SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jinjuan Xue,Jin Li,Jiamin Gao,Mingxin Wang,Shuaishuai Ma
Effective synchronous removal of water-immiscible oils and water-miscible refractory aromatic pollutants from wastewater is of great significance for water remediation. In this work, a low-cost and easy-prepared composite membrane was fabricated by vacuum assisted assembling of CoFe 2 O 4 and tannic acid on polyvinylidene fluoride (PVDF) substrate. The CoFe 2 O 4 functionalized PVDF membrane (CoFe 2 O 4 @PVDF) exhibited in-air superamphiphilic and underwater superoleophobic surface wettability. The resultant membrane displayed relatively favorable permeation flux (811.5 to 1837.5 Lm −2 h −1 ) and high separation efficiency (above 99 %) in the separation of a series of emulsified oils ranged from nanoscale to microscale from water. Meanwhile, the as-fabricated CoFe 2 O 4 @PVDF membrane coupled with peroxymonosulfate (PMS) exhibited an extensive oxidizing capacity and high degradation efficiency towards aromatic contaminants with desired mineralization ability. More importantly, considering that the fabricated CoFe 2 O 4 @PVDF membrane possessed special super-wettability as well as PMS activation-based catalytic ability, it also applied in the treatment of simulated complex wastewater. The process achieved effectively synchronous oil/water separation and PMS activation toward pollutants degradation. Besides, in five cyclic continuous “degradation-separation” tests, the recovered CoFe 2 O 4 @PVDF membrane after PMS-based degradation in each cycle could separate oil/water emulsions as usual. It exhibited almost complete oil rejection and flux recovery property under multicycle filtration, demonstrating its excellent durability and stability. This flexible integration of PMS-based AOP catalytic capability and super-wettability into a composite membrane can provide inspiration for effective complicated wastewater rehabilitation.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2022
·Vol. 33
·期 29
·22773-22784
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IF 2.779
Chen Xin,Ouyang Yuting,Liu Xiukun,Ruan Hong,Xu Xu,Lu Shaorong,Li Yuqi
Providing a green and sustainable cathodic protection method for metal surfaces is the key to increasing the service life of equipment. Herein, furan-modified CaCu 3 Ti 4 O 12 (F-CCTO) and polyurethane with maleimide group as side group (MPU) were synthesized to prepare the high-performance dynamic covalent-crosslinked F-CCTO/MPU (FP) composites. And then the FP composites were further used to construct a triboelectric nanogenerator (FP-TENG) for Q235 steel cathodic protection. The results show that at 1-wt% F-CCTO content, the tensile strength and T 10% of the FP composite increased by 83.3% and 30 °C, respectively, compared with those of pure MPU. In addition, short-circuit current ( I sc ), open-circuit voltage ( V oc ), and peak power density of the FP-TENG were 4.6 μA, 100 V, and 3.3 Wm −2 , respectively. Notably, the mechanical and electrical output properties of the reprocessed FP composites obtained using the inverse Diels–Alder (DA) reaction are almost unchanged compared to the original FP composites. Electrochemical experimental results confirmed that the Q235 steel connected to the FP-TENG cathodic protection system exhibits excellent corrosion resistance. The corrosion potential of Q235 steel was reduced by about 110 mV, and in addition, the corrosion prevention mechanism of self-powered cathodic protection of metal surfaces was discussed.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Suzhou Xu,Can Liu,Xuping Jiang,Xinyu Wang,Shijin Zhang,Yanting Zhang,Qingguo Wang,Weiling Xiong,Jing Zhang
The performance and mechanisms of a titanium carbide (Ti 3 C 2 ) MXene modified Fe 3+ /hydrogen peroxide (H 2 O 2 ) system were compared in detail under dark and visible light conditions, with a new mechanism proposed for the reaction and reduction of MXene by Fe 3+ . Using Bisphenol A (BPA) as the target pollutant, the degradation of BPA by the Fe 3+ /H 2 O 2 system was improved after adding MXene in the dark, and the degradation rate of BPA was ≥ 95 % within 12.5 min under visible light, six times higher than that in the dark. Fe 2+ was ascertained to be the effective component responsible for H 2 O 2 activation to produce ·OH. SEM , XPS, ICP, XRD, and FTIR spectroscopy , analyses show that MXene and Fe 3+ form a complex, and then MXene reacts with Fe 3+ by breaking the Ti–C bonding to accelerate the Fe 3+ /Fe 2+ cycle. MXene uses photogenerated electrons to promote this reaction under visible light. In addition, quenching experiments and electron spin resonance spectroscopy results show that ·OH and O 2 •− are the main reactive oxygen species under visible light, while ·OH is the main active species in the dark. MXene thus effectively uses O 2 to form O 2 •− under visible light and promotes the Fe 3+ /Fe 2+ cycle. This study provides a theoretical basis for the combination of visible light catalysis and the advanced oxidation process of a Ti 3 C 2 MXene.
