APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Song Cheng,Chen Shen,Hao Zheng,Fuqiang Liu,Aimin Li
Preparing heterogeneous electro-Fenton (HEF) catalysts without sacrificing activity towards the two-electron (2e − ) oxygen reduction reaction (ORR) is a challenge, since Fenton-like active sites consist mainly of transition metals that prefer the 4e − ORR pathway. In this study, oxidized carbon nanotubes (OCNTs), which are promising ORR catalysts for the 2e − ORR, were uniformly attached to the surface of Prussian blue analogue (PBA) microcubes, forming a unique chainmail-like catalyst (OCNTs/PBA). 50 mg/L of sulfamethazine (SMZ) was completely removed within 30 min over OCNTs/PBA HEF process, with the first-order kinetic constant increased by 287.2 % compared with that PBA alone. To reveal the mechanism behind the enhanced catalytic activity, several possible interactions between the OCNTs and PBA were proposed and investigated further. This study not only offers a facile method to prepare a chainmail-like HEF catalyst, but also provides valuable insights into the rational design of HEF electrocatalysts with dual Fenton-like and ORR activity.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
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IF 4.551
Tao Jiang,Weiling Luan,Yufeng Ren,Chenyao Fan,Qi Feng,Lyudmila Turyanska
Exploring an economical and efficient oxygen reduction reaction (ORR) is an essential but challenging field of study. Metal–organic frameworks (MOFs) have emerged as promising candidates for the preparation of porous catalysts. Here we propose a synergistic heat treatment (SHT) method to synthesize Fe–N–C-SHT catalyst with hierarchical porous hollow structures via a simple carbonization method by the synergistic heating of ZIF-8-Fe (ZIF-8 doped with Fe) and ZIF-67 in a tube furnace. Fe–N–C-SHT catalyst displays efficient ORR activity (half-wave potential ( E half ) = 0.88 V versus reversible hydrogen electrode (RHE) with a loading of 0.204 mg Fe-N-C-SHT cm −2 ), which is superior to that of Fe–N–C synthesized using individual heat treatment (IHT) ( E half = 0.84 V) and Pt/C catalyst ( E half = 0.86 V). We achieve enhanced catalytic properties, enhanced methanol tolerance, and long-term durability of the Fe–N–C-SHT catalyst in alkaline electrolyte . The improved ORR activity is attributed to the synergistic effect of Fe doping and optimized SHT methodology, which led to the formation of a highly porous catalyst with numerous active sites. The developed SHT method presents a novel route to fabricate Fe–N–C catalysts with hollow-mesoporous-microporous structures and high performance in ORR.
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LUMINESCENCE
·
2020
·Vol. 35
·期 8
·1350-1359
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IF 1.855
Liu Zhang,Yue Hou,Xiaoyan Guo,Wei Liu,Congcong Lv,Chunyang Zhang,Yan Jin,Baoxin Li
In this study, three types of Fe(III) bipyridyl or phenanthroline (Fe(III)-L 3 ) complex could directly catalyze 3,3′,5,5′-tetramethylbenzidine (TMB) to induce blue chromogenic changes without H 2 O 2 . Fe(III)-L 3 complex could induce a colour change in TMB directly after a short incubation time. Due to the high oxidase-like activity of the Fe(III)-L 3 complexes, superoxide anion radicals (O 2 •– ) were formed in solution. Intermediates radical involving oxo-iron species were then produced that oxidized TMB to its oxidation products (oxTMB), which had an absorbance maximum at 652 nm. Glutathione (GSH) could inhibit the oxidation reaction of the Fe(III)-L 3 complex–TMB system, a rapidly colorimetric method was established for the specific detection of GSH that had a detection limit of 0.1 μM. Furthermore, Fe(III)-L 3 complexes could catalyze TMB to oxTMB directly without H 2 O 2 . This fast and simple colorimetric method may open a new avenue for application in the point-of-care diagnosis field using the TMB chromogenic system.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Hejun Ren,Xiong Jin,Chenguang Li,Tingting Li,Yang Liu,Rui Zhou
In this study, we reported that the presence of rosemary acid (RA) could strongly enhance the Fe(III)-mediated Fenton oxidation of 2,4-DCP as the model contaminant at near neutral pH. This enhancement was verified by the strong chelating and reducing ability of RA, which could prevent ion precipitation and accelerate the Fe 3+ /Fe 2+ cycle. Radical quenching experiments and electron paramagnetic resonance confirmed the existence and roles of hydroxyl radicals in the Fe 3+ /RA/H 2 O 2 system. Lot size optimized experiments were executed to achieve efficient 2,4-DCP degradation (99.93%) under the optimum conditions of 100 μmol/L Fe 3+ , 100 μmol l/L RA and 8 mmol/L H 2 O 2 within 60 min. In addition, co-existing metal ions , inorganic anions and natural organic matters were proved that they could inhibit removal efficiency and rate at varying degrees. Total organic carbon and chloride ion measurements were employed to probe the mineralization of organic matters (including RA and 2,4-DCP). This study provides a new modified Fenton system to enhance the oxidation removal of refractory organics in water and will enrich the understanding on effective H 2 O 2 activation at neutral pH.
