JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qihui Wang,Zeyu Guan,Yi Xiong,Dongya Li
Lower reaction speed and excessive oxidant inputs impede the removal of contaminants from water via the advanced oxidation processes based on peroxymonosulfate. Herein, we report a new confined catalysis paradigm via the hollow hetero-shell structured CN@C (H-CN@C), which permits effective decontamination through polymerization with faster reaction rates and lower oxidant dosage. The confined space structures regulated the C N and C O and electron density of the inner shell, which increased the electron transfer rate and mass transfer rate. As a result, C N in H-CN@C-10 reacted with peroxymonosulfate in preference to C O to generate singlet oxygen, improving the second-order reaction kinetics by 503 times. The identification of oxidation products implied that bisphenol AF could effectively remove by polymerization, which could reduce carbon dioxide emissions. These favorable properties make the nanoconfined catalytic polymerization of contaminants a remarkably promising nanocatalytic water purification technology.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Linli Dai,Yi Xie,Yongkui Zhang,Yabo Wang
In this work, microorganism of Phanerochaete chrysosporium with iron-tolerating and accumulating abilities was cultivated and harvested as mycelial pellets, which could serve as a sustainable and environmental-friendly precursor for iron phosphide/N-doped biocarbon composite preparation. Through one-step pyrolysis process , the inherent Fe and P elements in mycelial pellet enabled the formation of well crystallized Fe 2 P particles, loading on N-doped biocarbon matrix. Benefiting from the porous structure, high specific surface area, N doping-induced defects and C O groups of biocarbon, as well as the good electron-donating property of Fe 2 P, the as-obtained Fe 2 P/BC composite performed well for bisphenol pollutant (e.g., BPAF) removal through peroxymonosulfate (PMS) activation. Specifically, almost complete BPAF removal was achieved within 30 min adsorption and 10 min catalysis process with an apparent reaction rate constant of 0.486 min −1 . The good crystallinity and protective carbon layer wrapping on Fe 2 P enabled the wide pH adaptability and low iron leaching of Fe 2 P/BC in catalytic reaction . Inorganic anions and humic acid brought only slight inhibition for BPAF removal, which could be overcome by prolonging reaction time to 30 min. Further mechanism studies indicated that reactive oxygen species , e.g., SO 4 - •, •OH and 1 O 2 were generated through both radical and non-radical pathways and contributed to BPAF degradation. After treatment by Fe 2 P/BC-PMS system, the total organic carbon (TOC) of original BPAF solution (20 mg L −1 ) was reduced by 51.6%. Fortunately, the residual degradation intermediate products showed much reduced ecotoxicity in both predicted (ECOSAR program) and experimental results (growth inhibition test using Raphidocelis subcapitata as ecological indicator).
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Yaxin Zhang,Zhuang Chen,Yimei Zhang,Wenwen Gu,Wendy Huang,Jiangshan Xi,Ting Cao,Yingjie Yu,Mingwang Yang,Luoyilang Ke
In this system, a highly-exposed TiO 2 photoanode was prepared as an effectively photoelectrocatalyst peroxymonosulfate (PMS) activator. Especially, we realize the highly-exposed TiO 2 grown on negatively charged MXene nanosheet which could provide dual active sites for stimulating PMS. The catalysts were characterized by XRD, XPS, SEM, UV–vis, Raman, TEM, and BET. The specific surface area for highly-exposed TiO 2 (S-400) is 10 times than Bulk catalyst (B-400), which is displayed in the BET result. The experimental results show that high exposure catalyst has excellent photoelectric activation performance. The degradation efficiency of the PEC + PMS system was 2.94 times higher than the EC + PMS and 2.76 times higher than the PC + PMS process. Compare with free PMS (1.36˚A), PMS adsorbed at the photoanode interface has a high bond angle (2.85˚A) easily to decompose into strong oxidizing SO 4 − . The electrochemical characterization results demonstrated that the highly-exposed TiO 2 had a higher separation rate of photogenerated carriers. From quenching experiments, the holes (h + ) contributed 80 % to BPA degradation in PEC + PMS system, the contribution order of other active radicals was O 2 − >SO 4 − > OH. It will help improving the control of the optimal free radical ratio. The probable mechanism and pathway of BPA degradation were suggested e − reacts with PMS and other substances to generate radicals. The research offers a new strategy for the effective activation about PMS to oxidation of the refractory organics. Besides, the results provide useful theoretical guidance for the development of new high-activity materials.
