WATER RESEARCH
·
2022
·
IF 13.4
Chaomeng Dai,Si Li,Yanping Duan,Kah Hon Leong,Shuguang Liu,Yalei Zhang,Lang Zhou,Yaojen Tu
Carbon-based materials activated peracetic acid (PAA) to repair groundwater is an environmentally friendly and low-cost technology to overcome secondary pollution problems. In this study, thermally modified activated carbon (AC600) was applied to activate PAA to degrade sulfamethoxazole (SMX). And the effect of groundwater pH, chloride ion (Cl − ), bicarbonate (HCO 3 − ), sulfate ion (SO 4 2− ), and natural organic matter (NOM) on SMX removal by AC600/PAA process was studied in detail. PAA could be effectively activated by AC600. Increasing AC600 dose (10–100mg/L) or PAA dosages (0.065–0.39 mM) generally enhanced the SMX removal, the excellent performance in SMX removal was achieved at 50 mg/L AC600 and 0.26 mM PAA. The removal of SMX was well-described by second-order kinetic, with the rate constant (k obs ) of 10.79 M −1 s −1 , both much greater than the removal constants of PAA alone (0.034 M −1 s −1 ) and AC600 alone (1.774 M −1 s −1 ). R-O·(CH 3 C(O)OO·, CH 3 C(O)O·) and electron-transfer process were proved to be responsible for the removal of SMX while HO· and 1 O 2 made little to no contribution to the novel PAA/AC600 system, which differs from typical advanced oxidation processes . The SMX can be removed effectively over a wide pH range (3-9), exhibiting a remarkable pH-tolerant performance. Sulfate ion (SO 4 2− ), dissolved oxygen (DO), NOM displayed negligible influence on the SMX removal. Bicarbonate (HCO 3 − ) exerted an inhibitory effect on SMX abatement, while chloride ion (Cl − ) promoted the removal of SMX. This showed excellent anti-interference capacity and satisfactory decontamination performance under actual groundwater conditions. Furthermore, the degradation pathways of SMX were proposed, there was no obvious difference in the acute toxicity of the mixed products during the degradation process. It will facilitate further research of metal-free catalyst/PAA system as a new strategy for groundwater in-situ remediation technology .
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Shizong Wang,Jun Hu,Jianlong Wang
In this study cobalt sulfides (Co 9 S 8 ) coated on the nitrogen and sulfur co-doped graphene (Co 9 S 8 @S-N-RG) was firstly prepared and used for degradation of antibiotic sulfamethoxazole (SMX). The results showed that SMX could be completely degraded by Co 9 S 8 @S-N-RG-activated peroxymonosulfate (PMS) within 20 min with its mineralization efficiency of 38.7%. The SMX degradation rate followed pseudo first-order kinetics with kinetic constant of 0.377 min −1 that was higher than that induced by Co 9 S 8 , N-RG, S-N-RG and Co 9 S 8 @S-RG, indicating Co 9 S 8 @S-N-RG had superior catalytic activity . Co 9 S 8 @S-N-RG can activate PMS to produce sulfate radicals and hydroxyl radicals , while sulfate radicals played major role. Co 9 S 8 participated in PMS activation in which Co 2+ was involved in sulfate radicals formation, while sulfur species facilitated the conversion of Co 3+ to Co 2+ . In addition, carbon defects, C O, pyridinic N and pyrrolic N also contributed to PMS activation.The superior catalytic activity was attributed to the synergistic effect of Co 9 S 8 and S-N-RG. This study could provide an efficient and stable PMS activator, and insight into the PMS activation mechanism by Co 9 S 8 @S-N-RG.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Amina,Qumber Abbas,Awais Shakoor,Mu Naushad,Balal Yousaf
Calcium peroxide (CaO₂) and persulfate (PS) dual oxidant system is an innovative in-situ chemical oxidation (ISCO) technique for the restoration of contaminated groundwater. Several field applications also confirm its efficacy in remediating the groundwater, however, published articles are rarely present. In this work, the performance of the CaO₂/PS system was examined for the degradation of sulfamethoxazole (SMX) in the SMX polluted soil and water. Results indicated that SMX could be efficiently degraded with CaO₂ and PS (2 g/L dosages for each oxidant) around neutral pH (7), and 95.8% pollutant removed after 36 h of reaction time. The removal efficiency of SMX improved as the concentrations of CaO₂ and PS were increased. Moreover, SMX removal was significantly decreased with the increase of initial solution pH. This dual oxidant system at 30 °C was also used for the remediation of SMX (10 mg/kg) spiked soil. Soil degradation experiment was performed at 150 rpm of shaking speed using soil slurry (soil/water; 1/1 ratio) at pH 7. Dual oxidant dosage was kept at 2 g/L CaO₂ and 2 g/L PS. The results showed that this dual oxidant system is also very efficient for the antibiotics SMX degradation in the soil system. Overall, an insight knowledge and practical information gained from this work will help in the treatment of SMX contaminated soil and water as well as wastewater with CaO₂/PS dual oxidant system.
