SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chen Wang,Zewei Hu,Wei Lou,Mingjie Huang,Wei Xiang,Tao Zhou,Juan Mao,Xiaohui Wu
This study has demonstrated that the Fenton fluidized bed (FFB) technology could successfully immobilize As ions on the iron-crystallized (IC) carriers, with simultaneous crystallization of ferric and mineralization of organic pollutants. It was found that rapid fluidized immobilization of aqueous As(V) on the IC carriers was through surface favorable bidentate complexion, while the adsorptive removal of As(III) was rather slow. Adding Fe 3+ caused competitive complexion and inhibited the As(V) immobilization. However, effective oxidative crystallization of Fe(II) and As(III) in FFB would take place. With the simultaneous generation of As(V) and Fe(III) by rapid •OH oxidation, two different crystalline precursors would be formed on the IC carriers, leading to efficient co-crystallization of As(V)/Fe(III). Recursive Fe(III) crystallization in the FFB continuously provided essential surface hydroxyl groups for capturing As(V), inducing layer-by-layer co-crystallized immobilization As(V)/Fe(III). The long-term continuous-flow treatment of a practical As(III)-containing industrial organic wastewater exhibited effective/stable co-crystallizations of As(V)/Fe(III), as well as COD removal. The FFB technology is expected to be a good option in treating complex industrial wastewater containing heavy metal and recalcitrant organic pollutants.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Xiaoqiu Lin,Linshan Zheng,Min Zhang,Yue Qin,Xiaolu Liu,Yuanfeng Liu,Huiyu Li,Congju Li
Nanomaterials are ideal for electrode modification to improve the power output of microbial fuel cells (MFCs). The nanomaterials decoration usually needs a conductive binder which faces the problem of high cost and low conductivity, significantly constraining further application. This study successfully fabricated the binder-free Fe nano oxides modified anodes through the solvothermal method. MFC assembled with carbon cloth/Fe nano oxides (M−CC/Fe) achieved the highest maximum power density (471.6 mW m −2 ), dramatically higher than that with carbon cloth (M−CC, 150.4 mW m −2 ), Ni foam/Fe nano oxides (M−NF/Fe, 130.6 mW m −2 ) and Ni foam (M−NF, 16.5 mW m −2 ). The electrochemical catalyzing activity, extracellular electron transfer rate, COD removal efficiency and coulombic efficiency were all improved after Fe nano oxides decoration in MFCs. Fe nano oxides enriched exoelectrogens/iron-reducing bacteria like Geobacter and Comamonas and showed a mutual benefit relationship with them. The formation of stable Fe nano oxide cubes significantly enhanced the electroactive biofilm development and alleviated the corrosion of the electrode substrate. The complementary merits of the carbon-based electrode and Fe nano oxides performed better in stimulating power generation in MFCs. These results provided knowledge of in-situ nanomaterials decoration for advanced anodes, providing suggestions for high-performance resource recovery from wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
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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PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2022
·Vol. 43
·期 2
·491-511
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IF 3.337
Huang Shaoyong,Huang Quanjia,Gan Jiaming,Li Ting,Wang Lei
In this study, Fe-rich sludge was pretreated by dielectric barrier discharge (DBD) and used as a Fenton catalyst for the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) in aqueous solution, where hydrogen peroxide was in situ supplied from a glow discharge plasma (GDP) in contact with the solution. Synergistic mechanism of the two plasmas during 2,4-D degradation was explored. The Fe-rich sludge pretreated by H 2 -DBD could significantly accelerate the 2,4-D degradation as it converted Fe(III) in the sludge to the active Fe(II). 2,4-D can be completely removed in the presence of H 2 -DBD pretreated Fe-rich sludge with 25 min of GDP at pH 0 3.0 and catalyst dosage of 1.0 g/L. Quenching experimental studies showed that both ·OH (oxidative degradation) and ·H (reductive dechlorination) were responsible for 2,4-D degradation. Reducing radicals (such as ·R and·H) formed during GDP can continuously reduce the Fe 3+ back to Fe 2+ , which further promoted the degradation and dechlorination of 2,4-D. The results of three consecutive experiments indicated the stability and reusability of catalyst. This study provides a potential method for the recycle of Fe-rich sludge as a novel and cost-effective catalyst for 2,4-D removal from aqueous environments, which is significant for the terminal disposal of Fe-rich sludge. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jun Luo,Chengcheng Ding,Yonghai Gan,Yang Guo,Yibin Cui,Cheng Sun
A dual-MOFs (Fe and Co)/g-C 3 N 4 heterojunction composite was successful constructed and used to activate peroxymonosulfate (PMS) for degrading sertraline (SER). The composite showed outstanding catalytic activity with 100% of SER removal efficiency in 60 min and the degradation rate 0.057 min −1 . At the same time, the amount of catalyst, concentration of PMS and environmental pH on the degradation for SER were investigated in detail. The main degradation products and pathways of SER were analyzed by Gaussian theory calculation and high-performance liquid chromatography-mass spectrometry (HPLC-MS). Based on the free radical quenching experiments and electron paramagnetic resonance (EPR) characterization analysis, it was confirmed that •OH and SO 4 •- were produced in the catalytic reaction process, and explained catalytic mechanism elaborately. This work demonstrates the connection of MOF-Fe nanoparticles , micropores and heterojunction with the catalytic activity, providing an efficient catalytic system that can promote electron transfer and circulation of high activity center.
