Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Ruina Xuan,Jiwen Chen,Yixin Dou,Zhuo Jiang,Xiaofang Li,Deng Ding,Chunlei Wang,Juntao Yan,Linbing Sun
Dual-co-catalyst-modified photocatalysts enhance charge separation efficiency, but the traditional dual co-catalyst is still difficult to get a high separation efficiency due to size and aggregation. Herein, we report bimetallic MIL-53(Fe/Mn) as dual co-catalysts with separate electron and hole mediators. CdS NPs were in-situ grown into MIL-53(Fe/Mn) at varying ratios. 20 %CdS/MIL-53(Fe/Mn) composites shown optimum photocatalytic CO 2 reduction activity. The XPS results shown the strong interaction between CdS and MIL-53(Fe/Mn). The EPR measure proved the carriers of CdS can be transferred to MIL-53(Fe/Mn) oxidation cluster by the oxo-Fe(III)/Fe(II) and oxo-Mn(II)/Mn(III) redox cycling, and the results also suggest the oxo-Fe(III) and oxo-Mn(II) were redox active sites. We believe the approach that bimetallic MOFs act as dual cocatalyst to improve the photocatalytic activity would open a new avenue for the separation efficiency of photo-generated charge carriers.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Jiangdong Dai,Sujun Tian,Yinhua Jiang,Zhongshuai Chang,Atian Xie,Ruilong Zhang,Chunxiang Li,Yongsheng Yan
Here, the magnetic hierarchical porous carbon (MHPC) with micromesopores was first prepared using ethylenediaminetetraacetic acid tripotassium (EDTA-3K) and iron nitrate by simultaneous magnetization/activation method. The optimal product was MHPC-20 with a high graphitization, which possessed a large SBET (1688 m2 g–1) and saturation magnetization (3.679 emu g–1). As expected, MHPC-20 had a very high maximum adsorption capacity (534.2 mg g–1) toward chloramphenicol (CAP) from water solution at 298 K with a positive correlation between SBET and adsorption amount. Additionally, MHPC-20 had a fast adsorption kinetic, only 250 min, and isothermal and kinetics data were well fitted by Langmuir and pseudo-second-order kinetic models, respectively. Moreover, the effect of ion strength, solution pH, and humic acid on CAP adsorption onto MHPC-20 were investigated, indicating a better stability. Besides, MHPC-20 showed good reusability and excellent magnetic separation performance, which implied MHPC-20 as a candidate could be applied in various complex wastewater environments.
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Journal of Environmental Sciences
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2018
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IF 3.12
Xiaole Zhao,Yingchun Su,Shubin Li,Yajun Bi,Xiaojun Han
Dyestuffs and heavy metal ions in water are seriously harmful to the ecological environment and human health. Three-dimensional (3D) flowerlike Fe(OH) 3 microspheres were synthesized through a green yet low-cost injection method, for the removal of organic dyes and heavy metal ions. The Fe(OH) 3 microspheres were characterized by thermal gravimetric analysis (TGA), Fourier transform infrared (FT-IR), and transmission electron microscopy (TEM) techniques. The adsorption kinetics of Congo Red (CR) on Fe(OH) 3 microspheres obeyed the pseudo-second-order model. Cr 6 + and Pb 2 + adsorption behaviors on Fe(OH) 3 microspheres followed the Langmuir isotherm model. The maximum adsorption capacities of the synthesized Fe(OH) 3 were 308, 52.94, and 75.64 mg/g for CR, Cr 6 + , and Pb 2 + respectively. The enhanced adsorption performance originated from its surface properties and large specific surface area of 250 m 2 /g. The microspheres also have excellent adsorption stability and recyclability . Another merit of the Fe(OH) 3 material is that it also acts as a Fenton-like catalyst. These twin functionalities (both as adsorbent and Fenton-like catalyst) give the synthesized Fe(OH) 3 microspheres great potential in the field of water treatment .
