CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yunning Chen,Xiaoyan Zhang,Lingling Wang,Xueying Cheng,Qingkun Shang
An Fe-HQLC/TiO 2 (HQLC: 8-hydroxyquinoline-7-carboxylic) flower composite was synthesized and characterized. Phenol and four antibiotics: ciprofloxacin, tetracycline, amoxicillin and erythromycin can be efficiently and rapidly degraded by the Fe-HQLC/TiO 2 flower under visible light. The results indicated that more than 95% of the four antibiotics could be removed within 15 min. The photodegradation products of the four antibiotics were studied by high-performance liquid chromatography and high-resolution liquid chromatography-mass spectrometry. It was found that the adsorption characteristics of the antibiotics and their degradation products had a great influence on the photocatalytic activity of the photocatalyst and on the degradation rate of the antibiotics in recycling. Although the Fe-HQLC/TiO 2 flower did not degrade the four antibiotics completely, the parent structure of the antibiotics was destroyed to some extent. Therefore, the environmental toxicity and cytotoxicity of the antibiotics were significantly decreased. Compared with other related research works, there are a few photocatalysts capable of efficient and rapid removal of antibiotics.
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CARBOHYDRATE POLYMERS
·
2020
·
IF 7.182
Chen Hou,Wenqiang Chen,Linhui Fu,Sufeng Zhang,Chen Liang,Yang Wang
In this study, a sulfate radical-advanced oxidation process (SR-AOP) was proposed by utilizing a bimetallic Co/Fe metal-organic frameworks/cellulose nanofiber membrane (Co/Fe bi-MOFs/CNF) as a catalyst for TBBPA degradation. Sulfate radicals (SO 4 –) and hydroxyl radicals (OH · ) were generated through the activation of peroxymonosulfate (PMS) by Co/Fe bi-MOFs/CNF. Co/Fe bi-MOFs/CNF was prepared by a facile solvothermal method and vacuum filtration. CNF acted as a natural substrates material to relieve the agglomeration of loaded MOFs . Additionally the composite membranes was easily separated from the reaction solution. The properties of the composite materials and the main factors that influenced TBBPA degradation were elucidated in detail, along with the TBBPA degradation intermediates, recyclability, and TBBPA degradation pathway. Almost 100 % of TBBPA was degraded within 30 min under optimal conditions, and the rate constant was determined to be 0.764 min −1 . Furthermore, the degradation rate of the composite membrane was 60 % after 4 cycles.
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Yiqiong Yang,Zenghui Zheng,Wenqing Ji,Jingcheng Xu,Xiaodong Zhang
Adsorption performance, interfacial interaction mechanism and contribution of pores concerning PFOA adsorption to Fe-based metal-organic frameworks (MOFs) including Fe-BTC, MIL-100-Fe and MIL-101-Fe are investigated using experiments and computational calculation at molecular level even electronic level. Fe-BTC (418 mg/g) with more Lewis acid sites demonstrates higher adsorption capacity of PFOA in comparison with MIL-100-Fe (349 mg/g) and MIL-101-Fe (370 mg/g). Adsorption isotherms and kinetics indicate presence of monolayer adsorption and chemisorption in adsorption process. The pH dependence of PFOA adsorption to Fe-based MOFs is statistically revealed by experiments and analysis of variance of response surface methodology (RSM). XPS spectra of MOF-PFOA corroborate that decreasing binding energy of Fe2p and increasing binding energy of F1s, suggesting the presence of Lewis acid/base complexing (LAB) and hydrophobic interaction in adsorption process. Differential charge demonstrates that Fe center and benzene of organic ligands are respectively electron acceptor and donor in adsorption process. Electronic level mechanism finds that LAB complexing dominates adsorption process due to highest overlap of electron cloud. Smaller pores such as triangle and pentagonal pores of Fe-based MOFs contribute to the load of PFOA, while larger hexagonal one enable PFOA to enter into cages, as revealed by computational calculation.
