CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Zehua Zeng,Aimal Khan,Zixuan Wang,Mengmeng Zhao,Wanling Mo,Zhuqi Chen
In this study, a series of Mn based catalysts with different oxidative states, crystal structures and morphologies was applied to activate peroxymonosulfate (PMS) for the degradation of atrazine (ATZ). Among them, α-MnO 2 nanowires (Mn-1) demonstrated the highest efficiency. The structure-performance relationship study revealed that the generation of Mn(III) along with the transformation of lattice oxygen to surface hydroxyl groups played the dominant role in controlling the efficiency, and Mn-1 are prone to undergo electron transfer to achieve the transition from Mn(IV) to Mn(III) or even Mn(II). Both radical (sulfate radical (SO 4 •− ) and hydroxyl radical (•OH)) and non-radical species ( 1 O 2 ) contributed to ATZ degradation and accordingly inhibit the formation of toxic BrO 3 − from Br − . Sixteen intermediates were identified in proposed degradation pathways. The toxicity tests, the consistent performance with coexisting anions and humic acid in water matrix, and the satisfying reusability implied the sustainable application of Mn-1/PMS in future.
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
RADIATION PHYSICS AND CHEMISTRY
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2023
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IF 2.9
Shizong Wang,Jianlong Wang
This study firstly reported the in-situ preparation of nitrogen-doped graphene oxide-supported nano Fe 3 O 4 (Fe 3 O 4 @NRGO) by ionizing radiation . The conversion of Fe(II) to iron oxide was modulated by absorbed dose in solution, which regulated the catalytic activity of Fe 3 O 4 /NRGO. When the initial concentration of Fe(II) was 0.5 mM and the absorbed dose was 10 kGy, the as-prepared catalyst (Fe 3 O 4 @NRGO-10) showed superior catalytic activity for activating peroxymonosulfate (PMS) to degrade phenol. In the presence of 0.4 mM PMS and 0.5 g/L Fe 3 O 4 @NRGO-10, the pseudo first-order kinetic rate of phenol degradation reached 0.0286 min −1 . Sulfate radicals, hydroxyl radicals and high-valent iron oxo made major contribution to phenol degradation. The superior catalytic activity of Fe 3 O 4 @NRGO-10 might be attributed to the synergistic effect of NRGO and Fe 3 O 4 , in which NRGO promoted the conversion of Fe(III) to Fe(II). Fe 3 O 4 @NRGO-10 exhibited good stability in the cycling experiments. In addition to phenol, the Fe 3 O 4 @NRGO-10/PMS system could degrade sulfamethoxazole, bisphenol A and atrazine, indicating the wide applicability. This study reported a facile way to prepare carbon-supported metal oxide catalysts and convenient way to modulate the catalytic activity by absorbed dose.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 12
·5040-5051
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IF 9.931
Qingping Wang,Chris R. Bowen,Wen Lei,Haibo Zhang,Bing Xie,Shiyong Qiu,Ming-Yu Li,Shenglin Jiang
The harvesting of waste heat is attracting increasing attention, due to its abundance and potential benefits to the environment. However, the need for high heat transfer rates in thermal harvesting systems is a longstanding obstacle for their practical application. In this work, we construct thermally conductive networks in Pb[(MnxNb1−x)1/2(MnxSb1−x)1/2]y(Zr95Ti5)1−yO3 (lead magnesium niobate–lead antimony–manganese–lead zirconate titanate: PMN–PMS–PZT) ceramics to improve heat transfer and enhance their ferroelectric properties by use of a thermally conductive AlN additive dispersed in the ceramic matrix. The ferroelectric properties, pyroelectric coefficient and thermal conductivity of the PMN–PMS–PZT: AlN composite materials are influenced by the AlN content as a result of the formation of random bridges or thermally conductive networks for phonon transfer in the ceramic matrix, thereby leading to high heat transfer. For a PMN–PMS–PZT composite with a 0.2 wt% AlN content, the ferroelectric properties, pyroelectric coefficient and thermal conductivity are shown to be enhanced owing to the improved crystallinity and density, and the relative permittivity is also reduced, which results in optimized pyroelectric figure of merits. This combination of materials property enhancements is shown to be beneficial for high performance pyroelectric materials in devices for energy harvesting applications.