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PubMed
高影响因子
Water
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2022
·Vol. 14
·期 21
·3450
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IF 3.53
Wei Zhou,Yu Li,Min Zhang,Guang-Guo Ying,Yong Feng
In this study, chalcopyrite (CuFeS2), a natural mineral with a bimetallic structure, was used as the activator to generate radicals for removing organic pollutants from aqueous solutions via the activation of peroxymonosulfate (PMS). Sulfisoxazole (SIX), a sulfonamide antibiotic, was selected as the model pollutant. The results showed that chalcopyrite was highly reactive toward the activation of PMS; under the conditions of 50 µM PMS and 1 g/L chalcopyrite, approximately 95.7% of the SIX was degraded after reaction for only 5 min. An increase in the loading of chalcopyrite (0.25–2 g/L) promoted the degradation of SIX, while elevated levels of PMS (0.05–0.5 mM) slightly retarded the degradation kinetics. Although the best performance was observed under acidic conditions (pHs 3 and 4), near complete degradation of SIX was also achieved at pH 5.5. Identification of reactive species revealed that both a hydroxyl radical and a sulfate radical were formed in chalcopyrite–PMS oxidation, and they were responsible for the degradation of SIX. Trace amounts of copper and iron were leached out from chalcopyrite during the activation, and both the heterogeneous and homogeneous activation of PMS contributed to the generation of oxidizing radicals. Common water constituents including Cl−,HCO3−, and natural organic matter at their environmentally relevant levels showed a limited effect on the degradation of SIX, which suggests that chalcopyrite–PMS oxidation has high reactivity and stability in the degradation of organic pollutants and shows great practical application potential.Keywords:peroxymonosulfate;CuFeS2;sulfate radicals;sulfide mineral;water matrices
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Mengke Li,Zhiguo He,Hui Zhong,Wei Sun,Mingqiang Ye,Yihui Zhou
In this study, a novel carbon-wrapped-iron hierarchical porous catalyst (Fe/C-Mn 800 ) was prepared from electrolytic manganese residue (EMR) and sewage sludge (SS), which showed outstanding degradation ability toward benzohydroxamic acid (BHA, nearly 90 % was removed within 60 min) with low metal leaching rate. Mechanism exploration found transition metal ions (Fe and Mn) can serve as electron acceptors and facilitate the generation of persistent free radicals (PFRs). These transition metal ions and PFRs mainly participated in the single-electron pathway via activating PMS to generate a large amount of reactive oxygen species (ROS). While the electron negative graphitic N and C O groups not only improve the electronegatively of catalyst, but also acted as the electron sacrificers to favor the electron transfer and directly oxidized the absorbed BHA through the ternary activated outer-sphere complexes. Eley–Rideal (E-R) and Langmuir–Hinshelwood (L-H) analysis further demonstrated the crucial role of pre-adsorption during the degradation process. This work provided a deep insight into the degradation mechanism of metal/carbon composite and promising opportunity widened the horizon of the high-value utilization of EMR and SS.