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PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 26
·12041-12052
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IF 3.553
Yi Xuerui,He Xiaobo,Yin Fengxiang,Yang Tong,Chen Biaohua,Li Guoru
The global NH 3 production is dominated by Haber–Bosch process, requiring high temperature and pressure. Electrochemical N 2 reduction reaction (NRR) under ambient conditions is a greener path for artificial N 2 fixation to NH 3 but calling for efficient catalyst to increase activity and selectivity. Herein, we report the iron-based metal–organic frameworks (MOFs), i.e., MIL-88B–Fe and amine-functionalized MIL-88B–Fe (NH 2 –MIL-88B–Fe) as efficient catalysts for electrochemical NRR under ambient temperature and pressure in neutral electrolyte. NH 2 –MIL-88B–Fe shows higher NH 3 yield rate of 1.205 × 10 –10 mol s −1 cm −2 than MIL-88B–Fe (3.575 × 10 –11 mol s −1 cm −2 ). Furthermore, NH 2 –MIL-88B–Fe exhibits the highest Faradaic efficiency of 12.45% at 0.05 V versus RHE. The control experiments prove that NH 3 is produced through electrocatalytic NRR. This work may trigger the interest of using MOFs as highly efficient catalysts for electrochemical NH 3 production.
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Frontiers in Chemistry
·
2020
·
IF 3.693
Rauf Muhammad,Wang Jingwen,Iqbal Waheed,Abbas Mazhar,Khan Sayed Ali,Khan Qudrat Ullah,Ren Xiangzhong,Zhang Peixin,Li Yongliang
The exploration of noble metal-free catalysts with efficient electrochemical performance toward oxygen reduction reaction in the acid electrolyte is very important for the development of fuel cells technology. Novel pyrolyzed heteroatom-doped Fe/N/C catalysts have been regarded as the most efficient electrocatalytic materials for ORR due to their tunable electronic structure, and distinctive chemical and physical properties. Herein, nitrogen- and sulfur-doped (Fe/N/C and Fe/N/C-S) electrocatalysts were synthesized using ferric chloride hexahydrate as the Fe precursor, N-rich polymer as N precursor, and Ketjen Black EC-600 (KJ600) as the carbon supports. Among these electrocatalysts, the as prepared S and N-doped Fe/N/C-S reveals the paramount ORR activity with a positive half-wave potential value (E1/2) 0.82 at 0.80 V vs. RHE in 0.1 mol/L H2SO4 solution, which is comparable to the commercial Pt/C (Pt 20 wt%) electrocatalyst. The mass activity of the Fe/N/C-S catalyst can reach 45% (12.7 A g−1 at 0.8 V) and 70% (5.3 A g−1 at 0.95 V) of the Pt/C electrocatalyst in acidic and alkaline solutions. As result, ORR activity of PGM-free electrocatalysts measured by the rotating-ring disk electrode method increases in the following order: Fe/N/C
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RSC Advances
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2020
·Vol. 10
·期 15
·8709-8716
·
IF 3.119
Lin Gu,Yunyun Dong,Yan Zhang,Bo Wang,Qing Yuan,Hongmei Du,Jinsheng Zhao
In this study, a nitrogen-containing ligand supramolecule named PPYTZ was successfully synthesized using 2,6-pyridinedicarboxylic acid chloride and 3,5-diamino-1,2,4-triazole in order to carry out oxygen reduction reaction (ORR). Such a polymer provides abundant coordination sites for iron ions, and the PPYTZ–Fe/C composite catalyst was formed with the PPYTZ–Fe complex loading on the surface of Vulcan XC-72 carbon. The physical characteristics and ORR performance of the composite catalysts were characterized systematically via various relevant techniques, and their catalytic activity and reaction mechanism were evaluated and compared. The results showed that the catalytic activities and the reaction mechanism of ORR were highly dependent on the formation of an Fe–N unit. Accordingly, the PPYTZ–Fe/C catalyst containing Fe–N active sites exhibited high ORR catalytic activity (an onset potential of +0.86 V vs. RHE) in 0.1 M KOH. Such an Fe–N catalyst can accelerate the adsorption of O2 and increase the limiting current density (from 2.49 mA cm−2 to 4.98 mA cm−2), optimizing the ORR catalytic process from a two-electron process to a four-electron process (an n value of 3.8).