研究领域:
材料科学
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能源工程
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Ze Yang,Songding Guo,Zhenglai Huan,Yongbing Zhu,Tingting Zhang,Shangyi Li
In this study, we dexterously constructed a unique in situ interface oxidation–adsorption dual-reaction platform through the self-excitation of ferrate (Fe(VI))/peroxymonosulfate (PMS) for phenylarsonic acid (PAA) and inorganic As(V) removal. When the molar ratio of Fe(VI)/PMS was 1:2, 80% degradation of PAA could be achieved within 180 min and the apparent constant value of the reaction rate ( k obs ) would reach up to 0.185 min −1 . 1 O 2 and Fe(IV) were the main active species for degradation of PAA in Fe(VI)/PMS reaction system. In addition, we explored the possible degradation intermediates and pathway of PAA. In situ Fe(III) oxides generated from Fe(VI) decomposition could adsorb arsenic pollutants through ligand exchange with inorganic As(V) through surface hydroxyl groups to form Fe-O-As bonds. The effect of coexisting anions on the removal performance of the system was investigated, and the results showed that the presence of PO 4 3− and CO 3 2− promoted the oxidative degradation of PAA owing to the activation of PMS by PO 4 3− and CO 3 2− , but Cl − can inhibit the PAA degradation through a free radical scavenging mechanism. PO 4 3− and SiO 3 2− affected the adsorption and removal of the released inorganic As(V) due to their competitive adsorption of in situ Fe(III) oxides. Density functional theory (DFT) calculations indicated an obvious electron transfer (1.83 e) between the in situ Fe(III) oxides and inorganic As(V) with a high adsorption energy of −10.30 eV. These results indicate that the combination of Fe(VI) and PMS can effectively control the total arsenic (total-As) in water bodies.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Jialin Jia,Stefanos Giannakis,Dong Li,Boyin Yan,Tao Lin
A novel catalytic system for effective photocatalytic inactivation of Escherichia coli ( E. coli ) was constructed by anchoring Ag nanoparticles (AgNPs) on silane coupling agent (SCA) pretreated TiO 2 nano-tube arrays (Ag/SCA/TiO 2 NTAs). Morphology and structural analyses revealed that SCA could disperse AgNPs evenly on TiO 2 NTAs, thus inducing a superior surface plasmon resonance (SPR) effect. Ag/SCA/TiO 2 NTAs catalyst exhibited excellent inactivation performance when in the presence of peroxymonosulfate (PMS) and visible light (VL), with 6-log E. coli was completely inactivated within 60 min, which was 5.3, 12.5 and 13.2 times higher than that of Ag/SCA/TiO 2 NTAs/VL, PMS/VL and Ag/SCA/TiO 2 NTAs/PMS/dark systems, respectively. Additionally, the photocatalyst exhibited a highly reusable property, with the inactivation performance almost unchanged after ten cycles of uses with minimal Ag leaching. The inactivation mechanism analysis demonstrated that both radical (SO 4 •- , OH) and non-radical (h + , 1 O 2 ) pathways involved in E. coli inactivation, and SCA played a pivotal role in the production of reactive species. Chloride ions (Cl − ) greatly enhanced the inactivation efficiency, while bicarbonate (HCO 3 − ) and phosphate (H 2 PO 4 − ) showed an inhibitory effect. Humic acid (HA) displayed a dual effect on inactivation performance, where the low concentration of HA facilitated the bacteria inactivation, while the higher dose suppressed bacteria inactivation. Moreover, the system exhibited excellent inactivation performance in tap water . This work first used SCA as the binder to fix AgNPs on TiO 2 NTAs for VL photocatalytic inactivation of bacteria with the assistance of PMS, which was expected to provide some insights into the practical treatment of drinking water .