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高影响因子
Catalysts
·
2022
·Vol. 12
·期 11
·1327
·
IF 4.501
Yifei Qi,Xiaoyue Zhou,Zhenjie Li,Renli Yin,Junhao Qin,Huashou Li,Wanqian Guo,Adela Jing Li,Rongliang Qiu
Peroxymonosulfate (PMS) has been intensively used to enhance the photocatalytic activity of catalysts, which is adopted as an electron acceptor to inhibit the recombination of electrons and holes. However, the effect of holes generated by visible light (VL) on PMS activation is always overlooked. Herein, the VL/Bi2WO6/PMS process was constructed for the efficient removal of organics, in which the degradation rate of carbamazepine (CBZ) increased by over 33.0 times by the introduction of PMS into Bi2WO6under visible light. The radical quenching and determination experiments confirmed that the photogenerated holes could firstly oxidize PMS to form SO5•−and react with HSO5−to produce1O2, then inducing the formation of other reactive species to greatly enhance the performance of pollutant removal by the VL/Bi2WO6/PMS process. Density functional theory (DFT) predicted that sites with high Fukui index (f0) on CBZ were more susceptible to being attacked, resulting in hydroxylation, ring closure, and C=C bond cleavage of CBZ. Toxicity estimation indicated that photocatalysis degradation products from CBZ were less toxic compared to the parent compound. This study provides a potential avenue for improving photocatalytic efficiency and widening the application of photocatalytic technology in wastewater purification.Keywords:Bi2WO6;carbamazepine;peroxymonosulfate;photocatalysis;singlet oxygen
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yin Li,Jiahui Hu,Yubin Zou,Lin Lin,Hebin Liang,Huaxin Lei,Bing Li,Xiao-yan Li
High-valent iron–oxo species (Fe V =O) generated through peroxide activation by Fe-based catalysts can realize the selective and efficient degradation of organic pollutants in water treatment. However, the rapid and efficient generation of Fe V =O for the selective degradation of pollutants over a wide pH range with high stability is challenging. In this study, a N, P, and S co-doped Fe-single atom (SA) catalyst (Fe SA -NPS@C) with FeN 4 active center was synthesized as a highly efficient catalyst for the peroxymonosulfate (PMS)-based oxidation. The Fe SA -NPS@C catalyst exhibited an excellent catalytic performance at low dosages of both the catalyst and PMS for the degradation of pollutants over a wide pH range with high stability. For the degradation of ofloxacin (OFX), the rate constant pertaining to PMS with Fe SA -NPS@C was 1.68 min −1 , considerably higher than those obtained using the N -doped and N and P co-doped Fe-SA catalysts. The degradation pathway of OFX revealed that the electrostatic effect was of significance in its degradation by Fe V N 4 =O with Fe V N 4 =O being the dominant reactive species. Density functional theory calculations revealed that the heteroatom doping effectively altered the electronic structure of the FeN 4 site of Fe SA -NPS@C, which strengthen its coordination with PMS, promote the electron transfer to PMS, and facilitate the interaction between Fe V N 4 = O and OFX, and thus significantly enhanced its catalytic activity. These findings provide new insights into the oxidation mechanism of Fe V =O in heterogeneous systems and the catalytic ability enhancement through heteroatom doping.