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FUEL
·
2024
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IF 6.7
Xixi Chen,Ruxing Gao,Qiang Wang,Kehao Hu,Fenfen Wang,Chao Deng,Lujing Xu,Chundong Zhang,Ki-Won Jun,Seok Ki Kim,Tiansheng Zhao,Hui Wan,Guofeng Guan
Direct hydrogenation of CO 2 to liquid hydrocarbons via modified Fischer-Tropsch synthesis represents an appealing and sustainable route for efficient CO 2 utilization. However, the selective production of liquid hydrocarbons remains a significant challenge. In this work, we designed a series of carbon-coated K/Fe-C catalysts with various K loadings (ranging from 0 to 8 wt%) that enhance C 5+ hydrocarbon selectivity during CO 2 hydrogenation. It is found that the 4 K/Fe-C catalyst exhibits the highest C 5+ selectivity of 54.78 % at CO 2 conversion of 32.40 % and good stability within 100 h time-on-stream. This is attributed to the high dispersion of the Fe nanoparticles and the confinement effect of porous carbon matrix on the aggregation of Fe nanoparticles, resulting in high catalytic activity and selectivity. Meanwhile, the well dispersed K on the porous carbon matrix can reduce the particle size of Fe nanoparticles and promote the production of iron carbide active species for CO 2 -FTS, thus facilitating the selective formation of C 5+ hydrocarbons. Moreover, we also discussed a possible reaction mechanism for the direct hydrogenation of CO 2 to C 5+ hydrocarbons over the K/Fe-C catalysts. This study provides deep insights into the design of efficient Fe-C catalysts for converting CO 2 to liquid hydrocarbons.
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AQUA-Water Infrastructure Ecosystems and Society
·
2024
·Vol. 73
·期 5
·930-944
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IF 2.1
Ye Miaomiao,Song Lei,Chen Peng,Li Kexin,Zheng Kai,Zhang Tuqiao,Liu Xiaowei
View large Download slide View large Download slide Close modal The S(IV)–Fe(II)/PM pretreatment has demonstrated preliminary potential as an effective ultrafiltration (UF) pretreatment technology. However, a comprehensive understanding of its impact on UF membrane fouling control and the dynamic evolution of membrane fouling during prolonged operation is still lacking. In this study, a relatively prolonged fouling experiment was conducted. Results revealed that the S(IV)–Fe(II)/PM pretreatment exhibited superior performance over Al(III) coagulation pretreatment in mitigating the transmembrane pressure difference and addressing both reversible and irreversible membrane fouling. The application of a cluster analysis method to classify membrane fouling evolution stages further confirmed that S(IV)–Fe(II)/PM pretreatment effectively decelerated the rate of membrane fouling evolution. The surface cake layer of UF membranes pretreated with S(IV)–Fe(II)/PM exhibited greater looseness and smoothness. It also showed better results than Al(III) coagulation pretreatment in reducing the accumulation of organic foulants, controlling the Si content and reducing the total microorganisms and live microorganisms in the UF feed water. Variance Partitioning Analysis indicated that the combined contribution of organic, inorganic, and biological foulants was the most significant for UF membranes after S(IV)–Fe(II)/PM pretreatment (50.4%) and UF membranes after Al(III) coagulation pretreatment (70.2%). These findings underscore the efficacy of S(IV)–Fe(II)/PM pretreatment in controlling UF membrane fouling under prolonged operation. S(IV)/Fe(II)/PM pretreatment efficiently mitigated UF membrane fouling during long-term operation. S(IV)/Fe(II)/PM pretreatment yielded a long uncontaminated stage and accelerated contaminated stage. S(IV)/Fe(II)/PM pretreatment suppressed the contribution of organic–inorganic–biological composite fouling.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Li-Zhi Huang,Xiang Zhan,Weiguo Chen,Changye Li,Liandong Zhu,Yitao Dai,Jia Deng
Carbon tetrachloride (CT), a common persistent pollutant in groundwater, has attracted widespread attention from environmental researchers. The dechlorination from CT to combustible hydrocarbons not only represents the removal of contaminants, but also offers the possibility of recovering carbon resources from water. In this work, we used the coprecipitation of Fe(II) and Pd(II) to synthesize Pd-Fe hydroxides for the dechlorination of CT. When Pd and Fe dosages were 0.4 and 5 mM respectively, CT with 26 µM concentration can be fast removed within 5 min, and 43.3 % of CH 4 and 11.6 % of C 2 H 6 (mol%) were generated after 110 min. The alkaline condition was more conducive to the complete dechlorination of CT comparing with acidic and neutral conditions. During the olation process, Fe(II) as electron donor transferred electrons to Pd(II) to form Pd(0) clusters. Pd(0) active sites act on the binding of CT and transfer electron to H + /H 2 O to form adsorbed atomic hydrogen (H ads •). The adsorbed CT molecules on the surface of Pd-Fe hydroxides undergo continuous dechlorination to form CH 4 and C 2 H 6 through the attack of H ads • and direct electron transfer. In real groundwater applications, CT was rapidly removed, with CH 4 and C 2 H 6 yields reaching 24.5 % and 4.6 % (mol%), respectively. Encouragingly, incomplete dechlorinated products, including chloroform and dichloromethane, did not show signs of subsequent rebound even after 60 min. Furthermore, Pd-Fe hydroxides also exhibit resistance to the oxidation effects of dissolved oxygen, which demonstrates the promising application prospects.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Si Duan,Yuan Gao,Guihong Lan,Haiyan Qiu,Bo Xu,Xiangming Liu,Ming Zhang,Yusong Chen
