Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Liuqun Fan,Zhiyan Hou,Tianbao Liu,Xiangjing Liang,Andrei Ivanets,Kongjun Ma,Xintai Su
Heteroatom-doped carbon materials derived from oil-bearing sludge exhibit excellent supercapacitor performance due to their unique electronic and chemical properties. However, the complex composition of heteroatoms in oil-bearing sludge makes it difficult to achieve sufficient and directional doping by direct pyrolysis . In this paper, an oleic acid pretreatment-roasting-secondary activation strategy was developed to make full use of hydrocarbons, iron- and nitrogen-containing compounds in oil-bearing sludge to prepare Fe-N X -C materials with excellent electrochemical properties. Characterization results such as transmission electron microscopy (TEM) and N 2 adsorption analysis showed that the best sample had a hierarchical pore structure and uniform Fe and N element loading. X-ray photoelectron spectroscopy (XPS) analysis found that the addition of oleic acid can promote the formation of Fe-Nx, and the dosage of oleic acid will affect the content of Fe-Nx in the carbon materials. Electrochemical characterization of this supercapacitor material was conducted. The best sample's specific capacitance was as high as 293.6 F g −1 at the current density of 0.5 A g −1 , and the capacitance retention rate could still reach 71.5% at the current density of 10 A g −1 . The assembled button-type symmetrical supercapacitors had an energy density of 8.68 Wh kg −1 and a power density of 137.53 W kg −1 , which is much higher than those of most other waste-based carbon materials. This work presents a new idea for the preparation of heteroatom doped carbon materials with excellent capacitive properties from oily sludge, which provides a new reference for the treatment and resource utilization of oily sludge.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 29
·期 52
·78874-78886
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IF 5.19
Xu Junge,Hu Die,Wang Yingmu,Zhang Ziwei
Ciprofloxacin (CIP) is a third-generation fluoroquinolones (FQs) antibiotic, and the occurrence of CIP in the water environment has raised growing concerns owning to its environmental toxicity. In this paper, a novel α-(Fe, Cu)OOH/RGO nanocomposite was synthesized via a one-step reflux method for CIP degradation through a photo-Fenton-like process. When the RGO content was 1 wt%, CIP degradation ratio by the α-(Fe, Cu)OOH/RGO nanocomposite reached 100% under visible light irradiation within 120 min, and total organic carbon (TOC) removal ratio reached 60% within 180 min. The result of molecular fluorescence spectra highlighted that the loading of RGO on the α-(Fe, Cu)OOH significantly increased the content of hydroxyl radicals (·OH) in the heterogeneous photo-Fenton-like system and simultaneously inhibited the recombination of photogenerated electron and hole, which played critical roles in the enhancement of CIP degradation. In addition, 11 main intermediates were identified as the degradation products of CIP in the α-(Fe, Cu)OOH/RGO/H 2 O 2 /visible light reaction systems using liquid chromatograph–mass spectrometer (LC-MS) analyses. The results demonstrated that three degradation pathways for CIP removal by α-(Fe, Cu)OOH/RGO nanocomposite occurred, including (i) oxidation on the piperazine ring and dealkylation, (ii) defluorination and decarboxylation, and (iii) hydroxylation on the quinolone ring. This work would provide a novel insight of CIP degradation pathways in photo-Fenton-like processes. Graphical abstract
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RSC Advances
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2022
·Vol. 12
·期 27
·17237-17248
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IF 4.036
Dongqing Feng,Jianxin Shou,Sen Guo,Mengna Ya,Jianfa Li,Huaping Dong,Yimin Li
Activation of hydrogen peroxide (H2O2) with biochar is a sustainable and low-cost approach for advanced oxidation of organic pollutants, but faces the challenge of a low yield of hydroxyl radical (˙OH). Herein, we hypothesize that the activation efficiency of H2O2 can be enhanced through co-catalysis of trace dissolved iron (Fe) with biochar. Two biochar samples derived from different feedstock, namely LB from liquor-making residue and WB from wood sawdust, were tested in the co-catalytic systems using trace Fe(III) (0.3 mg L−1). The cumulative ˙OH production in [Fe(III) + LB]/H2O2 was measured to be 3.28 times that in LB/H2O2, while the cumulative ˙OH production in [Fe(III) + WB]/H2O2 was 11.9 times that in WB/H2O2. No extra consumption of H2O2 was observed in LB/H2O2 or WB/H2O2 after addition of trace Fe(III). Consequently, the reaction rate constants (kobs) for oxidation of pollutants (2,4-dichlorophenoxyacetic acid and sulfamethazine) were enhanced by 3.13–9.16 times. Other iron species including dissolved Fe(II) and iron minerals showed a similar effect on catalyzing 2,4-D oxidation by biochar/H2O2. The interactions involved in adsorption and reduction of Fe(III) by biochar in which the defects acted as electron donors and oxygen-containing functional groups bridged the electron transfer. The fast regeneration of Fe(II) in the co-catalytic system resulted in the sustainable ˙OH production, thus the efficient oxidation of pollutants comparable to other advanced oxidation processes was achieved by using dissolved iron at a concentration as low as the concentration that can be found in natural water.