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Frontiers in Environmental Science
·
2022
·
IF 5.411
Wang Qinghong,Ji Yuanyuan,Hu Jingze,Ye Huangfan,Liu Ya,Wang Yuxian,Chen Chunmao,Li Zhuoyu
Cerium oxides loaded silica catalysts were synthesized by an impregnation method by simply mixing Ce precursor with silica spherule (Ce/SS) and ordered MCM-41 zeolites (Ce/MCM-41), followed by a mild calcination. Compared with pure SS and MCM-41, Ce modified Ce/SS and Ce/MCM-41 demonstrate much improved catalytic ozonation activities for mineralization of recalcitrant nitrobenzene (NB). At solution pH of 6, 86 and 97% TOC mineralization rates were achieved within 60 min for Ce/MCM-41 and Ce/SS, respectively. Characterization results suggest that Ce loading significantly increases the surface Lewis acidic sites, which would synergize with Ce3+/Ce4+ redox cycle for the activity improvement. With the aid of in situ electron paramagnetic resonance (EPR) spectra and quenching tests, hydroxyl radical (·OH), superoxide radical (O2•–), and singlet oxygen (1O2) are identified as the O3 catalytic decomposition products, while ·OH mainly accounts for NB mineralization. The detailed degradation route of NB was further investigated by the multi-chromatography analysis. NB is firstly oxidized into polyhydroxy compounds, followed by small molecular organic acids, and finally being mineralized into CO2 and H2O. This study established a facile strategy to synthesize highly active and stable Ce/SiO2 catalysts for catalytic ozonation, and elucidated the in-depth mechanisms for the activity origins of the Ce loaded silica-based materials in catalytic ozonation processes (COP).
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Lidong Wang,Xiuze Li,Hanxia Chen,Yifei Liang,Zhongfei Xu,Juzhe Liu,Wen Liu,Juanjuan Qi
Sulfite(S(IV))-induced advanced oxidation processes (AOPs) have great prospect in the field of removing organic pollutants , yet developing highly efficient sulfite activation systems and optimizing active sites for favorable catalytic processes are important but still challenging. Herein, we have achieved a composite catalyst with modulated Co electron structure for efficient AOPs by decorating Co(OH) 2 on ultrathin graphitic carbon nitride (g-C 3 N 4 ) nanosheet through an adjustable strategy, which exhibits high catalytic performance in S(IV) activation system. At optimal pH 9, 92% of paracetamol (APAP) (0.005 mM) is removed with the degradation rate constant of k 1 = 0.193 min −1 within 30 min in presence of the composite material. The in-situ synthesis mode introduces strong heterogeneous interface interaction, resulting in directional electron transfer from cobalt hydroxide layer to g-C 3 N 4 sheet revealed by X-ray photoelectron spectroscopy and density functional theory (DFT) calculations. The underlying activity enhanced mechanisms for APAP in S(IV) activation system using Co(OH) 2 /g-C 3 N 4 are proposed: (i) The ultrathin g-C 3 N 4 nanosheets provide more anchoring centers for generating small Co(OH) 2 nanoparticles with abundant active sites which benefit to form metastable intermediates of Co(II)-SO 3 ; (ii) The strong interface interaction induces charge redistribution between Co(OH) 2 and g-C 3 N 4 conformed by DFT calculation, which modulates the d-band center of Co site and strengthens the bind of Co(II)-SO 3 , thereby giving rise to radicals ( • OH, SO 4 • and O 2 • ) and nonradicals ( 1 O 2 and electron transfer) oxidation for highly-efficient removal APAP. Our work will pave the way to build an environmentally friendly strategy for emerging organic pollutant degradation in water through building efficient catalysts in sulfite activation system.
