchored onto N-doped porous carbon (CoNi-600@NC) catalyst was prepared using bimetallic doped metal-organic frameworks as precursors. The magnetic CoNi-600@NC can activate peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). Therefore, SMX can be removed 100% within 25 min. CoNi-600@NC/PMS has a broad pH (3–9) application range, good applicability, and repeatability. Radical quenching, quantitative and electrochemical experiments proved that the degradation of SMX was dominated by free radical (Superoxide anions) and non-free radical pathways (surface-bound radicals). Mechanistic analysis showed that the interaction between Co-N x /pyridine N-sites and graphitized carbon with PMS induced the formation of surface-bound active species. Moreover, CoNi nanoparticles promoted the redox cycle of metals. The synergistic catalytic mechanisms between the CoNi alloy and the abundant functional groups gave CoNi-600@NC excellent catalytic properties and applicability. Using density functional theory predicted the reaction sites of SMX and proposed four degradation pathways. The toxicity of intermediates was comprehensively evaluated. In addition, a CoNi-600@NC continuous flow reactor was constructed with a daily treatment capacity of 45 L and 100% SMX removal. This study expands the application of persulfate advanced oxidation technology by synthesizing recyclable magnetic catalysts and provides new synergistic degradation mechanisms for removing refractory organics.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jiayi Wu,Rui Wang,Yuyao Zhang,Baoliang Chen,Xiaoying Zhu
The interaction force of a typical antibiotic molecule during adsorption has never been experimentally determined and fractionated, which hindered the evolution of removal strategies. In this study, sulfamethoxazole (SMX) as a typical antibiotic was stably immobilized onto an atomic force microscopy (AFM) tip without affecting original properties. The SMX modified AFM tip visualized the potential adsorption sites on a graphene oxide (GO) nanosheet for the first time by mapping the SMX adhesion force distribution. Moreover, the interaction force of a single SMX molecule to GO was determined at 38.6 pN which was subsequently fractionated into the hydrophobic (17.9 pN) and π-π (160.0 pN) attractions as well as the electrostatic repulsion (− 139.3 pN) at pH: 5.7. As compared with highly-ordered pyrolytic graphite (HOPG), the introduced oxygen containing groups on GO not only reduced the hydrophobic interaction but also generated an opposite electrostatic repulsion force to SMX. This study experimentally and theoretically revealed the adhesion mechanisms of SMX and potentially other sulfonamide antibiotics in molecular level, which may contribute to the study of antibiotic environmental transportation and the development of next-generation antibiotic remediation protocols.
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CHEMOSPHERE
·
2020
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IF 5.778
Shizong Wang,Jianlong Wang
To enhance the mineralization of toxic organic pollutants is crucial for the alleviation of environmental pollution . In this study, the successive non-radicals and radicals process (SNRP) of peroxymonosulfate (PMS)-based oxidation was performed using various methods for PMS activation , including UV, ozone, gamma radiation and biochar and applied for enhancing the mineralization of sulfamethoxazole (SMX). The results showed that SNRP-UV could improve the mineralization of SMX, and both SNRP-UV and PMS/UV could completely mineralize SMX. For SNRP-Ozone, SNRP-Radiation and SNRP-Biochar, compared to the sole radical oxidation, all SNRPs could enhance the mineralization of SMX. The biochar-induced SNRP obtained the maximum mineralization increment, followed by gamma irradiation-induced SNRP and ozone-induced SNRP. Sulfate radicals were mainly responsible for SMX mineralization for SNRP-Biochar, while hydroxyl radicals for SNRP-Radiation, and the synergetic effect of ozone and sulfate radicals for SNRP-Ozone. Different degradation intermediate products were identified in different SNRP, further revealing that SNRP induced by different methods had different mineralization capacity. This study further demonstrated that SNRP could be a new strategy for enhancing the mineralization of SMX.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Wei Wang,Abdul Saeed,Junyong He,Zhijun Wang,Deyi Zhan,Zixuan Li,Chengming Wang,Yufeng Sun,Feng Tao,Weihong Xu
Helical carbon fibers (HCFs) are a new kind of fascinating carbon material, and have caused much attention for their distinctive features, diversified novel properties, and applications. However, the application of HCFs still faces a series of barriers, especially in the repetitive preparation of HCFs. In this paper, we initially report the synthesis of the HCFs with ultrahigh specific surface area (3089 m 2 g −1 ) by a bio-template process using the high purified spiral vessels (SVs) as the template. The helical structure with the ultrahigh specific surface area can efficaciously shorten the pathway for antibiotics diffusion, and the high content of nanopores (1 to 3 nm) not only guarantees the accessibility of the surface for antibiotics storage but also easily provides approachable channels for antibiotics transmission. The highest adsorption capacity for sulfamethoxazole (SMX) is 1091 mg/g at pH 6.0 ± 0.1 with a stable temperature of 20 °C when the initial SMX concentration is 80 mg/L. This study motivates a new bio-inspired design for preparing the high purified HCFs with a simple bio-template method. The results show that the porous HCFs are a new kind of ultrahigh adsorption material for the removal of SMX in aqueous solution and can be used in new technological applications.