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Peng Liu,Dengjie Zhong,Yunlan Xu,Nianbing Zhong,Guangjun He
Co/Fe co-doped porous graphite carbon (Co/Fe-PGC) nanocomposites were successfully prepared by one-step pyrolysis with CoFe-MOF, in which the Co/Fe nanoparticles were uniformly coated on porous graphite carbon derived from MOF. It was used to microelectrolysis-Fenton degrade rhodamine B through the main active substance ∙OH. The color and TOC removal rate of 100 mg/L rhodamine B reached 99.41% and 64.6%, respectively, for 30 min. Rhodamine B was degraded into small molecular organic acids, alcohols and lipids by N-demethylation and chromophore cleavage, until it was finally degraded into CO 2 and H 2 O, and no new colored organics were produced in the degradation process. The degradation process follows the first-order reaction kinetics, and its rate constant is much higher than that of the previous similar studies. The excellent catalytic performance of Co/Fe-PGC catalyst is attributed to the coupling effect of micro-electrolysis and Fenton reaction, and the acceleration of cobalt on electron transport and Fe 2+ reduction. Co 0 /Fe 0 undergoes galvanic corrosion to generate Co 2+ /Fe 2+ and H 2 O 2 , and then these products undergo Fenton reaction to generate Co 3+ /Fe 3+ and ∙OH, thus forming a circulating system of Co 3+ /Fe 3+ and Co 2+ /Fe 2+ , enhancing the activation of H 2 O 2 and ensuring the efficient degradation of RhB.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Mingjie Huang,Sisi Peng,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Tao Zhou
This study has revealed how the strong metal-support interaction (SMSI) between carbon nanotubes (CNTs) and Mn 0.65 Fe 2.35 O 4 (MnFeO) in boosting peroxymonosulfate (PMS) activation for rapid sulfamethoxazole (SMX) degradation. As synergized by CNTs, the PMS-activation efficiency of MnFeO could be enhanced by>24 times, but with the similar PMS-activation mechanism. It was explored that the SMSI-induced abundant surface hydroxyl groups, in cooperation with the highly hydrophobic CNTs, favored the rapid in situ interfacial degradation of SMX. This feature also endowed the MnFeO-CNTs catalyst resistance to high salinity waters containing inorganic anions (e.g., Cl - and NO 3 – ) of weak complexing abilities. Moreover, the SMSI allowed the greatly accelerated redox cycle rate of Mn species by electron-rich CNTs, resulting in efficient PMS activation. Furthermore, the application feasibility of the MnFeO-CNTs/PMS system was demonstrated for a SMX-spiked real reverse osmosis (RO) concentrate. It was found that higher concentration of PMS could realize the complete removal of SMX, despite the existence of electron-rich tyrosine-like substances would compete with the SMX degradation in the MnFeO-CNTs/PMS system. This study demonstrated that the SMSI could boost the PMS activation , and could serve as an effective material strategy for in situ interfacial organics degradation in the high salinity wastewater.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yuanfeng Wei,Weijian Yang,Zhimin Wang,Kai Yin,Tao Chen,Chengbin Liu
Iron oxide-modified biochars are increasingly recognized as a promising arsenic adsorbent. However, most of them face serious challenges in the rapid and efficient removal of As(III). Herein, we integrated the iron oxide nanoneedles vertically covered biochar fibers (Fe-BFs) with H 2 O 2 and Hydroxylamine (HA) to construct a heterogeneous catalytic system for the rapid oxidation and deep removal of As(III) from water. The system oxidized the As(III) to As(V) with high efficiency, and then the generated As(V) could be rapidly removed by adsorption onto Fe-BFs. The removal efficiency of As(III) by Fe-BFs/H 2 O 2 /HA at 120 min reached up to 98.93%, which is much higher than that of by Fe-BFs (69.20%) and Fe-BFs/H 2 O 2 (92.32%). The system could work reliably in a wide pH range (4–10). Moreover, fixed-bed column experiments demonstrated that the addition of H 2 O 2 and HA could increase the effective treatment volume from ~350 bed volume (BV) to ~700 BV to meet the drinking water standard (<10 μg/L). The introduction of HA induced the reduction of surface Fe(III) of Fe-BFs to surface Fe(II), which reacted with H 2 O 2 to produce OH. The OH played a very important role in promoting the removal of As(III). This study offers a new strategy to enhance the applicability of Fe modified biochar for As(III) removal.