Functionalization of ligands is an effective strategy to enhance the adsorption performance of adsorbents. In this study, MIL-101(Fe)-R (R = -H, –OH, –NH 2 , and –NO 2 ) was selected as a platform for systematically studying the impact of functionalization on the adsorption behavior of chlortetracycline (CTC). A series of characterizations were conducted on the prepared MIL-101(Fe)-R to clarify the influence of organic linkers on the microscopic morphology, pore structure, and surface functionality of the adsorbents. Additionally, the effects of different functional groups on the adsorption behavior of MIL-101(Fe)-R were compared to screen for MOFs with high efficiency in removing CTC. Experimental results showed that the maximum adsorption capacities (q m ) of MIL-101(Fe), MIL-101(Fe)–NH 2 , MIL-101(Fe)–OH, and MIL-101(Fe)–NO 2 were 418.980 mg/g, 559.854 mg/g, 187.387 mg/g, and 154.131 mg/g, respectively. Among them, MIL-101(Fe)–NH 2 exhibited a higher mass transfer rate (reaching equilibrium in 15 min). Based on apparent adsorption behavior, adsorption kinetics, isotherm and thermodynamic studies, as well as FTIR and XPS characterizations before and after adsorption, the performance modulation mechanism of MIL-101(Fe)-R in CTC adsorption was discussed in detail. Combined with density functional theory (DFT) calculations, the host–guest interaction controlling the adsorption behavior was understood at the molecular level, demonstrating the optimal binding sites of the adsorbents. This study provides guidance for the design of efficient MOF adsorbents for antibiotic wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Wei Dong,Chunyan Du,Yin Zhang,Jiao Cao,Jingyi Jiang,Lu Zhou,Guanlong Yu,Yulv Zou,Huaiyuan Peng,Rong Yan,Yu Yang
Visible light-driven photocatalysis often struggles with fast recombination of photogenerated electron-hole pair and unsatisfactory degradation efficiency of hazardous micropollutants, such as antibiotics. Constructing an effective heterojunction can address these challenges. In this study, a novel S-scheme MIL-53(Fe)/FeOCl heterojunction composite was synthesized using a hydrothermal method. Factors influencing oxytetracycline (OTC) removal and the underlying reaction mechanism were investigated. The MF-10 composite demonstrated a remarkable removal efficiency of 90 %, significantly higher than that of MIL-53(Fe), which was 54 %. Even after six cycles, the degradation efficiency only decreased by 8 %, and the composition of MF-10 remained unchanged, indicating excellent durability. The photocatalytic process involves crucial reactive species such as · OH, SO 4 • – , O 2 • – , and h + . The heterojunction construction extends the absorption range of visible light, and the internal electric field enhances the separation of photogenerated electron-hole pairs while maintaining robust electron and hole activity. Additionally, photogenerated electrons facilitate the Fe(II)/Fe(III) cycling, resulting in the production of more reactive species for OTC degradation. This work introduces a novel approach to enhance the activity of photocatalysts and provides valuable insights into the design of peroxydisulfate activators.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Ahmed Zaki Alhakemy,Genxiang Wang,Kai Chen,Ahmed E. Hassan,Zhenhai Wen
Sluggish oxygen reduction reaction (ORR) kinetics limit the development of metal-air batteries and fuel cells, hindering overall energy conversion efficiency. Therefore, significant research has focused on cost-effective, highly active, and exceptionally stable non-precious metal ORR electrocatalysts. This study presents the synthesis of a nanohybrid material called Fe SAs/FN-CNs. It is made up of single iron atoms embedded in ultrathin porous carbon nanosheets that are co-doped with F and N. The synthesis process involves an easy one-step pyrolysis technique without additional post-treatment. The Fe SAs/FN-CNs material is designed to function as an effective zinc-air battery ORR electrocatalyst. Based on their distinctive components and structure, the optimal Fe SAs/FN-CNs exhibit outstanding catalytic efficiency and long-lasting performance in the alkaline ORR. They have an onset potential (E onset ) of 0.95 V, a half-wave potential (E 0.5 ) of 0.85 V, a kinetic current density (J K ) of 20.49 mA cm −2 at 0.8 V, and a diffusion-limited current (J d ) of 6.2 mA cm −2 . In addition, a Zn-air battery made using homemade Fe SAs/FN-CNs demonstrated a power density of 197 mW cm −2 , a specific capacitance of 813.5 mAh g −1 , and exceptional stability. It outperformed the commercial Pt/C by operating continuously for over 147 hours at 10 mA/cm² (discharge-charge). The Fe SAs/FN-CNs nanohybrid electrocatalyst shows great potential as an electrocatalyst for various metal-air batteries.