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CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Shizong Wang,Yong Liu,Jianlong Wang
In this study, the iron and sulfur co-doped graphite carbon nitride (FeO y /S-g-C 3 N 4 ) was easily prepared by one-step pyrolysis using thiourea and ferric chloride hexahydrate as precursors and applied to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). The characterization results showed that iron existed as Fe 2 O 3 and Fe 3 O 4 . Partial nitrogen atoms in the frame of g-C 3 N 4 were substituted by sulfur atoms. FeO y /S-g-C 3 N 4 can effectively activate PMS to produce sulfate radicals, hydroxyl radicals and singlet oxygen contributing to the SMX degradation. According to the density functional theory (DFT) calculation, the co-doping of iron and sulfur altered the charge density and its distribution of g-C 3 N 4 surface, which enhanced the PMS activation. The effect of initial concentrations of SMX and PMS, pH, temperature and inorganic ion concentrations on SMX degradation was investigated. 0.8 mM of PMS could degrade up to 10 mg/L of SMX. The initial pH had no obvious effect on the SMX degradation. Higher temperature accelerated the SMX degradation, and the activation energy was calculated to be 43.7 kJ/mol. The effect of inorganic ions was dependent on their initial concentration. Based on the comparison of XPS spectrum before and after reaction, the decreased catalytic activity of FeO y /S-g-C 3 N 4 after five cycle reuse was due to the breakdown of surface functional groups. Seven intermediate products were identified, and the possible degradation pathway was proposed. This study could provide a facile and cost-effective method to synthesize the efficient activator of PMS, and a mechanistic insight into PMS activation by FeO y /S-g-C 3 N 4 for the degradation of emerging pollutants in water and wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yanan Shang,Cheng Chen,Ping Zhang,Qinyan Yue,Yanwei Li,Baoyu Gao,Xing Xu
In this work, the nitrogen-doped carbon nanotubes with encapsulated Fe 3 C nanoparticles (Fe 3 C@NCNTs) were prepared through a simple process by pyrolyzing the precursor of ferric trichloride hexahydrate and melamine composite. It was studied systematically that multiple Fe 3 C@NCNTs synthesized under 600–1000 °C activated persulfate (PS) for the degradation of sulfamethoxazole (SMX), a widely used antibiotic of sulfonamides. Raman spectrum , X-Ray Diffraction (XRD), X-ray photoelectron spectroscopy (XPS) were used to characterize the transformation of catalyst with the increase of annulling temperature. The Fe 3 C@NCNTs synthesized under 800, 900 and 1000 °C showed similar degradation ability to SMX with degradation rates of 0.650–0.893 min −1 . During catalytic process, the specific structure of Fe 3 C encapsulated NCNTs could both benefit the electron transfer and prevent the Fe 3 C dissolving in the solution. The results of quenching experiments coupling with electron paramagnetic resonance (EPR) spectra suggested the OH, SO 4 − and 1 O 2 contributed to the degradation of SMX and the singlet oxygen took effect for longer time. The degradation intermediates were mainly derived from the reactions of hydroxylation, oxidation , aniline ring opening, deamination, desulfonation, as well as bond cleavage. In terms of the density functional theory (DFT) calculations, the graphitic N exhibited the highest ΔE ads (−0.437 eV) for the PS molecule, and it was followed by the pyrrolic N (−0.304 eV), pristine graphene (−0.146 eV) and pyridine N (−0.072 eV), which means that the graphitic N is more favorable for the binding affinity with PS, forming the reactive complexes on the surface of the NCNTs catalysts to promote the nonradical oxidation.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2019