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NANOTECHNOLOGY
·
2020
·Vol. 31
·期 13
·135403
·
IF 3.551
Taowen Dong,Ting Deng,Xianyu Chu,Tingting Qin,Haoxiang Wang,Zizhun Wang,Wei Zhang,Weitao Zheng
Earth-abundant Fe2O3 is a promising material for the negative electrode of supercapacitors by virtue of its wide potential windows. However, the unsatisfactory electrical conductivity and poor ionic diffusion rate within Fe2O3 results in degraded electrochemical performance. In this work, to address these issues, we demonstrate an easy method to synthesize Fe-based zeolitic imidazolate framework (Fe–ZIF) derived α–Fe2O3@C with remarkable supercapacitive properties. The as-obtained α–Fe2O3@C electrode, with the particular benefit of dispersed distribution of carbon, enabling fast electrochemical response, presents a prospective specific capacitance of 161 Fg−1 at a current density of 1 Ag−1. Furthermore, by using the α–Fe2O3@C architecture as the negative electrode, we fabricated a supercapacitor with Na0.5MnO2 as the positive electrode. Our supercapacitor shows a high energy density of 25 Whkg−1, while the corresponding power density is 2400 Wkg−1 at a current density of 2 Ag−1.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Wenwu Zhou,Yue Liu,Qi Sun,Jianyong Ye,Long Chen,Jia Wang,Guiqin Li,He Lin,Yuanqing Ye,Weifan Chen
A new series of orange highly near-infrared reflective pigments based on Fe-doped La2W2O9 were effectively fabricated via solution combustion synthesis. The acquired pigment powders were characterized by powder X-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, ultraviolet–visible–near-infrared spectrophotometry, and CIE 1976 L*a*b* color scales. Then, the energy consumption of the air-conditioning system was simulated based on EnergyPlus software. The results showed that the doping of Fe3+ ions will change the color of the pigment from white to orange. Meanwhile, the band gaps of La2W1.85Fe0.15O9-δ and La2W1.8Fe0.2O9-δ shifted from 3.71 to 3.07 eV and 2.96 eV, respectively. The typical La2W1.85Fe0.15O9-δ pigment powders showed the highest near-infrared reflectance of 89.25% between 700 and 2500 nm and impressive color (L* = 74.20, a* = 22.69, and c* = 22.42). The simulation results illustrated that the homeowner could save $7.32 per month by coating the walls and roofs of the building with the energy-saving paint composed of La2W1.8Fe0.2O9-δ. Excellent chemical stability and high near-infrared reflectance made the synthesized pigments a potential candidate for energy-saving coatings.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Chen Zhe-qin,Zhong Xiao-cong,Xie Yong-min,Liu Jia-ming,Xu Zhi-feng,Wang Rui-xiang
Metal–air batteries have shown tremendous potential as devices for electrical energy storage and conversion; however, their commercial applications are limited owing to the high costs of precious metal catalysts. In this study, urea was employed as a dispersant and as an additional nitrogen source to synthesize zeolitic imidazolate framework-derived iron-nitrogen-carbon catalysts (ZIF-8-derived Fe-NCs). The fabricated nitrogen-rich catalyst was found to have a high specific surface area and numerous surface defects, while maintaining the original ZIF-8 morphology. Electrochemical analysis with a rotating ring-disk electrode revealed that the onset potential of nitrogen-rich Fe-NC was 0.91 V at 1600 rpm with a limiting current density of 5.38 mA·cm −2 , which indicated a high catalytic activity for the oxygen reduction reaction. Additionally, the decent stability of the catalyst was confirmed by a 2 h cycle test.
