SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Quan Chen,Hongjuan Feng,Jihong Dong,Yu Huang,Peng Yi,Min Wu,Bo Pan
Sorption and degradation occur simultaneously during the removal of aromatic organics by biochar. However, the unclear association between sorption and degradation limited our understanding of the underlying mechanisms of organic removal by biochars. Herein, the removal of monocyclic 2,6-dimethylphenol (DMP) and bicyclic bisphenol A (BPA) by raw and potassium hydroxide modified biochars was comparatively investigated by batch removal experiments and theoretical calculations. Under identical initial concentrations, biochar displayed lower sorption but higher degradation for DMP compared to BPA, whilst higher sorption corresponded to greater degradation for the same chemical. Sorption mechanisms revealed by molecular dynamic simulations include π-π, hydrophobic, and hydrogen bonding interactions. Density functional theory calculations identified the preferred degradation sites on biochar for adsorbed organics are graphitic nitrogen, defects, carboxyl, and hydroxyl functional groups. Analysis of free radicals and degradation intermediates concluded that the degradation pathways involve both free radical pathways and electron transfer processes for DMP, while only free radicals for BPA. Experimental and computational results indicated an increase in ring quantity can lead to higher sorption affinity but lower degradability of aromatic organics by biochar. Findings of this research provide theoretical support for the advancement of biochar based aromatic contaminant mitigation strategies.
研究领域:
环境科学
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化学
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高影响因子
Water
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2024
·Vol. 16
·期 24
·3658
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IF 3
Jialin Chen,Yi Xie,Jun Xia,Xiaolin Zhang,Dong Chen
An advanced photochemical reduction system involving the UV/Fe(III)–oxalate system was developed for the reduction of nitrate (NO3−) to harmless N-gaseous species, primarily nitrogen (N2), by carbon dioxide radical (·CO2−) generated in the presence of dissolved oxygen (DO). Electron paramagnetic resonance (EPR) analyses confirmed the presence of both ·CO2−and ·OH radicals. Systematic investigations were conducted on various operational parameters, such as the initial Fe(III) concentration, oxalate concentration, and pH levels, to assess their impacts on the efficiency and products of NO3−reduction. Notably, solution pH played a significant role in influencing the NO3−reduction efficiency and the final products. At pH 2, approximately 75% of NO3−was converted into N2with an 80% selectivity. In the pH range of 3 to 5, a remarkable NO3−removal rate of about 90% was achieved. Furthermore, higher concentrations of Fe(III) (2 mM) and oxalate (10 mM) were found to enhance NO3−removal to 91.95% and 88.71%, respectively. The presence of DO increased the oxidative potential in the reaction system, subsequently enhancing the selectivity conversion of NO3−to N2. In summary, the UV/Fe(III)–oxalate system exhibits significant potential for effective removal of NO3−while achieving high selectivity for the production of N2in water remediation applications.
研究领域:
环境科学
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化学
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高影响因子
Journal of Water Process Engineering
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2024
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IF 6.3
Da Wang,Yuyue Huang,Sisi Xiao,Qingjie Xie,Bianbadrolma,Huijuan Wang
This study applied the advanced oxidation process of simulated sunlight-induced periodate activation (SSL/PI) to degrade antibiotics. In order to enhance degradation, TiO 2 was also added to the SSL/PI system to create a synergistic effect (SSL/PI/TiO 2 ) and boost the degradation process. Sulfadiazine (SDZ) was selected as the target pollutant to investigate the enhancement from TiO 2 addition and the influential parameters on degradation. The obtained results showed that PI concentration was the most important parameter affecting SDZ degradation, while TiO 2 dosage and solution pH had less impact. Adding Fe 2+ and CO 3 2− inhibited SDZ degradation, while Cu 2+ and Cl − had minimal effect. DFT analysis indicated that the C4, C5, N23, N26, and N27 sites of the SDZ molecule were susceptible to be attacked by the formed reactive species. The key reactive species responsible for SDZ degradation in the SSL/PI/TiO 2 system were •O 2 − , 1 O 2 , IO 3 •, and •OH. LC-MS analysis identified 10 main byproducts during SDZ degradation, then three possible degradation pathways were predicted. The concentration detection of I 2 , I 3 − , and HOI, along with lettuce seed germination experiments, verified that the toxicity of the SDZ solution reduced after treatment with the SSL/PI/TiO 2 process.