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IF 5.589
Lei Zhou,Xuerui Yang,Yuefei Ji,Jie Wei
The widespread occurrence of sulfonamides (SAs) in natural waters, wastewater, soil and sediment has raised increasing concerns about their potential risks to human health and ecological systems. Sulfate radical (SO 4 − )-based advanced oxidation processes (SR-AOPs) have become promising technologies to remove such contaminants in the environment. The present study systematically investigated the degradation of four selected SAs with different five-membered heterocyclic rings, namely, sulfamethoxazole (SMX), sulfisoxazole (SIX), sulfathiazole (STZ), and sulfamethizole (SMT), by thermo-activated persulfate (PS) process, and the role of heterocyclic rings was assessed particularly. The results revealed that all the selected SAs could be degraded efficiently by thermo-activated PS process and their decay rates were appreciably increased with increasing temperature. For instance, degradation rates of STZ increased from 0.3 × 10 −3 to 19.5 × 10 −3 min −1 as the temperature was increased from 30 to 60 °C. Under the same experimental conditions, the degradation rates of SAs followed the order of SIX > SMX ≈ STZ > SMT, which was in accordance with decay rates of their R-NH 2 moieties. Kinetic results indicated that five-membered heterocyclic rings could serve as reactive moieties toward SO 4 − attack, which were confirmed by frontier electron density (FED) calculations. Based on the transformation products identified by high-resolution mass spectrometry (HR-MS), five different oxidation pathways, including hydroxylation, aniline moiety oxidation, dimerization , sulfonamide bond cleavage, and heterocyclic ring oxidation/cleavage were proposed. Moreover, the degradation efficiency in real surface water (RSW) was found to be slightly slower than that in artificial surface water (ASW), suggesting that SR-AOPs could be an efficient approach for remediation of soil and water contaminated by these SAs.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Juntao Tang,Jianlong Wang
Fe-based magnetic nanoparticles (NPs) embedded into mesoporous carbon hybrid (Fe@MesoC) was successfully fabricated from Fe-based metal-organic framework (MIL-100(Fe)) through a pyrolysis method, which was for the first time proposed as a novel Fenton-like catalyst for the degradation of sulfamethoxazole (SMX). The catalytic activity of Fe@MesoC was systematically evaluated on the basis of several reaction parameters including initial pH, initial H 2 O 2 concentration and temperature. Under the optimal conditions, the Fe@MesoC composite demonstrated a superior catalytic activity for decomposing SMX in the presence of H 2 O 2 , and it accomplished 100% SMX and 54.5% total organic carbon (TOC) conversion within 120 min. Such outstanding performance can be explained by the excellent enrichment ability of the outer mesoporous carbon matrix, the abundant active sites of the inner Fe-based NPs, as well as the possible synergistic effect between the two components. Moreover, the facile electrons transfer from Fe 0 to iron oxide in the inner Fe-based NPs could facilitate the reduction of Fe 3+ to Fe 2+ ( represents the iron species anchored to the surface of the catalyst) and further improve the generation of hydroxyl radicals. With the high structural stability and saturation magnetization, the Fe@MesoC composite can be easily recycled for three subsequent runs without significant activity loss. The possible catalytic mechanism and degradation pathways for SMX degradation induced by hydroxyl radicals in Fe@MesoC/H 2 O 2 Fenton-like system were also tentatively proposed.
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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.