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Science China-Materials
·
2023
·Vol. 66
·期 5
·1779-1792
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IF 8.1
Yang Jia,Wang Mengxiao,Chen Tao,Yu Xiang,Qin Gang,Fang Xiaohan,Su Xiaoxiang,Chen Qiang
Supercapacitors exhibiting toughness, self-healing, and high specific capacitance have practical significance for use in flexible and wearable electronic equipment. To meet these requirements, a novel multifunctional gel polymer electrolyte (GPE) consisting of polyvinyl alcohol (PVA)-sodium alginate (SA)-K 3 [Fe(CN)] 6 -Na 2 SO 4 was prepared. In this GPE, K 3 [Fe(CN)] 6 plays three crucial roles by serving as a carrier donor, ionic crosslinking agent and redox-active mediator. Consequently, the usual conflict between the conductivity and mechanical properties of GPEs is alleviated to some extent. In addition, the electrode specific capacitance and the energy density of the assembled supercapacitor are obviously improved because of the pseudocapacitance generated from the redox reaction of K 3 [Fe(CN)] 6 . Based on this GPE, the supercapacitor exhibits outstanding bending and stretching stabilities, significant self-healing, and anti-freezing properties. Therefore, the prepared GPE and supercapacitor are promising for application in flexible and wearable electronic equipment with complex service conditions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xiaoyu He,Xutao Gao,Xiao Chen,Shen Hu,Fangchang Tan,Yujie Xiong,Ran Long,Min Liu,Edmund C.M. Tse,Fei Wei,Hong Yang,Jungang Hou,Chunshan Song,Xinwen Guo
Increasing CO 2 conversion efficiency over metal-organic framework (MOF) based photocatalysts is of great significance to promote the carbon capture and utilization. In this work, a dual-benefit design strategy is deployed in the synthesis of a new two-dimensional Fe/Ti-BPDC MOF photocatalyst with atomically dispersed Fe sites. This catalyst demonstrated an excellent catalytic performance in the visible-light-driven CO 2 conversion to HCOOH, achieving a high yield of 703.9 μmol g -1 h -1 at a selectivity greater than 99.7%. This is attributed to the ‘dual-optimization’ achieved by this catalyst to sustain the supply of photogenerated electrons and to effectively activate CO 2 . Specifically, the Fe/Ti-BPDC catalyst provides a high proportion of effective photogenerated electrons for the CO 2 photocatalysis process via a unique electron transfer mechanism. Meanwhile, the strong O/Fe affinity between CO 2 and atomically dispersed Fe active sites not only enables a fast CO 2 activation, but also dictates the intermediate reaction pathways towards high HCOOH selectivity.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Jian Sun,Shengbin Bai,KeKe Li,Yue Zhou,Yuning Chen,Lei Liu,Zijian Zhou
CaCO3/CaO materials possess the advantages of low cost, high energy storage density, and working temperature, which offer these materials the potential to be used in thermochemical energy storage systems for concentrated solar power plants. However, CaCO3/CaO materials possess poor antisintering and optical absorption abilities, largely limiting their practicability for direct solar utilization. In this study, binary ion doping of Fe/Mn and Zr-based stabilizer incorporation were simultaneously conducted to improve the cyclic thermal energy storage/release performance of CaCO3/CaO materials. The spectral absorbance of synthetic CaO-based composites (ranging from 77.8% to 84.0%) doped with binary ions of Fe/Mn is greatly increased in comparison to that of pure CaO (∼12.2%) due to the generation of black Ca2Fe2O5 and Ca4Mn3O10. The cyclic thermal energy storage/release performances of synthetic CaO-based composites were comparatively investigated under two thermal energy storage modes (CSP-N2 and CSP-CO2). The Zr-doped, CaO-based composites exhibit a cycling stability superior to those of Zr-free CaO-based composites due to the generated inert CaZrO3 with desirable antisintering ability, and the superiority is more prominent under CSP-CO2 mode. After 50 cycles, the CaO-based composite with a molar ratio of Ca:Zr = 100:6.7 exhibits a remarkably stable energy release density of 1.02 MJ/kg under CSP-CO2 mode, retaining 88.9% of its initial energy release density.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yaqi Zhang,Yaming Sun,Yong Man,Hang Yuan,Renyong Zhao,Guoqiang Xiang,Xiuming Jiang,Lijun He,Shusheng Zhang
The development of peroxymonosulfate (PMS) catalysts with sufficient active sites and high mass transfer capacity is a desirable but challenging aspect in advanced oxidation processes. In this work, an Fe/N-co-doped porous carbon (Fe/N-PC) material derived from silica-coated Fe-doped zeolitic imidazolate framework-8 (Fe-ZIF-8) was developed and used as catalyst for the degradation of aflatoxin B 1 (AFB 1 ). Fe-ZIF-8 introduced additional Fe-N sites with high catalytic PMS activity. Importantly, the strategy of silica coating on the surface of Fe-ZIF-8 effectively prevented the aggregation of catalyst particles during the pyrolysis process and introduced a hierarchical porous structure in Fe/N-PC, significantly improving the mass transfer of reactants on the catalyst. As a result, Fe/N-PC possessed a much higher adsorption capacity for AFB 1 (202.8 mg g −1 ) than other reported carbon adsorbents and exhibited fast degradation of AFB 1 with ultra-high removal efficiency (99.88%) within 30 min. Singlet oxygen ( 1 O 2 ) was proved to be the dominant reactive species for AFB 1 degradation. In addition, four degradation products were identified, and two possible degradation pathways were proposed. The double bond of the terminal furan ring or the methoxy group was destroyed, which implied that the toxicity of the degradation products was significantly reduced. Based on the above results, Fe/N-PC can be considered an efficient catalyst for the removal of hard-to-degrade AFB 1 in practical applications.