✓ 已验证
产品关联
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Bo Jiang,Yunshu Zhang,Cong Li,Jiaqi Guo,Chunmeng Sun
Nanoscale zero-valent iron loaded on N-doped biochar (nZVI/NBC) is a novel catalyst for activating peroxydisulfate (PDS) toward efficient degradation of endocrine disruptors in water. In this study, spent coffee grounds were modified by K 2 FeO 4 and then transformed into nZVI/NBC by one-step pyrolysis . The nZVI/NBC modified with 0.3 mol/L K 2 FeO 4 displayed an excellent PDS activating performance, and the specific surface area and average pore width of this nZVI/NBC were 277.19 m 2 /g and 2.47 nm, respectively. Bisphenol A (BPA) as a typical endocrine disruptor can be efficiently degraded by nZVI/NBC/persulfate advanced oxidation process . The optimum dosage of nZVI/NBC was 0.1 g/L, and the optimum PDS concentration was 20 mM. pH (3−9) had little effect on BPA degradation. In addition, the presence of Cl − had a facilitating effect on BPA degradation, while CO 3 2− and HPO 4 2− had strong inhibitory effects. nZVI/NBC had long-term stability in that the activation rate remained stable after five cycles and 90 days of storage in air and natural light. This study also investigated the activation mechanism of PDS by nZVI/NBC and concluded that radical (•OH, SO 4 •− , and O 2 •− ) and non-radical ( 1 O 2 ) processes were simultaneously presented under the synergistic catalysis of ZVI and N. The formation of metastable PDS intermediates on the surface of biochar substantially enhanced the adsorption of PDS/BPA and the electron transfer process. Finally, the degradation pathways of BPA were speculated based on nine identified intermediates. Overall, this study described a rapid and green method for nZVI/NBC fabrication, which simultaneously achieved the recycling of spent coffee grounds and the degradation of endocrine disruptors in water.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2022
·
IF 7.34
Xinfei Fan,Jia Yang,Na Liu,Yuanlu Xu,Yueling Yu,Chengwen Song,Yanming Liu
Peroxymonosulfate (PMS) activation based on iron-based catalyst has caught increasing attention in wastewater treatment , but is strongly impeded by the sluggish kinetics of Fe(II) recovery. In this study, nitrogen-doped carbon encapsulated Fe 3 C with dual-reaction centres coupled via C Fe channel was developed by electrospinning and Chemical Vapor Deposition (CVD) technique. The remarkable catalysis performance was conferred by the formation of C Fe short bond which linked C poor electron reaction centres from N-doped carbon frameworks and the Fe rich electron reaction centres from Fe 3 C. Fe@NC-800 achieved 100% sulfamethoxazole (SMX) degradation within 20 min, and showed excellent cycle stability after 5 cycles. The electron transfer rate between the dual-reaction region was accelerated due to short transport distance and low transmission resistance. Electrons from pollutants were compensated to Fe 3+ via C Fe bond bridges, promoting the regeneration of Fe 2+ and accelerating the efficiency of the Fe 2+ /Fe 3+ cycle. Besides, the experiments of reactive oxygen species (ROS) quenching and capture revealed the degradation pathway. Both radical and nonradical oxidation played a key role in the Fe@NC-800/PMS system. This work will offer a valuable clue on the design of multi-benefit catalysts to achieve efficient removal of pollutants in wastewater.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2023
·
IF 6.9
Xiuying Liu,Qianna Xia,Jiao Zhou,Bowen Li,Shuaiqi Zhao,Long Chen,Aimal Khan,Xiaoxia Li,Aihua Xu
The design of efficient heterogeneous catalysts in bicarbonate-activated hydrogen peroxide systems (BAP) is a hot topic in wastewater treatment. In this work, Cu 2 O nanoparticles with different morphologies including cubic shape (c-Cu 2 O), octahedron shape (o-Cu 2 O) and spherical shape (s-Cu 2 O), were applied in BAP for the first time to degrade tetracycline hydrochloride (TC). Compared with Cu 2+ ions and CuO, TC degradation was boosted in the presence of Cu 2 O in the BAP system, with the degradation rate following the order c-Cu 2 O > o-Cu 2 O > s-Cu 2 O. The morphology-dependent effects could be linearly correlated with the ratio of surface oxygen species (O S ), but not with the surface area or Cu(I) ratio. The c-Cu 2 O catalyst with exposure of (100) facets contained 76.6% O S as the active site for H 2 O 2 adsorption and activation, while the value was much lower for o-Cu 2 O and s-Cu 2 O with dominant (111) facets. The presence of HCO 3 − enhanced the interactions among Cu 2 O, H 2 O 2 and TC, leading to facile oxidation of Cu(I) to Cu(II) by H 2 O 2 , and the formation of various reactive species such as hydroxyl radicals and Cu(III) contributed to TC degradation. This work provides a new method for enhancing H 2 O 2 activation with heterogeneous catalysts by crystal facet engineering.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Binghong Chen,Jing Wang,Renjie Li,Hongjun Lin,Bisheng Li,Liguo Shen,Yanchao Xu,Meijia Zhang