研究领域:
环境科学
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化学工程
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高影响因子
Journal of Water Process Engineering
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2025
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IF 6.7
Weibao Liu,Shengwen Zhou,Wen Xu,Jiangwei Shang,Ming Yi,Xiuwen Cheng
The advancement of environmentally friendly, cost-effective and efficient persulfate catalysts represents a pivotal step in the evolution of advanced oxidation technology involving persulfate. In this study, manganese sand composites modified with Co 3 O 4 quantum dots were prepared by isovolumetric impregnation and employed to activate persulfate (PMS) for levofloxacin (LVF) degradation. The resulting materials were characterized, and the results demonstrated that the Co 3 O 4 quantum dots enhanced the electron transfer ability of the materials, which in turn improved the catalytic ability. The degradation rate of levofloxacin was 99 % within 60 min, and the total organic carbon mineralization rate was 46 % at dosages of 0.4 g/L and 0.3 g/L of catalyst and PMS, respectively. The results of probe experiments demonstrated that •OH, SO 4 •- , and non-radicals were responsible for 11.8 %, 6.6 % and 81.6 % of the observed degradation, respectively. Potential degradation pathways of levofloxacin were proposed based on HPLC-MS and Fukui index analysis, and the toxicity changes of the degradation products were investigated. Cycling experiments and ionic dissolution tests demonstrated the stability of the material, which exhibited 94 % degradation and a markedly reduced ionic dissolution at the fifth cycle. Subsequently, the Co 3 O 4 quantum dots‑manganese sand composite system was evaluated in extended continuous flow device experiments for the treatment of real medical wastewater. The mineralization rate of the medical wastewater was 77 % in 48 h of operation, demonstrating the feasibility of the reaction system for the treatment of real medical wastewater and providing technical references for the future treatment of difficult-to-degrade organic wastewater.
研究领域:
环境科学
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化学工程
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xinyu Wang,Shiqi Chen,Can Liu,Jiapeng Yue,Zhiwei Yang,Qian Ye,Hao Xu,Yujian Zhang,Xinyi Xing,Jing Zhang
In this study, the charge transfer capability of MoO 2 materials was significantly improved by introducing carbon materials in situ. The resulting MoO 2 -C material could accelerate the Fe(III)/Fe(II) redox cycle and promote the continuous generation of reactive oxygen species in Fenton-like system. The results suggested that MoO 2 -C exhibited significant co-catalytic activity against a variety of pollutants. Meanwhile, the mechanisms behind the Fe(III)/Fe(II) cycle and reactive oxygen species generation were clarified. Analysis indicated that the incorporation of carbon material provided a reduction active site for the reduction of Fe(III) to Fe(II) on the surface of molybdenum oxide, and also reduced the thermodynamic energy barrier associated with Fe(III) reduction. Furthermore, quenching experiments and electron paramagnetic resonance (EPR) technology demonstrated that hydroxyl radicals ( ∙ O H ) and singlet oxygen ( 1 O 2 ) rapidly degrade the target pollutants. Fe(II) was verified as the primary component responsible for peroxymonosulfate (PMS) and peroxydisulfate (PDS) activation. Additionally, the main generation pathway for 1 O 2 differed between the MoO 2 -C/Fe(III)/PDS and MoO 2 -C/Fe(III)/PMS systems. This study provides a new strategy to improve the iron reduction properties of metal oxide materials.
研究领域:
环境科学
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催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Tianyao Shen,Yi Yang,Haihe Yu,Peng Wang,Peng Xu,Jianhua Qu,Guangshan Zhang
Coal is the primary energy and consumption accounts for a higher proportion of fossil fuels, but its combustion product (fly ash) is a hazardous industrial solid waste (ISW). To alleviate its environmental problem and reuse waste, an appropriate disposal method for fly ash was proposed, which is using fly ash to construct the ceramsite as a catalyst carrier. To improve the catalysis property of the composite, layer double oxides (LDO) was doped into the lightweight ceramsite (CoFe-LDO/FAC) with dielectric barrier discharge plasma (DBDP) catalysis activity. In addition, following the mindset of a “waste-to-waste” strategy, apply the composite ceramsite enhancing the diuron-containing (DUR) water purification in a DBDP self-Fenton-like system, creatively using one stone kills two birds. The porous structure endows the CoFe-LDO/FAC possessed water adsorption ability, assisting oxidants and contaminants diffusion with water inside CoFe-LDO/FAC. More than 95 % of DUR could be removed within 10 min, and the DBDP + CoFe-LDO/FAC performed the properties of stability as evidenced by low metal ion leaching in the eight times recycle. During the catalysis process, CoFe-LDO/FAC promotes the dominant reactive species ( 1 O 2 and • OH) yield by the valence cycle of Fe 2+ /Fe 3+ and Co 2+ /Co 3+ in DUR decomposition. Abundant oxygen vacancy remedies the electron consumption and maintains the surface charge balance. This work provides a novel application of fly ash and LDO in water treatment and is helpful in ISW disposal.