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CHEMOSPHERE
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2022
·
IF 8.943
Jiaojiao Yang,Binyu Guo,Lei Li,Quanyuan Chen,Chensi Shen,Juan Zhou
The limited regeneration of Fe 2+ in the Fe-catalyzed advanced oxidation processes (AOPs) constrained its application for the removal of organic pollutants. Herein, MoSe 2 was introduced to promote the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) in the Fe 2+ /PMS system. Compared with Fe 2+ /PMS processes, the 2,4-D degradation efficiency and PMS decomposition rate respectively increased by 73.8% and 84.2% in the MoSe 2 /Fe 2+ /PMS system. DFT simulation results suggested that Se atoms acted smoothly as the bridge supporting the charge transfer from Mo to adjacent Fe atoms, which led to the reduction of Fe 3+ . The rapid regeneration of Fe 2+ boosted the activation of PMS and the degradation of pollutants. Additionally, the electron paramagnetic resonance (EPR) and quenching experiments results indicated that SO 4 ∙ − , ∙OH, and 1 O 2 accounted for 2,4-D degradation, and SO 4 ∙ − and 1 O 2 predominated the reaction. The Mo based co-catalysts showed better co-catalytic effect than the W counterparts, and the moderate adsorption for PMS and lower electron transfer electron transfer resistance accounted for the more excellent co-catalytic performance of MoSe 2 than that of WSe 2 . In addition, the degradation efficiency of 2,4-D was up to 95.5% after five cycles of MoSe 2 in the co-catalytic system. The coexistent humic acid (HA) and Cl − showed ignorant negative effect on the degradation, while HCO 3 − would depress the oxidation reaction. The acidic etching wastewater can be applied as the Fe ions source in this co-catalytic process to remove 2,4-D effectively.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Chaojie Lyu,Jiarun Cheng,Kaili Wu,Jiwen Wu,Ju Hao,Yuanyuan Chen,Huichao Wang,Yunguo Yang,Ning Wang,Woon-Ming Lau,Jinlong Zheng
Transition metal-based electrocatalysts are the promising candidates to substitute noble metal-based catalysts for water electrolysis, owing to its abundant earth reserves and inexpensive fabrication costs. Interface engineering and cation doping engineering are verified as the effective methods to improve the sluggish electrocatalytic performance of transition metal-based electrocatalysts. Here, we synthesized a self-supported heterostructure of Ce doped Co(OH) 2 nanosheets/CoP nanowires on the support of nickel foam (Ce-Co(OH) 2 /CoP/NF) by simple hydrothermal method , low-temperature phosphorization method. The Ce atom doping can lead to lattice distortion and abundant superficial defects on crystal surface, which will generate more active sites and faster charges transformation. The heterointerface between Ce-Co(OH) 2 and CoP also can lead to electronic structure modulation at interface domain, which not can induce much fresh active sites in this area, but can optimize the active sites to the optimal state for superior catalytic activity. Benefitting from these, it only needs the overpotentials of 253 and 56 mV to realize 10 mA/cm 2 for OER and HER under 1 M KOH solution, which is much enhance than single-phased samples. As the bifunctional electrocatalyst for two-electrode system, it merely requires 1.53 V to attain 10 mA/cm 2 in 1 M KOH, and it also exhibits outstanding overall water splitting performance in alkaline natural electrolyte, along with excellent catalytic long-time durability. In addition, the Ce-Co(OH) 2 /CoP/NF-based electrolyzer also could achieve energy-saving hydrogen production, and simultaneously oxidative degradation of organic materials or biomass upgrading at anode under lower voltages. This work paves a novel idea to fabricate high-efficient bifunctional electrocatalysts for energy-saving H 2 production.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yang Peng,Zhanwei Xu,Le Yu,Xucheng Li,Weiran Yang
The direct conversion of furfural (FUR) to 2-methyltetrahydrofuran (2-MTHF) was investigated over a trimetallic CuNiRe/Hβ catalyst. Under optimal reaction conditions at 240 °C under 3 MPa H 2 for 1 h, almost complete conversion of FUR and high-yield of 2-MTHF (81 %) was achieved. This is the highest yield reported for the direct conversion of FUR to 2-MTHF. HR-TEM demonstrated that the growth of Cu nanoparticles (NPs) on the surface of Hβ was inhibited after loading Ni or Re resulted in the smaller Cu particle size and better hydrogenation and hydrodeoxygenation activity. H 2 -TPR characterization exhibited that the reducibility of bimetallic and trimetallic catalysts was higher than that of monometallic catalysts·NH 3 -TPD explained that Hβ acid sites mainly contributed to FUR deoxygenation. The adsorption configurations of FUR, furfuryl alcohol (FOL) and 2-methylfuran (2-MF) on the catalyst were revealed by ATR-IR. Catalyst evaluation and control experiments proved that FUR was first hydrogenated to FOL, followed by hydrodeoxygenation to 2-MF, and finally hydrogenated to 2-MTHF catalyzed by the combination of three metals.
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