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WATER AIR AND SOIL POLLUTION
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2021
·Vol. 232
·期 9
·1-13
·
IF 2.52
Li Qiuyue,Huang Kaibo,Duan Xingchun,Liang Jiahao,Chen Xinran,Tao Xueqin,Lu Guining
In this research, the feasibility of UV/Fe(III) photocatalytic technology for the degradation of tris (2-chloroethyl) phosphate (TCEP) was investigated. Experimental results showed that TCEP had a significant removal efficiency in UV/Fe(III) ([TCEP] 0 = 10 ppm, [Fe 2 (SO 4 ) 3 ] 0 = 0.5 mM, near-100% degradation rate after 90 min). A free radical scavenging experiment and EPR detection indicated that the formation of ·OH by the Fe(III) under ultraviolet light played a major role. Experiments on influencing factors revealed that oxygen accelerated the degradation of TCEP by accelerating the Fe(II)/Fe(III) cycle, but Cl − and PO 4 3− inhibited TCEP degradation. Three intermediate products were generated, including C 4 H 9 Cl 2 O 4 P (product A, m/z 222.9690), C 6 H 13 Cl 2 O 5 P (product B, m/z 266.9954), and C 2 H 6 ClO 4 P (product C, m/z 160.9762). Moreover, the degradation pathways primarily involved the C–Cl bond and phosphoric center being attacked. Escherichia coli toxicity test revealed that UV/Fe(III) treatment reduced environmental risk of TCEP. Therefore, UV/Fe(III) photocatalysis is a promising technique for TCEP control in wastewater treatment. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Ahmed Mahmoud Idris,Xinyan Jiang,Jun Tan,Zhenzhi Cai,Xiaodan Lou,Jin Wang,Zhengquan Li
Dye-sensitized system holds great potential for the development of visible-light-responsive photocatalysts not only because it can enhance the light absorption and charge separation efficiency of the systems but also because it can tune the band structure of catalysts. Herein, two-dimensional (2D) Fe-MOF nanosheets (Fe-MNS) with a LUMO potential of 0.11 V ( vs. RHE) was prepared. Interestingly, it has been found that when the 2D Fe-MNS catalyst was functionalized with visible-light-responsive [Ru(bpy)] 3 2+ as a dye-sensitizer, the electrons from the [Ru(bpy)] 3 2+ can effectively inject into the 2D Fe-MNS, which resulted in a negative shift of the LUMO potential of the 2D Fe-MNS to −0.15 V ( vs. RHE). Consequently, the [Ru(bpy)] 3 2+ /Fe-MNS catalytic system exhibits a sound photocatalytic CO 2 -to-CO activity of 1120 μmol g -1 h −1 under visible-light-irradiation. The photocatalytic CO production was further ameliorated by regulating the electronic structure of the 2D Fe-MNS by doping Co ions , achieving a remarkable photocatalytic activity of 1637 μmol g -1 h −1 . This work further supports that the dye-sensitized system is an auspicious strategy worth exploring with different catalysts for the development of visible-light-responsive photocatalytic systems.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yunjin Yao,Huanhuan Hu,Hongda Zheng,Hongwei Hu,Yinghao Tang,Xiaoyan Liu,Shaobin Wang
Bimetallic Fe- and Mo-embedded N-enriched porous biochar (Fe-Mo@N-BC) is developed and serves as a cost-effective and highly efficient catalyst for mineralization of non-biodegradation organic contaminants . Fe-Mo@N-BC was prepared by pyrolysis of complex Fe/Mo -containing precursors. Transmission electron microscopy and elemental mapping suggested that Fe and Mo are uniformly dispersed in nitrogen-doped biochar with hierarchical mesopores . In comparison to Fe@N-BC and Mo@N-BC, Fe-Mo@N-BC exhibited a superior activity for activating peroxymonosulfate (PMS). The stable activity was ascribed to N-doping and synergistic effect of Fe and Mo species, where both Fe-N x and Mo-N x can simultaneously serve as the active sites and N-BC can act as a carrier and an activator as