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CHEMOSPHERE
·
2022
·
IF 8.943
Jinghao Wang,Huimin Liu,Song Song,Yuancai Chen,Yongyou Hu
Microbial electron output capacity is critical for organic contaminants biodegradation. Herein, original C. freundii JH could oxidate formate in anaerobic respiration, but lack the ability to degrade sulfamethoxazole (SMX). While the incorporation of Pd(0) could effectively improve the electron output via improving the combination between flavins and c-type cytochromes (c-Cyts), increasing the activities of key enzymes (formate dehydrogenase , hydrogenase, F 0 F 1 -ATPases), etc. More importantly, the presence of Pd(0) caused the NADH dehydrogenase (complex I) nearly in idle, and triggered the decrease of NADH/NAD + ratio and increase of H + -efflux transmembrane gradient, eventually resulting in the electrons diverting from CoQ-involved long respiratory chain (decreasing from 91.67% to 36.25%) to FDH/Hases-based hydrogen-producing short chain (increasing from 22.44% to 84.88%), which further intensified the electron output. Above changes effectively launched and guaranteed the high-level SMX degradation by palladized C. freundii JH, alleviating the ecotoxicity of SMX in aquatic and terrestrial environments. These conclusions provided the new view to regulate the microbial electron output behaviors.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Tao Ke,Shuyi Shen,Kun Yang,Daohui Lin
Developing visible-light-driven photocatalysts with high charge separation and transfer efficiency to degrade organic pollutants in wastewater remains a major issue. In this work, quaternary Bi 2 O 3 /C 3 N 4 /TiO 2 @C (BCTC) hybrids were successfully fabricated by hydrothermal and calcination two-step method using Bi(NO 3 ) 3 ·5H 2 O, C 3 N 4 , and Ti 3 C 2 as precursors. The optimized BCTC hybrids with the dosage of 1 g L −1 (BCTC-2%) exhibited high photocatalytic activity, degrading 100% sulfamethoxazole (SMZ, 5 mg L −1 ) within 100 min under visible light irradiation. Moreover, the photocatalytic degradation rate of SMZ by the quaternary junction was found to be 5.12-, 2.87-, and 1.35-fold higher as compared with Bi 2 O 3 /C 3 N 4 , C 3 N 4 /TiO 2 @C, and Bi 2 O 3 /TiO 2 @C junctions, respectively. The enhanced photocatalytic performance of BCTC hybrids could be attributed to the formation of a double Z-scheme photocatalytic system and the photosensitization of Bi 2 O 3 and C 3 N 4 . The photogenerated hole (h + ) was the primary reactive species that degraded SMZ. The plausible intermediates during the photocatalytic degradation of SMZ were identified by high-performance liquid chromatography quadrupole time-of-flight tandem mass spectrometry and the degradation pathway was postulated. Importantly, BCTC-2% had a good photocatalytic activity for degrading SMZ in natural water samples, indicating the high potential of BCTC hybrids for wastewater treatment applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yijie Feng,Wenjiao Sang,Zhiyi Deng,Shiyang Zhang,Cuihua Li
Co-N-C@SiO 2 with Co, N doped carbon as core and SiO 2 as shell was successfully synthesized by template method, and SiO 2 shell was about 43 wt%. Impressively, the SiO 2 shell increased the active sites of the core in Co-N-C@SiO 2 preparation, and reduced the loss of active sites during use. Co-N-C@SiO 2 /PMS was a 1 O 2 dominated non-radical reaction, which was less interfered by solution pH and water constituents. In addition, Co-N-C@SiO 2 possessed better cycling performance compared with Co-N-C. Finally, the possible SMX degradation pathways were presented based on the identified intermediate products.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Xinyao Liu,Liangjie Wang,Feng Qian,Zhuolin Qing,Xiaolin Xie,Yonghui Song