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ENVIRONMENTAL POLLUTION
·
2024
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IF 7.6
Yuanxiao Jin,Jiang Yu,Jie Yu,Yuerong Wu,Siwei Deng,Yinying Jiang,Zhi Huang,Donghai Wu,Weiwei Zhu
A novel carbon catalyst was created based on plant metallurgy strategy for organic pollutants removal. Plants rich in CeO 2 NPs in water were used as carbon precursors and pyrolyzed with urea to obtain Ce/N co-doped carbon catalysts, which were used in the degradation of sulfamethoxazole (SMX) by active peroxymonosulfate (PMS). The results showed that the Ce/N @BC/PMS system achieved to 94.5% degradation of SMX in 40 min at a rate constant of 0.0602 cm −1 . The activation center of PMS is widely dispersed Ce oxide nanocrystals, and CeO 2 NPs promote the formation of oxygen centered PFR with enhanced catalytic ability and longer half-life. In addition, N-doping facilitates the transfer of π-electrons within the sp2 carbon of biochar, increasing active sites and thus improving PMS activation efficiency. The degradation process was contributed to by both radical and non-radical activation mechanisms including 1 O 2 and direct electron transfer, with O 2 •- serving as 1 O 2 's precursor. Through the DFT calculations, LC-MS and toxicological analyses, the degradation pathway of pollutants and the toxicity changes throughout the entire degradation process were further revealed, indicating that the degradation of SMX could effectively reduce ecological toxicity.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Yali Song,Ziyan Li,Shuaibin Li,Cairong Yang,Long Huang,Xiaojing Zhang,Qiong Wang,Hongzhong Zhang
Holes and O 2 − have been proved the primary species for sulfamethoxazole (SMX) degradation in g-C 3 N 4 photocatalytic system. On the basis, P doped g-C 3 N 4 (PCN) photocatalyst with midgap states was prepared by the polymerization of urea and etidronic acid, in order to enhance the role of main species in SMX removal via tailoring band gap structure. Compared with g-C 3 N 4 , the energy gap, CB position and VB position of PCN change little, however, PCN shows lower recombination efficiency of photogenerated carriers, strong adsorption and harvest of more visible light due to the midgap states induced by P doping, which is favorable to improve the photocatalytic activity. When the additive amount of etidronic acid is 0.03 g for 10 g urea, the obtained PCN-0.03 exhibits excellent visible-driven photocatalytic ability on SMX degradation. The kinetic constant is 2.1 times than that of pure g-C 3 N 4 . Electron spin resonance tests and trapping experiments imply that OH, holes and O 2 − are produced and enhanced by PCN-0.03 under visible light in comparison with g-C 3 N 4 . Holes and O 2 − take the primary role in SMX photodegradation . The detailed and systematical work may provide an effective strategy for water purification , especially containing SMX.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhikang Deng,Jinyao Zhu,Chenyu Zeng,Rui Mu,Yongfei Ma,Zulin Zhang
Ferrate [Fe (VI)] has been shown to be an effective oxidant for pollutants degradation. However, its propensity to self-decompose in water has limited its application. In this study, a novel method was developed for the activation of Fe (VI) using corncob biochar (CBC) with assistance of electrochemistry (EC/Fe (VI)/CBC), aiming to continuous activation of Fe (VI) for the removal of sulfamethoxazole (SMX) from water. Experimental results showed a remarkable SMX removal efficiency of 99.23 %, with simultaneous removal of over 49.68 % of the total organic carbon (TOC) within 60 min (C 0 (Fe (VI)) = 0.50 mM, C 0 (SMX) = 0.02 mM, E = 25 V, m CBC = 20 mg). The electrochemistry was introduced to guarantee the regeneration of the functional groups on CBC, among which the C O was the possible active site for activation of Fe (VI). Excessive background constituents (NO 3 – , SO 4 2- , HCO 3 – , and HA) and high pH were critical influencing factors. The results of cyclic experiments and SMX removal in different real water have demonstrated the stability and potential practical applications of the EC/Fe (VI)/CBC system. The quenching, electron paramagnetic resonance, and probe experiments revealed that 1 O 2 and Fe (V)/Fe (IV) were identified as the primary active species responsible for the SMX degradation. Theoretical calculation further revealed that the N atoms of SMX were susceptible to be attacked by the reactive species. Subsequently, the SMX was transformed into non-toxic or less toxic products. This work suggested that the combination of electrochemistry and biochar to activate Fe (VI) was a promising technology for antibiotics elimination.
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