well as an electron mediator. Electron paramagnetic resonance and quenching experiments indicated that H O • , O 2 • − and 1 O 2 were responsible for organic degradation . The effects of PMS dosage, initial Orange II concentration, temperature, solution pH, coexisting anions and humic acids on organic degradation were also investigated. With the assistance of an external magnet, Fe-Mo@N-BC can be easily separated after reaction and remains stable in the reusability tests. This work demonstrates a feasible strategy towards the fabrication of Fe, Mo-embedded N-enriched porous biochar catalysts for the detoxification of organic contaminants.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Shabab Hussain,Xinsheng Peng
Metal organic frameworks (MOFs) based Nanofiltration (NF) membranes have promising advantages in the separation of dyes and salts to purify the industrial polluted water. Herein, we report the synthesis of porphyrinic, porous and ultra-fast photothermal sensitive iron tetrakis(4-carboxyphenyl)porphyrin) (Fe-TCPP) MOFs nanofibers and the corresponding thin film nanocomposite (TFN) membranes by facile interfacial polymerization (IP). The Fe-TCPP nanofibers based TFN membrane enhances the pure water permeance to 28.1 L·m −2 ·h −1 ·bar −1 ( i.e., 3.5-fold higher than thin film composite (TFC)) by providing continuous hydrophilic flow pathways to permeate. The Fe-TCPP nanofibers contribute to the surface of TFN membrane, resulting not only fast permeation, but also ultra-high rejection of dyes i.e., 97.2%, 98.3% and 99.1% for Indocyanine Green, Brilliant Blue-R and Direct Red-80, respectively. Additionally, the TFN membrane also demonstrates 23–43 % salts rejection. Due to the ultra-fast photothermal responsive nature of Fe-TCPP nanofibers (88.4 °C increased temperature in 2 sec photo exposure), the water permeation of TFN NF membrane increases 30 % with 0.5 min under visible light-irradiation. This photo-induced ON/OFF separation is switchable. The enhanced permeation, high dyes rejection and photo-modulated ON/OFF nano-separation opens a new avenue for TCPP-based MOFs in the water purification technologies.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2021
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IF 4.291
Yuliya E. Tyutereva,Petr S. Sherin,Evgeniya V. Polyakova,Vyacheslav P. Grivin,Victor F. Plyusnin,Olga V. Shuvaeva,Jing Xu,Feng Wu,Ivan P. Pozdnyakov
The p-arsanilic acid (p-ASA) is widely used in agriculture as a food additive to control parasites. It leaves the body almost unchanged and is subsequently destroyed by environmental factors with the formation of toxic forms of inorganic arsenic. UVA irradiation of p-ASA with the addition of the Fe(III) oxalate complex leads to an effective photodegradation of the target compound. However, this method needs high concentrations of reagents and the keeping high [oxalate]:[Fe(III)] ratio to maintain proper efficiency of Fe(III) oxalate system. In this work, to overcome these problems, potassium persulfate (PS) was used as an additional oxidizer to improve Fe(III) oxalate system. It was found that the sulfate radical produced upon PS activation reacts readily with both neutral and monoanionic forms of p-ASA yielding corresponding organic cation radical, bimolecular rate constants are (7.3 ± 0.6) × 10 9 and (2.4 ± 0.4) × 10 9 M −1 s −1 , accordingly. Addition of 1 mM of PS reduces to one order (from 1.6 to 0.12 mM) the working concentration of oxalate and allows to achieve the complete degradation of both p-ASA and organic byproducts to inorganic As(V). Also the proposed approach demonstrates high efficiency in a wide range (from <0.5 to 3 ppm) of p-ASA concentrations.
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