Nitrogen-doped carbon materials can effectively activate peroxymonosulfate (PMS) to degrade organic pollutants. In this study, one or more of the following raw ingredients, ferric nitrate, dopamine hydrochloride and melamine, were used as raw materials to prepare different carbon-based catalysts. The different effects of each raw ingredient on the performance of the catalyst were studied. Characterization by X-ray diffract grams spectra, Raman spectroscopy and X-ray photoelectron spectroscopy found that Fe(NO 3 ) 3 ·9H 2 O in the catalyst is beneficial to promote the degree of graphitization, and melamine can increase the nitrogen content in the catalyst. The prepared Fe-DA-CN catalyst, prepared with three materials has the highest activity. When the catalyst dose was 50 mg/L and the PMS concentration was 0.25 mM, the removal rate of 5 mg/L sulfamethoxazole (SMX) reached more than 99% after 30 min of reaction; furthermore, the pH, presence of inorganic anions (HPO 4 2- , NO 3 – , CO 3 2– , Cl - ) and presence of humic acid had little effect on the SMX removal rate. Repeated use experiments show that the catalyst has good stability. Through electron paramagnetic resonance and quenching tests, it is found that the main active substances that activate PMS to degrade SMX are free radicals (·OH, SO 4 ·- ) bound on the catalyst surface and a small part of singlet oxygen ( 1 O 2 ).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yinghao Li,Wenjie Zhu,Qian Guo,Xi Wang,Liming Zhang,Xiaoya Gao,Yongming Luo
The cobalt ferrite materials (Co x Fe 3−x O 4 ) with different molar ratios of Co:Fe (1:16, 1:8, 1:4, 1:2, and 3:4) were synthesized by simple co-precipitation method, and used for catalyzing activation of peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). The effects of catalyst dose, PMS dose, pH value, and inorganic ions on the degradation of SMX were investigated. Particularly, the degradation efficiency of SMX reached 91% within 10 min in CoFe 2 O 4 /PMS, and the removal rate of SMX achieved 81% at first 1 min. Meanwhile, the CoFe 2 O 4 /PMS reaction system exhibited excellent catalytic performance at a wide pH range from 3.00 to 11.00. The CoFe 2 O 4 catalyst could be easily magnetically separated and exhibited high stability in cycle experiments. EPR and quenching experiments showed that 1 O 2 , SO 4 − , and OH species were produced in the CoFe 2 O 4 /PMS system, especially OH and 1 O 2 played dominant roles during the degradation of SMX. The catalytic degradation mechanism of SMX in the CoFe 2 O 4 /SMX system was proposed, involving radical process and non-radical process. This work will provide a new way for the efficient treatment of wastewater especially those containing SMX compounds.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Lehui Ren,Mei Chen,Jinxing Ma,Yang Li,Zhiwei Wang
In this study, a novel reactive electrochemical membrane (REM) made of Pd-loaded porous Ti was prepared to achieve ultrafast and efficient oxidation of trace antibiotics sulfamethoxazole (SMX) under anodic polarization. At a current density of 0.5 mA/cm 2 , the percentage removal of SMX by the REM was 96.3% in flow-through mode, with the energy cost ( i.e. , the electrical energy per order of removal, 1.34 Wh/m 3 ) being much lower than the flow-by mode (125.76 Wh/m 3 ) under the same operating condition. Quenching experiments and electron spin resonance spectra demonstrated that singlet oxygen ( 1 O 2 ) was the main reactive oxygen species in the REM system, playing a vital role in SMX degradation. Results of this study indicated that 1 O 2 was mainly generated on the anode via Pd–O 2 interaction that directly activated oxygen, rather than the evolution of 1 O 2 precursors ( e.g ., O 2 − and H 2 O 2 ). The constantly high electrochemical removal of SMX (88.5–91.9%) from actual surface water demonstrated that the matrix effect on the process performance was minimal in realistic applications, highlighting this novel REM to be a viable way to remove trace organic contaminants from surface water.