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PubMed
高影响因子
CHEMOSPHERE
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2023
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IF 8.8
Chunsheng Ding,Xinze Song,Zhongyi Zheng,Hainan Wang,Yuqiang Pan,Hangtian Zhang,Xueyan Li,Jing Deng
Fe(II)-catalyzed PMS process was widely used in the degradation of refractory pollutants in wastewater, while its performance was restricted by the slow regeneration efficiency of Fe(II). Herein, caffeic acid (CFA), a representative of hydroxycinnamic acids, was introduced into Fe(III)/PMS system to accelerate the transformation of Fe(III) to Fe(II) and promote the removal of bisphenol A (BPA). Under optimum condition of 0.1 mM CFA, 0.05 mM Fe(III), and 0.5 mM PMS, almost complete removal of BPA can be achieved within 20 min, which was roughly 6.2 times higher than that in Fe(III)/PMS system. As the addition of CFA into Fe(III)/PMS system, pH application range was widened from acidic to alkaline conditions. The reduction and chelation of CFA expedited the Fe(III)/Fe(II) cycle by forming CFA-Fe chelate, thereby facilitating the PMS activation . Based on LC-MS analysis and DFT calculation, the intermediate products of CFA were found to play a decisive role in boosting the regeneration of Fe(II), and the toxicity of these intermediates towards organisms was evaluated by ECOSAR . The alcohol-scavenging and chemical probe tests certified that hydroxyl radical (•OH), sulfate radical (SO 4 •- ), and Fe(IV) coexisted in Fe(III)/CFA/PMS system, and the second-order reaction rate constants of •OH and SO 4 •- reacted with CFA were calculated to be 3.16✕10 9 and 2.30✕10 10 M −1 s −1 , respectively. Two major degradation pathways of BPA, •OH addition and SO 4 •- induced hydroxylation reaction, were proposed. This work presented a novel green phenolic compound that expedited the Fe(II)-catalyzed PMS activation process for the treatment of organic contaminants .
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高影响因子
Materials Chemistry Frontiers
·
2023
·Vol. 7
·期 19
·4535-4546
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IF 7
Qiaoqiao Ding,Mang Niu,Hong Su,Zhanyin Liu,Jianfei Gao,Yanhui Zhao,Chunlei Liu,Yuan Liu,Chunzhao Liu
Developing highly efficient catalysts to effectively activate peroxymonosulfate (PMS) is a key challenge for degrading polychlorinated phenols posing a long-term risk of toxicity to environmental water. Here, a novel surface hierarchically nanostructured Co3O4/hydrogen titanate (HTO) composite catalyst (Co3O4/HTO) was prepared using electrospinning technology followed by a low-temperature alkaline hydrothermal process. Such a structural design endows the Co-based composite catalysts with rich and efficient surface-active cobalt sites, and provides rich hydroxyl groups for the composite catalyst, both of which enhance the catalytic performance of the composite catalyst in PMS based reactions. As expected, the optimum Co3O4/HTO catalyst can efficiently catalyze PMS to produce large amounts of free radicals, enabling the degradation of 2,4-dichlorophenol (2,4-DCP) completely within a very short time period (nearly 10 min). Density functional theory calculation further demonstrated that the Co3O4/HTO catalyst helps to enrich the charge density of PMS for the easy breakdown of the O–OH bond to generate more free radicals than the single Co3O4 catalyst. By analyzing the free radicals and intermediate products generated in catalytic reactions, possible degradation mechanisms and pathways of 2,4-DCP were proposed. This work offers a new approach to design low-cost and highly active PMS activators for the purification of wastewater.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Mengke Tang,Liang Jiang,Cunmin Wang,Xinyu Li,Xinjian He,Yichen Li,Changhui Liu,Yanqing Wang,Jiefeng Gao,Huan Xu