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 30
·期 1
·1399-1412
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IF 5.19
Chen Jun,Zhang Boding,Wang Bingxing,Zhang Wenlong,Wang Jichao,Cui Chengxing,Wang Songlin
Wastewater containing quinoline has become a common pollutant in water and soil environments, which poses a threat to human health due to its carcinogenicity, teratogenicity, and mutagenicity. Quinoline’s stability and toxicity hinders its degradation by conventional physicochemical and biological methods. In this contribution, Fe-Co-Bi/kaolin particle electrodes were prepared for the efficient degradation of quinoline in wastewater, and characterized by using scanning electron microscope, X-ray diffraction, pyridine-IR, Brunauer–Emmett–Teller, X-ray photoelectron spectroscopy, and four-probe resistivity test. Parameters affecting the degradation efficiency were optimized to be the particle electrode dosage of 40 g/L, pH 3.5, H 2 O 2 addition of 67.6 mmol/L, electrical conductivity of 12.7 ms/cm, and voltage of 20 V. The constructed three-dimensional catalytic particle electrode system (3D-CPE) achieved 92.1% removal rate of chemical oxygen demand (COD) under the optimal conditions. Hydroxyl radicals (•OH) generated in the 3D-CPE process were identified by radical scavenging tests and electron spin response analysis. To unravel the degradation mechanism, the intermediate products were identified by using high performance liquid chromatography-mass spectrometry. The degradation mechanism was discussed with the help of theoretical calculation.
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APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Jianhui Zhu,Linchao Zeng,Xiaoya Li,Ning Zhao,Yanyi Wang,Zhilan Lin,Tingshu He,Libo Deng,Peixin Zhang
The inexpensive room-temperature sodium-sulfur (RT Na-S) battery has attracted extensive attention due to its various potential application but is still suffering from the low utilization of sulfur, the shuttle effect and the sluggish reaction activity of sodium polysulfides (SPSs). In this work, a TiO 2 /sulfur/atomic-iron loaded carbon nanosheet cathode is designed for high performance RT Na-S battery. When the atomic iron exists, a much higher electrochemical activity of sulfur was obtained, indicating the atomic iron can accelerate the conversion of SPSs. Furthermore, the TiO 2 layer can inhibit the shuttle effect of SPSs and the side-reaction between the intermediates and carbonate electrolyte. As a result, the constructed sulfur cathode exhibits a high reversible capacity (569.9 mAh g −1 with an initial coulombic efficiency of 57.57%) at 0.1 A g −1 and outstanding cycling performance (507 mAh g −1 after 50 cycles). This work provides a new strategy for preparing high performance cathode materials for RT Na-S battery.
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ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Shurui Xu,Guoyu Zhong,Linxin Qu,Zihao Liang,Tao Li,Yifei Yuan,Shaona Zheng,Wenbo Liao,Abdul Waqas Anjum,Xiaobo Fu,Jing Xiao
Selectively oxidizing alcohols to carbonyl compounds in an eco-friendly and sustainable way is of great importance. Instead of the noble catalytic system, we developed a novel catalytic system based on drilled carbon nanotubes (CNTs) assisted by Fe(NO3)3 that exhibits high activity for aerobic oxidation reactions. Interestingly, our studies demonstrated a direct relationship between the defects in the drilled CNTs and their activity. Catalytic evaluations revealed that the synergistic effect of drilled CNTs combined with Fe(NO3)3 resulted in unprecedented activity. The edge defects of the CNTs and electron transformation of Fe work synergistically to activate O2. Furthermore, the electronic transition from the drilled CNTs to Fe3+ confirmed the synergistic effect of the drilled CNTs/Fe(NO3)3. Thus, our studies not only demonstrate the use of drilled CNTs/Fe(NO3)3 in a sustainable catalytic system but also provide insight into the synergistic effect between these components for the universal oxidation of alcohols to carbonyl compounds.