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 35
·18147-18155
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IF 14.511
Jin Li,Kaicai Fan,Hongliang Jiang,Fenghong Lu,Lixiu Cui,Bin Li,Qi Zhang,Gao-Chao Fan,Lingbo Zong,Lei Wang
Fe–N–C single atom electrocatalysts (SAECs) with porphyrin-like Fe–N4 species are one of the most promising alternatives to the platinum-group-metal-based electrocatalysts used for oxygen reduction reaction (ORR). However, limited attention is paid on delicately optimizing the free energy barrier of Fe–N4 active sites through heteroatom doping in the carbon skeleton. Herein, Fe single atoms (SAs) on heteroatoms N- and P-codoped porous honeycomb-like carbon (Fe–N4/NP-PHC) have been rationally designed. The as-developed Fe–N4/NP-PHC catalyst with abundant accessible active sites showed an impressive onset potential (Eonset = 1.0 V) and half-wave potential (E1/2 = 0.89 V) under low electrocatalyst loading capacity, which is more positive than those of Pt/C and most SAECs. Encouragingly, the experimental results and DFT calculations systematically demonstrated that the optimized adsorption energy of the Fe–N4 sites in the P-doped carbon matrix facilitated the release of OH* and thus boosted the ORR performance. The metal–air battery containing Fe–N4/NP-PHC exhibited high peak power density and long-term working feasibility with a low voltage gap at large current densities. This study demonstrates that P doping in carbon matrix is an effective strategy to promote catalytic properties and presents a novel avenue for developing high-performance electrocatalysts for various electrochemical reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Wen Wen Xie,Tong Zhen Tian,Min Yang,Nian Wu Li,Le Yu
Rational design of effective bifunctional inexpensive oxygen electrocatalyst is highly important for Zn-air batteries (ZABs), which can accelerate both oxygen reduction/evolution reactions at the oxygen electrode. Herein, we present the formation of hierarchical hollow frameworks of dual-sided Fe/Fe 3 C@N-doped carbon nanotubes (FNCHFs) through a template-engaged method. Benefitting from the synergistic effect between the robust hollow frameworks and in-situ grown dual-sided N-doped carbon nanotubes, the FNCHF electrocatalyst presents enhanced mass/electron transport with high structural stability. As a result, the FNCHFs based bifunctional oxygen electrode demonstrates a desirable oxygen electrocatalytic activity and stability with a half-wave potential of 0.863 V for oxygen reduction and an overpotential of 340 mV to reach the current density of 10 mA cm −2 for oxygen evolution. The corresponding ZAB exhibits a high peak power density of 206 mW cm −2 , a high specific capacity of 781 mAh g Zn −1 , and a good cycling stability more than 300 h.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Mengxue Yang,Ruixian Wu,Shengshuai Cao,Yanwei Li,Sisi Huo,Wei Wang,Zhen Hu,Xing Xu
Herein, we prepared two kinds of single-atom catalysts (SACs) with uniformed coordination structures (M−N 4 , M = Fe, and Cu) for evaluating the versatile pathways of peroxymonosulfate (PMS) activation by different metal sites. Fe-SAC exhibited a higher catalytic performance than that of Cu-SAC for chloroquine phosphate (CQP) oxidation. Results showed that the high-valent iron-oxo species accounted for 74.5 % for CQP oxidation in Fe-SAC/PMS system, while radicals (SO 4 •– and HO • ) dominated the CQP oxidation (58.3 %) in Cu-SAC/PMS system, which was associated to the different spin-state of the metal sites for PMS adsorption and breakage of O O in PMS as well as the intermediates in versatile pathways. The SACs were then fixed onto the catalytic filter for PMS activation , which showed stable and effective catalytic performance for versatile recalcitrant organics. Overall, this work not only provided the atomic-level knowledge on PMS activation, but also gave the potential applications of Fenton-like for water remediation.
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