研究领域:
环境科学
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材料科学
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高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Zishui Dong,Sinuo Li,Eldon R. Rene,Yixuan Liu,Weifang Ma
2,4,6-Trichlorophenol (2,4,6-TCP) is commonly used in the production of insecticides and preservatives with the characteristics of accumulation and toxicity due to the complex chemical structure with a halogenated aromatic ring. In order to effectively degrade and mineralize 2,4,6-TCP from water, a stack-coral-like catalyst of magnetic sulfur doping constructed nitrogen vacancies in graphitic carbon nitrides (Fe 3 O 4 /S-g-C 3 N 4 , FSCN-T) was designed and prepared through polymerization combined with precipitation. This visible-light-driven photocatalytic degradation to 5 mg/L 2,4,6-TCP was 95 % within 60 min with 0.1 g/L FSCN-T amendment. The degradation and carbonization rate constant were 0.118 and 0.089 min −1 respectively. This high removal was attributed to nitrogen vacancies, which broaden the visible light absorption range and shorten the electron transfer path with narrow CN bandgap (from 2.94 eV to 2.49 eV). Moreover, the introduction of iron accelerated electron cycling and enhanced magnetic recovery performance with above 95 % recovery and catalytic stability after 5 cycles of use. The degradation contribution from the active species were h + (41 %)> •OH (28.9 %) > •O 2 - (16.1 %)> 1 O 2 (8.7 %). This degradation underwent three pathways of substitution, elimination, and hydroxyl oxidation. Further, the intermediates were oxidized with ring opening and mineralization according to density functional theory (DFT) calculations and LC-Qtof-MS identification. The oxidative degradation process reduced the toxicity of 2,4,6-TCP and its intermediates. This study provided an efficient catalyst and low-energy consumption approach for toxic wastewater treatment.
研究领域:
环境科学
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材料科学
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高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Yifei Leng,Ying Zhang,Xiong Chen,Ting He,Fengyi Chang,Zhu Li,Yu Huang,Jun Wang,Wen Xiong
The catalysis of horseradish peroxidase (HRP) and activated persulfate (PDS) are both feasible ways to remove heterologous contaminants. This work demonstrated that HRP/H 2 O 2 can effectively activate PDS to degrade sulfadiazine (SDZ). Types of salt ions could suppress the efficiency of the system through free radical scavenging of anions and superposition effect of part cations, followed the series: FeCl 3 > CaCl 2 > NaCl > NH 4 Cl > NaHCO 3 > NaNO 3 . 5 mg L −1 humic acid (HA) could decrease 5.14 times transformation rate constants K . Interestingly, the addition of the above salt ion can slightly restore the level of inhibition by HA. Fourteen possible intermediates were identified, and potential pathways and mechanisms were proposed. There were three pathways to transform SDZ in systems. HRP directly acted on SDZ after being activated by H 2 O 2 , including δ/γ site-cleavage, hydroxylation, denitrification, carbonylation, and sulfur oxide (SO 2 /SO 3 ) extrusion. In addition, both HRP activated PDS and thermal/H 2 O 2 , generating SO 4 - • and •OH for the oxidation of SDZ, including oxidation of the α-amine, hydroxylation of the benzene ring, ζ position cleavage on SDZ. The electron paramagnetic resonance (EPR) technique verified that specific free radicals had been generated and that HRP could activate the PDS process. The ECOSAR software predicted the biotoxicity of most transformation products was less toxic than the parent compound. The results of luminescence inhibition of Vibrio fischeri indicated the low toxicity of SDZ intermediates. These findings may help us expand our knowledge of PDS activation approaches and may also provide a potential method for antibiotic removal in environments.
研究领域:
环境科学
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生物化学
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高影响因子
C-Journal of Carbon Research
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2024
·Vol. 10
·期 3
·75
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IF 3.9
Yanchi Zhou,Xingdi Ma,Zhonglin Chen,Ruihang Chen,Yingxu Gong,Lei Cui,Jing Kang,Jimin Shen,Shengxin Zhao,Chen Li
Hydrothermal carbonation carbon (HTCC) is emerging as a promising material for the adsorption and photodegradation of environmental contaminants. However, the chemical and structural properties of HTCC derived from different lignocellulose biomass have obvious impacts on adsorption and photodegradation. This work employed three different lignocellulose components, including cellulose, hemicellulose, and lignin to synthesize HTCC within a hydrothermal temperature range of 210~290 °C. In comparison to HTCC derived from cellulose and hemicellulose, HTCC derived from lignin (HTCC-L) demonstrated the optimal synergistic adsorption and photodegradation ability for TC degradation, achieving a 63.5% removal efficiency within 120 min. Characterization highlighted the crucial involvement of oxygenated functional groups, especially carboxyl groups, presented on the surface of HTCC-L in TC adsorption. Moreover, the photodegradation of HTCC-L was found to follow a non-radical mechanism, characterized by the charge transformation occurring between the excited unpaired electrons of HTCC-L and TC adsorbed on its surface. This work clarified the differences in HTCC derived from different lignocellulose components on the adsorption and photodegradation of organic pollutants, and provided a novel perspective on the application of HTCC in water treatment.