Despite the great potential in fabrication of biodegradable and eco-friendly air filters by electrospinning poly(lactic acid) (PLA) membranes, the filtering performance is frequently dwarfed by inadequate physical sieving or electrostatic adsorption mechanisms to capture airborne particulate matters (PMs). Here, using the parallel spinning approach, the unique micro/nanoscale architecture was established by conjugation of neighboring PLA nanofibers, creating bimodal fibers in electrospun PLA membranes for the enhanced slip effect to significantly reduce the air resistance. Moreover, the bone-like nanocrystalline hydroxyapatite bioelectret (HABE) was exploited to enhance the dielectric and polarization properties of electrospun PLA, accompanied by the controlled generation of junctions induced by the microaggregation of HABE (10–30 wt %). The incorporated HABE was supposed to orderly align in the applied E-field and largely promote the charging capability and surface potential, gradually increasing to 7.2 kV from the lowest level of 2.5 kV for pure PLA. This was mainly attributed to HABE-induced orientation of PLA backbone chains and C═O dipoles, as well as the interfacial charges trapped at the interphases of HABE–PLA and crystalline region–amorphous PLA. Given the multiple capturing mechanisms, the micro/nanostructured PLA/HABE membranes were characterized by excellent and sustainable filtering performance, e.g., the filtration efficiency of PM0.3 was promoted from 59.38% for pure PLA to 94.38% after addition of 30 wt % HABE at a moderate airflow capacity of 32 L/min and from 30.78 to 83.75% at the highest level of 85 L/min. It is of interest that the pressure drop was significantly decreased, mainly arising from the slip effect between the ultrafine nanofibers and conjugated microfibers. The proposed combination of the nanostructured electret and the multistructuring strategy offers the function integration of efficient filtration and low resistance that are highly useful to pursue fully biodegradable filters.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Youpu Zhao,Qing Sun,Jian Zhang,Jiawei Sheng
In this study, natural porous diatomite was utilized as a conciliatory carrier for the fabrication of Fe/N/C nano-clusters with assistance of binary molten salt of NaCl-ZnCl 2 under different annealing temperature and used to removal of norfloxacin (NFA). The sample Fe/D m900 (prepared at 900 °C) exhibited a high surface area and great catalytic performance for antibiotics in the presence of PMS. Over 97% NFA can be decomposed within 5 min and the final degradation rate reached 98%. Meaningfully, high-efficiency Fe/D m900 -PMS system was nearly impervious to pH values and inorganic cations in aqueous solution and could be a likely candidate for degradation of multiple contaminants in pharmaceutical outlet water. Furthermore, the other impacting variables such as catalyst dosage, PMS dosage, NFA concentration and initial pH were moreover explored towards debasement, and conceivable degradation pathways of NFA were presented through LC-MS. This work builds up a compelling procedure to synthesize super-dispersed Fe clusters, which may be amplified to other transition metal-based catalyst via molten salt.
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JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Zhenyu Shen,Zhexin Zhu,Gangqiang Wang,Zhendong Wang,Wenxing Chen,Wangyang Lu
It is of great significance for improving the electron transmission performance of graphite phase carbon nitride (g-C 3 N 4 ) by an economical method. Herein, urea was mixed with tourmaline (TM) and calcined to obtain g-C 3 N 4 /TM composite photocatalyst . Under solar light, g-C 3 N 4 /TM activated peroxymonosulfate (PMS) to degrade carbamazepine (CBZ) entirely within 25 min. g-C 3 N 4 /TM had a superior photocatalytic oxidation performance under solar light than g-C 3 N 4 . Photogenerated electron-hole pairs of g-C 3 N 4 were efficaciously suppressed, originating from the more excellent electronic transfer to TM. Four active species, including SO 4 • - , •OH, 1 O 2 , and O 2 • - , were identified for the degradation of CBZ. Ten intermediates of CBZ and six intermediates of sulfaquinoxaline sodium (SQXNa) were determined by using ultra-performance liquid chromatography coupled with a high definition mass spectrometer (UPLC-HDMS), and a degradation pathway was proposed. As the reaction progressed, all aromatic nuclear intermediates were mineralized. The degradation of other organic pollutants by the g-C 3 N 4 /TM/PMS system validated the universal adaptability in practical applications. This research provided an effective way to improve the g-C 3 N 4 photocatalytic activity in wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Shizong Wang,Jianlong Wang