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WATER ENVIRONMENT RESEARCH
·
2019
·Vol. 92
·期 4
·604-611
·
IF 1.24
Weifan Liu,Daqiang Yin,Xiaohong Guan,Dandan Rao,Guomin Cao,Yuankui Sun
Activating permanganate with reductants has gained increasing attention recently for efficient organic contaminants abatement via reactive intermediate Mn species. However, few studies have been conducted to explore the role of pyrophosphate (PP), a typical complexing agent for intermediate Mn species, in activated permanganate systems. In this study, taking sulfamethoxazole (SMX) as a probe compound, the influences of PP on SMX degradation by permanganate/thiosulfate and permanganate/hydroxylamine were extensively studied. It was found that both thiosulfate and hydroxylamine were able to activate permanganate for oxidation of SMX in the absence of PP. However, upon the introduction of PP, opposite effects were observed in the two systems where PP further improved the activation of permanganate by thiosulfate but dampened the performance of permanganate/hydroxylamine markedly. For permanganate/hydroxylamine system, MnO 2 was determined to be the only reactive oxidative species accounting for SMX degradation in the absence of PP, and its generation could be completely inhibited by PP. While in permanganate/thiosulfate system, both Mn(V) and MnO 2 were responsible for SMX oxidation, and the introduction of PP could strengthen the oxidative ability of Mn(V). These results could shed some insights on the suitability of applying PP to explore the kinetics and mechanisms of manganese involved redox reactions. Practitioner points Both Na 2 S 2 O 3 and NH 2 OH·HCl can activate KMnO 4 for SMX removal without PP. MnO 2 is the reactive oxidative species involved in KMnO 4 /NH 2 OH·HCl system. Mn(V) and MnO 2 account for the SMX oxidation by KMnO 4 /Na 2 S 2 O 3 system. PP could inhibit the formation of MnO 2 but enhance the oxidative ability of Mn(V).
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yinxue Li,Hongru Shang,Yongna Cao,Chunhui Yang,Yujie Feng,Yanling Yu
This study aimed to investigate the degree of contribution of adsorption mechanisms of sulfamethoxazole (SMX) on corncob - derived biochar CC800 through competition experiments. The SMX adsorption was governed by diverse mechanisms under different pH, resulting in high pH dependent adsorption of SMX on biochar. The adsorption of SMX on CC800 in the presence of ions was evaluated, demonstrating that the ion exchange mechanism had a weak effect on the adsorption. The intense competitiveness of SMX structural analogs verified π + –π electron donor-acceptor (EDA) effect was the dominant adsorption mechanism of SMX on CC800 at low pH, and the negative charge-assisted hydrogen bond (CAHB) was critical to the adsorption at high pH. The adsorption mechanisms contribution of SMX on CC800 were further quantified. The SMX adsorption on CC800 was mainly controlled by 51% pore filling and 43% π + –π EDA effect in the acid region, 62% pore filling mechanism and 25% (−)CAHB mechanism in the alkalic region, and less than 5% of hydrophobic interaction and ion exchange. Consequently, the above mechanisms provided a theoretical basis for biochar application to remove sulfonamide antibiotics and other similar organic contaminants and targeted design of biochar products. Also, this quantification method can be extended to quantify the adsorption mechanisms between other antibiotics or organics and biochar adsorbent materials by selecting suitable adsorption competitors.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Wang Lu,Nan Chen,Chuanping Feng,Ning An,Yanyan Dong
Although has high oxidation capacity and low toxic by-product formation potential, the feasibility, mechanism, and antibiotic treatment performance of peracetic acid (PAA)-based electrochemical system remains unknown. This work systematically studied the electro-activation process of PAA, and distinguished the different mechanisms of anode and cathode. In the PAA-based electrochemical system, the anode mainly produces BDD(•OH), and the cathode is mainly the R-O• (especially CH 3 CO 3 •). These differences lead to different degradation pathway and toxicity evolution of sulfamethoxazole (SMX). The anode transformation products (TPs) show negative toxicity and are difficult to be further removed, while TPs from PAA-dominated cathode posed electron-donating effect and a tapering ecological risk. The BDD(•OH) can well mineralize the TPs produced from cathode. Moreover, the active chlorine produced by the anode can effectively avoid the accumulation of NH 4 + - N released by antibiotic degradation. In an undivided cell, PAA-based treatment for real antibiotic wastewater achieved 73.9%, 59.4%, 76.9%, and 31.7% of COD, TOC , NH 4 + - N, and TN removal, respectively. More importantly, when PAA existed in this system, the active chlorine and AOCl accumulation are inhibited (inhibition ratio 83.5% and 82.7%, respectively). This study provides theoretical and technical support for the practical application of PAA-based electrochemical system.
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