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APPLIED CATALYSIS A-GENERAL
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2022
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IF 5.723
Minjie Xu,Chenxi Cao,Jing Xu
Direct CO 2 hydrogenation into linear α-olefins presents a promising route in carbon-neutral chemical manufacture. This work systematically investigated the variable interplay between Reverse Water-Gas Shift (RWGS) and Fischer-Tropsch Synthesis (FTS) during CO 2 hydrogenation using model Na-Fe 5 C 2 catalysts, combining dynamic/steady-state CO/CO 2 hydrogenation performance, intrinsic kinetics and multiple characterization results. Na-Fe 5 C 2 proves to be surface-enriched with FeO x sites over which RWGS readily proceeds. Meanwhile, CO 2 conversion under integral reaction conditions is limited by the subsequent FTS step due to a lack of available FeC x sites. The catalyst performance is steered by the properties and relative quantities of the two different active sites. Na addition promotes the refresh of FeO x sites and β-elimination of alkyl intermediates over FeC x sites, but at the cost of inhibiting the surface fraction of FeC x sites and thus the single-pass CO 2 conversion. These fundamental understandings will enlighten further development of CO 2 hydrogenation catalysts with improved hydrocarbon yields.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qiansheng Li,Hong Lu,Xiaolei Wang,Zhongqiang Hong,Ze Fu,Xinxin Liu,Jiti Zhou
Low solar energy utilization, instability of Fe ions and Fe(III)/Fe(II) cycle difficulty are three main factors, limiting the photocatalytic activity of the Fe/peroxymonosulfate (PMS) system. Herein, based on the N and Fe co-doped carbon dots (N, Fe-CDs) synthesized by a facile one-pot hydrothermal method, a new Fe(III)/Fe(II) cycle system for PMS activation under visible light irradiation was proposed. The characterization experiments showed that Fe has been successfully doped to the sp 2 graphitic structure and mainly existed as Fe-N and Fe-OH complexes, which played an important role in harvesting visible light, enhancing the stability of Fe ions and acting as active sites to accelerate electron transfer. Under visible light irradiation, the photogenerated electrons of N, Fe-CDs could be directly transferred to Fe (III) for Fe (II) formation via the ligand-to-mental charge transfer process, thus accelerating the Fe(III)/Fe(II) cycle. When N, Fe-CDs were used for activating PMS under visible light irradiation, aminopyrine could be efficiently degraded and mineralized to CO 2 via the cleavage of pyrazole ring, demethylation, hydroxylation, decarbonylation and the cleavage of benzene ring. The produced O 2 − and 1 O 2 played the main roles in the whole photocatalytic reaction. The above results revealed that the novel N, Fe-CDs could effectively activate PMS under visible light irradiation for the degradation of pharmaceuticals in the polluted water.
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ACS Omega
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2022
·
IF 4.132
Lina Zhang,Ying Zhang,Baikang Zhu,Jian Guo,Dongguang Wang,Zhongqi Cao,Lihui Chen,Luhui Wang,Chunyang Zhai,Hengcong Tao
Electrochemical CO2 reduction has been acknowledged as a hopeful tactic to alleviate environmental and global energy crises. Herein, we designed an Fe@C/g-C3N4 heterogeneous nanocomposite material by a simple one-pot method, which we applied to the electrocatalytic CO2 reduction reaction (ECR). Our optimized 20 mg-Fe@C/g-C3N4-1100 catalyst displays excellent performance for the ECR and a maximum Faradaic efficiency (FE) of 88% with a low overpotential of −0.38 V vs. RHE. The Tafel slope reveals that the first electron transfer, which involves a surface-adsorbed *COOH intermediate, is the rate-determining step for 20 mg-Fe@C/C3N4-1100 during the ECR. More precisely, the coordinating capability of the g-C3N4 framework and Fe@C species as a highly active site promote the intermediate product transmission. These results indicate that the combination of temperature adjustment and precursor optimization is key to facilitating the ECR of an iron-based catalyst.