研究领域:
环境科学
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材料科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Dandan Yang,Chao Xie,Yulian Li,Zijian Wu,Yahui Li,Jiandong Lu,Peidong Hong,Junyong He,Zhengguo Zhu,Lingtao Kong
There is an urgent need to develop effective and sustainable methods for reducing water pollution. Non-homogeneous Fenton catalysts are commonly used to eliminate pollutants from water. However, the effectiveness of these catalysts is limited by the restricted availability and accessibility of the active site (AS). In this work, we presented a strategy for modulating the exposure of active nanometallic particles to fully expose the AS at the nanoscale. We also confined the AS in carbon frameworks with micropores and mesopores to enhance the effectiveness of AS utilization in Fenton-like reactions. The experimental results indicate that the Fe-out@N-C/PMS system achieved complete degradation of tetracycline within 10 min and maintained an efficient degradation rate of over 91% after five consecutive cycles. The degradation of contaminants was due to an effective non-radical mechanism, as shown by free radical quenching experiments, EPR reactive species capture tests, in situ Raman, and PMSO probe experiments. Furthermore, density-functional theory (DFT) calculations revealed that iron nanoparticles supported on nitrogen-doped carbon acted as active sites, enhancing electron transfer capacity (N-C (0.24 e) vs. Fe-out@N-C (0.69 e)). Finally, the intermediates have a limited environmental impact because of their extremely low concentrations, despite having a high relative toxicity. The exposed metal nanoparticle catalysts provide a new approach for effectively activating PMS to efficiently degrade organic contaminants with a high mineralization rate via the non-radical pathway.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Yinghao Li,Ying Li,Qinglong Meng,Ke Jing,Jingyi Zhang,Qingyu Guan
Achieving efficient phosphorus recovery and reuse from wastewater presents formidable challenges. In this study, a synergistic adsorption photocatalysis process was successfully constructed. 0.1Bi-MIL-101-NH 2 showed the maximum phosphorus adsorption performance of 112 mg/g. After phosphorus adsorption, photoelectrochemical measurements confirmed that the photoelectric properties of the 0.1Bi-MIL-101-NH 2 -P sample was improved, and the degradation efficiency of SMX was increased by 20 % within 120 min. Meanwhile, the mineralization rate reached 91 %. The incorporation of Bi significantly enhanced the adsorption energy of the 0.1Bi-MIL-101-NH 2 sample. Notably, the presence of phosphorus on the surface of 0.1Bi-MIL-101-NH 2 -P enhanced the adsorption of water molecules by the material, thereby augmenting the generation of •OH. •O 2 - and •OH played dominant roles in the photodegradation of SMX. Finally, the degradation pathways of intermediates were further studied by Density functional theory (DFT) calculations and LC-MS analysis. This study provides a new avenue for phosphorus recovery and organic pollutant degradation.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Hui Li,Xinlei Ren,Wenxue Pan,Shiting Zhu,Jin Zhang,Zhiyuan Yang,Liu Qian,Yueying Wang,Yujing Huang,Lin Guo,Minghui Xiang
The reasonable control of the structure of metal–organic frameworks (MOFs) is a promising strategy for improving their peroxymonosulfate (PMS) activation activity. In this study, ZIF-67 @ZIF-8 was used as a template to prepare bimetallic core–shell Co-Fe@NC via Fe doping and high-temperature carbonization . Co-Fe@NC maintained the core–shell structure of the original MOF, in which cobalt was uniformly distributed in the nitrogen-doped graphite carbon skeleton and the surface of the graphite carbon skeleton was covered with iron. With the synergistic effect of the nitrogen-doped graphite carbon skeleton, iron, and cobalt, 100% of tetrabromobisphenol S (TBBPS) was removed in 60 min with k obs = 0.062 min −1 in Co-Fe@NC-0.2/PMS system. The addition of iron increased the graphitization degree with I D /I G value increased from 0.98 (Co@NC) to 1.034 (Co-Fe@NC-0.2) and electron transfer rate of the carbon skeleton. Besides, the Co leaching was effectively attenuated from 1.86 mg/L(Co@NC) to 0.78 mg/L (Co-Fe@NC-0.2) by the core-shell structure and bimetal strategy. Both O 2 · - and 1 O 2 contributed to the degradation of TBBPS according to quenching experiments. TBBPS was deeply degraded into small-molecule compounds through three degradation pathways by the Co-Fe@NC-0.2/PMS system. This study provides a new strategy for designing highly efficient bimetal–carbon composites for environmental remediation.
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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高影响因子
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