Integration of sulfate radicals-based advanced oxidation processes (SR-AOPs) with separation membranes has enthralled considerable attentions because it can remove persistent toxic micropollutants in a low-energy and cost-effective manner. However, fabrication of such an integrated membrane simultaneously with excellent self-cleaning property, catalytic capability and long-term durability remains a challenge. Herein, for the first time, CoFe 2 O 4 (CFO) and Mn 3 O 4 (MO) nanoparticles were anchored on ultrathin graphitic carbon nitride (UCN) nanosheets via a solvothermal method to prepare heterogeneous Fenton-like catalysts (MO/CFOUCN). Systematic characterizations demonstrated the successful preparation of powder catalysts with favorable degradation ability. Notably, the optimal composite catalyst possessed satisfactory degradation (94.5 %) and kinetic rate (0.1367 min −1 ) for norfloxacin (NOR) within 30 min. Thereafter, an integrated MO/CFO/UCN@P membrane was fabricated by vacuum-assisted filtration of the catalyst on a supporting membrane surface. It was interestingly found that, benefiting from the synergistic effect of in-situ oxidation and membrane filtration, activating peroxymonosulfate (PMS) endowed the membrane with high removal rates (over 91.8 % for tetracycline, bisphenol A, humic acid (HA)) and high permeation flux (332.7 L·m −2 ·h −1 ) driven solely by gravity. Significantly, the membrane achieved a flux recovery rate of 91.9 % with the assistance of PMS after filtering HA solution. Furthermore, quenching experiments and electron paramagnetic resonance (EPR) tests confirmed that both radical and nonradical pathways contributed to the mineralization of NOR. Based on the detection of intermediates in the degradation process, potential NOR degradation pathways were proposed. Overall, this study provided new ideas about integrating Fenton-like catalysts with membrane technology for removal of persistent organic pollutants.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Sui-Qin Yang,Zheng-Qian Liu,Yu-Hong Cui,Ming-Kui Wang
Ubiquitous chloride ion (Cl - ) in wastewaters usually inhibits the degradation of organic contaminants and generates numerous toxic chlorinated products in conventional degradation-based advanced oxidation processes (AOPs). Herein, a more Cl - tolerant polymerization-based electrochemical AOP for organic contaminants abatement and simultaneous organic resource recovery was demonstrated with eight typical organic contaminants and two real industrial wastewaters for the first time. This process can significantly promote dissolved organic carbon (DOC) abatement in the presence of Cl - , differing greatly from conventional degradation-based processes. Compared to sulfate radical (SO 4 •- ) (or hydroxyl radical (HO • )), dichloride radical (Cl 2 •- ) derived from Cl - has moderate reactivity towards most contaminants, which facilitates the organics polymerization as it ensures the formation of polymerizable organic radicals while inhibiting their excessive degradation. Thus, high DOC abatement (over 75 %) and high organic resource recovery ratio (48–79 % separable organic-polymer yield) can be achieved for most contaminants. Both soluble chlorinated compounds and solid chlorinated polymers are formed in the presence of Cl - . The chlorinated products (e.g. chlorophenols) can be polymerized as new monomers , thus the concentration of dissolved organic chlorinated products is much lower than that in conventional degradation-based process. The tolerance of the present process to Cl - is tested in real coking wastewaters, and exceeding 60 % of the abated chemical oxygen demand (COD) is obtained in the form of recoverable organic-polymers.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Microorganisms
·
2022
·Vol. 11
·期 1
·67
·
IF 4.926
Kejian Tian,Yue Yu,Qing Qiu,Xuejian Sun,Fanxing Meng,Yuanping Bi,Jinming Gu,Yibing Wang,Fenglin Zhang,Hongliang Huo