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Sustainable Environment Research
·
2021
·Vol. 31
·期 1
·1-12
·
IF 4.98
Liang Dongxu,Chen Yu,Zhu Suiyi,Gao Yidi,Sun Tong,Ri Kyonghun,Xie Xinfeng
Herein, a KFeS2 whisker was formed in mass production at a low temperature, with waste cold-rolling sludge as Fe source, which exhibited good performance in the removal of Zn/Ni from real electroplating effluent. At laboratory scale, KFeS2 was generated at 80 °C by the hydrothermal method, and KFeS2 whisker grew radially with the extension of the reaction time. This method was applied at pilot scale, where a similar KFeS2 whisker was also produced with waste cold-rolling sludge as Fe source, and a residual brownish supernatant was observed after the reaction and then completely recycled in the next round for KFeS2 synthesis. After recycling five times, the produced KFeS2 whisker did not change. The drying and storage of KFeS2 have also been verified. Freeze drying and vacuum drying were applicable, whereas air drying was not profitable. Moreover, the efficiency of Zn/Ni removal using undried KFeS2 was similar to that of dried KFeS2. The efficiencies of Zn/Ni removal using KFeS2 were apparently higher those of common reagents for wastewater treatment.
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Journal of the Taiwan Institute of Chemical Engineers
·
2021
·
IF 5.876
Xin Li,Shengxiao Zhang,Mingwu Yu,Hu Xu,Jungang Lv,Shuangshuang Yang,Xiaotong Zhu,Li Li
Background It was an effective method and research focus to remove recalcitrant organic pollutants by advanced oxidation processes based on persulfate activation with composite material as heterogeneous catalysts. Methods Fe/N co-doped biochar (Fe/N-BC) was synthesized via one-pot calcination method with anhydrous FeCl 3 , melamine, and grape skin powder as precursors. Characterization results showed that biomass and melamine could anchor iron species on BC matrixes by coordination. Significant findings The Fe/N 0.1 -BC exhibited significant activities toward peroxymonosulfate (PMS) activation, and 20 mg/L RhB can be degraded completely in 10 min with 0.05 g/L of the material and 0.5 g/L PMS. Electron paramagnetic resonance (EPR) study and free radical quenching experiments indicated that singlet oxygen ( 1 O 2 ), sulfate radicals (SO 4 •− ), and hydroxyl radicals (•OH) were the main reactive oxidizing species, and non-radical mechanism and free radical process were considered to be involved in the degradation of the pollutants. Control experiments revealed that the enhanced active sites were mainly ascribed to rich defects as well as the synergistic effect among Fe and N doping into carbon substrate. The Fe/N-BC owned the merits of environmentally friendly raw materials, easy synthesis, and high activation efficiency, exhibiting splendid prospect for environmental application.
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Nano Research
·
2021
·Vol. 14
·期 11
·4304-4313
·
IF 8.897
Zhai Yi,Wang Fumin,Zhang Xubin,Lv Guojun,Wu Yuzhou,Jiang Tao,Zhang Qing,Li Mengyue,Li Mengyao,Liu Yongkui
How to directionally design the hollow zeolite via a green route is of great significance. Here, we successfully synthesized the hollow Fe-silicate-1 encapsulated ultra-small Fe 2 O 3 nanoparticles (2.5 nm) with higher yield (85.2%) by mother liquid than traditional dissolution-recrystallization for the first time, which was achieved by precisely regulating the number and distribution of defects in zeolite and cleverly utilizing the TPAOH and nuclei in mother liquor. The effects of synthetic temperature, synthetic period and addition amount of parent zeolite on the formation of hollow zeolite have been investigated and the effect of synthetic conditions on the defects in parent zeolite has been also firstly quantified. The corresponding formation mechanism has been proposed. The abundant inner defects provided by the zeolite synthesized at 130 °C for 1 day and large amount of TPAOH remaining in mother liquid are conducive to the formation of hollow zeolite. Meanwhile, both parent zeolite and nuclei (4-, 5-member rings and structure units) in mother liquid obtained at 130 °C play the crucial roles in enhancing the zeolite yield. Notably, Fe 2 O 3 nanoparticles could decompose into small fragments by the interaction with nuclei in mother liquid. Partial ultra-small Fe 2 O 3 nanoparticles would be encapsulated in cavity and the rest could be inserted in the zeolite framework, which is significantly different from the conventional dissolution-recrystallization mechanism. The obtained encapsulated catalyst shows the superior catalytic performance and stability in phenol and tetracycline degradation reactions.
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