High efficient activator is highly desired in the field of persulfate-based advanced oxidation process. In comparison with the previous studies, this study adopted nitrogen, sulfur and oxygen co-doped carbon material to support Fe 0 encapsulate in Fe 3 O 4 to prepare iron-based modified carbon composite (Fe 0 @Fe 3 O 4 -MC) by a facile two-step pyrolysis. Fe 0 @Fe 3 O 4 -MC was then used for degradation of sulfamethoxazole. The results showed that Fe 0 @Fe 3 O 4 -MC had superior catalytic activity for PMS activation due to the synergistic effect of iron-based compound and modified carbon. In the presence of 0.1 g/L of Fe 0 @Fe 3 O 4 -MC, SMX (0.04 mM) could be completely degraded within 120 min at pH 3.4 and 3 mM of PMS. The SMX degradation followed pseudo first-order kinetic model, with the rate constant of 0.12 min −1 , and the mineralization of SMX achieved 48.4%. Sulfate radicals dominated in the SMX degradation. In addition to Fe 0 and Fe 3 O 4 , carbon defects, graphitic N, sulfur and FeN 4 also contributed to PMS activation. Fe 0 oxidation was the rate-limiting step for PMS activation. Dissolved oxygen made a minor contribution to Fe 0 oxidation. The intermediate products of SMX degradation were identified, and two pathways of SMX degradation were proposed. The influencing factors on SMX degradation were studied, including pH, temperature, PMS concentration, Fe 0 @Fe 3 O 4 -MC dosage, chloridion, carbonate and humic acids, and the influencing mechanism was discussed. This study could provide an efficient PMS activator for the degradation of emerging organic pollutants in water and wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Jawad Ali,Ajmal Shahzad,Jia Wang,Jerosha Ifthikar,Wenli Lei,Gebremedhin G. Aregay,Zhulei Chen,Zhuqi Chen
The slow transformation of Fe 3+ back to Fe 2+ restrict the practical application of Fe-based catalytic treatment of organic pollutants . Herein, we report a new findings of MgAl-MoS 4 to accelerate the redox cycle of Fe 3+ /Fe 2+ in Fe 3+ /PMS system. Based on the degradation of 4-chlorophenol (4-CP) profile, the rate constant of Fe 3+ /MgAl-MoS 4 /PMS system was 40 to 42 folds higher than MgAl-CO 3 /PMS, MgAl-MoS 4 /PMS and Fe 3+ /PMS respectively. Moreover, Fe 3+ /MgAl-MoS 4 /PMS system was superior both in the degradation efficiency of pollutants as well as in the stoichiometric efficiency of oxidants from the recently reported Fe 3+ /WS 2 /PMS, Fe 3+ /MoS 2 /PMS or other well-known nano-catalysts systems. This co-catalytic effect of MgAl-MoS 4 on the studied redox metals falls in the order of Fe 3+ > V 5+ > Cu 2+ > Mn 2+ ~Ag + . Furthermore, the Fe 3+ /PMS/MgAl-MoS 4 system shows smooth degradation over a wide pH (3.0–7.0) and complete stabilities in the recycled studies. Additionally, the presence of excessive amounts of inorganic anions or organic matters also did not influence the degradation profile. In mechanism studies, both the unsaturated S 2− and Mo 4+ of MgAl-MoS 4 were disclosed to fuel electron continuously during the reduction of Fe 3+ ions, and thus accelerate the rate limiting step (Fe 3+ /Fe 2+ ). Additionally, the layered structure, memory effect and suitable surface charge of LDH material also concentrates the reactants molecules and hence, the boosted effect of MgAl-MoS 4 was associated with the better adsorption of Fe 3+ ions, the faster PMS decomposition, and the acceleration of Fe 3+ /Fe 2+ redox cycle. This work indicates a breakthrough in the field of classical homogenous Fe/PMS system, offers the very first report on the role of Mo 6+ and S 2− to modulate the redox behaviour of homogenous Fe ions in persulfate based advanced oxidation processes .
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