Bisphenol A (BPA) pollution poses an increasingly serious problem. BPA has been detected in a variety of environmental media and human tissues. Microbial degradation is an effective method of environmental BPA remediation. However, BPA is also biotoxic to microorganisms. In this study,Rhodococcus equiDSSKP-R-001 (R-001) was used to degrade BPA, and the effects of BPA on the growth metabolism, gene expression patterns, and toxicity-resistance mechanisms ofRhodococcus equiwere analyzed. The results showed that R-001 degraded 51.2% of 5 mg/L BPA and that 40 mg/L BPA was the maximum BPA concentration tolerated by strain R-001. Cytochrome P450 monooxygenase and multicopper oxidases played key roles in BPA degradation. However, BPA was toxic to strain R-001, exhibiting nonlinear inhibitory effects on the growth and metabolism of this bacterium. R-001 bacterial biomass, total protein content, and ATP content exhibited V-shaped trends as BPA concentration increased. The toxic effects of BPA included the downregulation of R-001 genes related to glycolysis/gluconeogenesis, pentose phosphate metabolism, and glyoxylate and dicarboxylate metabolism. Genes involved in aspects of the BPA-resistance response, such as base excision repair, osmoprotectant transport, iron-complex transport, and some energy metabolisms, were upregulated to mitigate the loss of energy associated with BPA exposure. This study helped to clarify the bacterial mechanisms involved in BPA biodegradation and toxicity resistance, and our results provide a theoretical basis for the application of strain R-001 in BPA pollution treatments.Keywords:Bisphenol A;Rhodococcus;biodegradation;toxicity resistance
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qingyi Zeng,Yumei Wang,Qingyan Zhang,Jiayu Hu,Yanjun Wen,Jin Wang,Rongzhong Wang,Shuaifei Zhao
Transition metal sulfides have been demonstrated to be effective for peroxymonosulfate (PMS) activation towards wastewater treatment. However, the activity of vanadium sulfide (VS 4 ) and the role of the chemical state of V have not been revealed. Here, three types of VS 4 with various morphologies and chemical states of V were synthesized by using methanol (M−VS 4 , nanosphere composed of nanosheets), ethanol (E-VS 4 , sea urchin like nanosphere) and ultrapure water (U-VS 4 , compact nanosphere) as hydrothermal solvent, respectively, and used as heterogeneous catalysts to activate PMS for the degradation of refractory organic pollutants. The effects of PMS concentration, temperature, pH, inorganic ions, and humic acid (HA) on the degradation efficiency of VS 4 /PMS system were investigated systematically. The results indicated that the highest specific surface area and lowest ratio of V 5+ enable E-VS 4 /PMS system possessed the highest performance in degrading tetracycline hydrochloride (TCH), in which 100% TCH was removed after operating 10 min (0.805 min −1 ) under a relatively low concentration of PMS (1 mM) and catalyst (100 mg/L). It also revealed that the system exhibited a typical radical process in TCH degradation, which could be attributed to the redox cycles between V 5+ , V 4+ and V 3+ in the presence of PMS to generate various radicals. This radical process enabled the E-VS 4 /PMS system with a high activity in wide reaction conditions and high mineralization ratios in degrading various refractory organic pollutants within 10 min. In addition, the E-VS 4 /PMS system exhibited favorable reusability and stability with very less V and S ions leaching, and showed excellent performance in real water purification.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Separations
·
2023
·Vol. 10
·期 2
·123
·
IF 2.6
Zhou Cheng,Xuanhao Lin,Ming Wu,Guoping Lu,Yanru Hao,Cehui Mo,Qusheng Li,Jianfeng Wu,Jichun Wu,Bill X. Hu
Polyamide (PA) and bisphenol A (BPA) are selected as typical microplastic and endocrine-disrupting chemicals in this study. The adsorption of BPA on the surface of PA and the effect of PA on the transport behavior of BPA in groundwater are systematically investigated using a combination of batch experiments, column experiments and numerical models. The results of scanning electron microscope (SEM) and Fourier transform infrared spectra (FTIR) show that the surface of PA particles is changed significantly after adsorption of BPA. The isothermal adsorption process of BPA can be simulated by the Langmuir model and the Freundlich model. Kinetic adsorption, on the other hand, can be fitted by a quasi-first-order adsorption model, and the adsorption results indicate that the maximum adsorption of BPA on PA reaches 13 mg·g−1. The results of the column experiments suggest that the mass recovery rate of BPA decreases with PA content, and increases with flow velocity, while initial concentration has no apparent influence on BPA transport. In addition, due to the hydrolysis of BPA, the mass recovery rate of BPA does not change with pH under conditions of pH < 10.2 and increases substantially to 94% when pH > 10.2. Moreover, Ca2+has a significant inhibitory effect on the transport of BPA, while Na+has no apparent influence on the transport of BPA. The transport process of BPA in porous media is simulated using a single-point kinetic model, and the fitted mathematical relationships for the variation of kinetic parameters with environmental factors are obtained by regression analysis.Keywords:bisphenol A;microplastics;adsorption;transport;polyamide;kinetic parameter
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）