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MOLECULES
·
2022
·Vol. 27
·期 6
·2035
·
IF 4.927
Jiao Jia,Hao Wu,Le Xu,Fengchun Dong,Yongtang Jia,Xi Liu
A nanofiber metal–organic framework filter, a polyacrylonitrile (PAN) nanofiber membrane composite with an iron/2-amino-terephthalic acid-based metal–organic framework (MIL101(Fe)-NH2), was prepared by one-step electrospinning. MIL101(Fe)-NH2was combined into the polymer nanofibers in situ. PAN-MIL101(Fe)-NH2composite nanofiber membranes (NFMs) were prepared from a homogeneous spinning stock containing MIL101(Fe)-NH2prebody fluid and PAN. Crystallization of MIL101(Fe)-NH2and solidification of the polymer occurred simultaneously during electrospinning. The PAN-MIL101(Fe)-NH2composite NFM showed that MIL101(Fe)-NH2was uniformly distributed throughout the nanofiber and was used to adsorb and separate acidic organic ionic dyes from the aqueous solution. The results of Fourier transform infrared spectroscopy, energy-dispersive X-ray spectroscopy, and X-ray diffraction analysis showed that MIL101(Fe)-NH2crystals were effectively bonded in the PAN nanofiber matrix, and the crystallinity of MIL101(Fe)-NH2crystals remained good, while the distribution was uniform. Owing to the synergistic effect of PAN and the MIL101(Fe)-NH2crystal, the PAN-MIL101(Fe)-NH2composite NFM showed a fast adsorption rate for acidic ionic dyes. This study provides a reference for the rapid separation and purification of organic ionic dyes from wastewater.Keywords:electrospinning;MIL101(Fe)-NH2;functional nanofibers;water treatment membrane
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ANALYTICAL LETTERS
·
2022
·
IF 2.267
Yuhui Weng,Huangjie Li,Mincong Zhu,Aojia Tao,Sha Wang,Wen Weng
Novel nitrogen/iron-codoped carbon dots (N/Fe-CDs) were prepared from citric acid, ethylenediamine, and ferric chloride by a facile one-step solvothermal method and their peroxidase-like activity was evaluated. The structure and composition of the obtained carbon dots were characterized by several methods, including electron microscopy, X-ray diffraction, and spectral techniques. The presence of dopants in the particles was confirmed by X-ray photoelectron spectroscopy and inductively coupled plasma – mass spectrometry (ICP-MS). The obtained N/Fe-CDs displayed excellent peroxidase-like activity and efficiently catalyzed the oxidation of 3,3',5,5'-tetramethylbenzidine in the presence of H2O2, leading to a rapid change in the solution color from colorless to blue. Based on this reaction, H2O2 was determined from 0 to 40 μM under optimal conditions with a detection limit of 9.0 nM. In addition, L-cysteine was shown to cause the blue color to fade. Considering this feature, a highly sensitive, fast, and specific colorimetric method was developed for L-cysteine with a detection limit of 15.8 pM, which is lower than observed in similar studies. Further, this colorimetric method was applied for the determination of L-cysteine in real samples, and the results of recovery and relative standard deviation were satisfactory. The reported catalyst can be prepared conveniently using readily available raw materials and is inexpensive, which is advantageous for its widespread application.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Mingyu Li,Yuhan Ma,Jingjing Jiang,Tianren Li,Chongjun Zhang,Zhonghui Han,Shuangshi Dong
Heterogeneous photo-Fenton technology has drawn tremendous attention for removal of recalcitrant pollutants. Fe-based metal-organic frameworks (Fe-MOFs) are regarded to be superior candidates in wastewater treatment technology . However, the central metal sites of the MOFs are coordinated with the linkers, which reduces active site exposure and decelerates H 2 O 2 activation. In this study, a series of 2, 5-dioxido-1, 4-benzenedicarboxylate (H 2 DOBDC)-functionalized MIL-100(Fe) with enhanced degradation performance was successfully constructed via solvothermal strategy. The modified MIL-100(Fe) displayed an improvement in photo-Fenton behaviors. The photocatalytic rate constant of optimized MIL-100(Fe)-1/2/3 are 2.3, 3.6 and 4.4 times higher compared with the original MIL-100(Fe). The introduced H 2 DOBDC accelerates the separation and transfer in photo-induced charges and promotes Fe(II)/Fe(III) cycle, thus improving the performance. •OH and •O 2 − are main reactive radicals in tetracycline (TCH) degradation. Dealkylation, hydroxylation, dehydration and dealdehyding are the main pathways for TCH degradation.
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