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LANGMUIR
·
2024
·
IF 3.7
Wenqing Han,Yehai Yan,Huifang Wang,Jinzhong Li,Ping Zhao,Zhihao Liu,Fei Yu,Jian Cui,Guangfa Zhang
Solar-driven interfacial water evaporation has become one of the most promising approaches to effectively harvesting freshwater, yet the fabrication of high-performance and multifunctional solar interfacial evaporators (SIEs) still remains a huge challenge to date. In this study, a multifunctional MXene and Fe-MOF@cellulose acetate/polyvinylpyrrolidone (MXM@CP) SIE was prepared via a facile “electrospinning and suction filtration deposition” coupling strategy. Thanks to the incorporation of MXene, MXM@CP displayed excellent photothermal conversion performance. Together with the fast water transport channel provided by the porous cellulose acetate electrospinning substrate, a remarkable solar-driven water evaporation property was achieved for MXM@CP, showing a higher water evaporation rate of 1.1 kg m–2 h–1 under one sun irradiation. Moreover, the resultant composite film also exhibited excellent Fenton catalytic activity to effectively degrade volatile organic compounds (VOCs) due to the synergistic effect of the MXene and Fe-based MOF (Fe-MOF). Particularly, a relatively higher degradation rate of 82.8% was acquired for the resulting evaporator toward the benzene contaminant. These results provide new insights into the construction of high-performance and multifunctional SIEs toward clean freshwater collection from the VOC-contaminated water system.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yan Jiao,Shaoqing Wang,Boyang Sun,Yu Han,Zilu Zhang,Xiuli Shen,Zhihe Li
The efficient removal and degradation of microplastics are critical for protecting aquatic ecosystems. Herein, Fe-modified magnetic biochar (MBC) was synthesized as an adsorbent for removing microplastics in water. The effects of lignin/Fe salt mass ratios, adsorbent amount, adsorption time, adsorption temperature, solution pH, and presence of coexisting anions on adsorption efficiency were investigated. The thermal degradation behaviour and recycling characteristic of microplastics was also explored. Results showed that MBC has a developed pore structure, superparamagnetic property, and abundant oxygen-containing functional groups. The removal efficiency of polystyrene microplastics using MBC-11 was 99 %, with an adsorption capacity of 68.57 mg/g, which was 25 times higher than that of unmodified lignin biochar. The kinetics of the adsorption process followed the pseudo-first kinetic model, and the equilibrium data best fitted the Freundlich model. Thermodynamic results confirmed that adsorption over MBC was a spontaneous, heat-absorbing, and entropy-increasing process. The adsorption mechanism of PS by biochar was mainly via electrostatic and hydrophobic interactions and pore throttle. The thermal-degradation products of PS were mainly hydrocarbons, including styrene, benzene, and toluene, owing to the enhanced β-scission, H-shift, and methylation reactions at MBC catalytic sites. This study provides a scientific basis for the development of control technologies for microplastics removal in water.
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ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Huanhuan Zhu,Shuo Chen,Xiaoying Huang,Xi Chen,Zhengjun Gong
Background Organophosphate flame retardants (OPFRs) are notorious emerging contaminants threatening the environment and human health. Triphenyl phosphate (TPHP), which has an extremely serious biotoxicity, is a typical harmful OPFR. Due to its wide use, TPHP has been discovered in various environmental mediums. Moreover, it is pretty recalcitrant to the removal process, resulting in the need for a technique to understand it better. Hence, accurate and quick discrimination of TPHP in the environment is critical to further evaluate its potential effect on ecosystems and human health. Results An ingenious oxidant-free chemiluminescence (CL) sensor based on the oxidant-free UV/MIL-100(Fe) gel system was established for TPHP detection. The oxidation of luminol in the UV-activated MIL-100(Fe) gel has resulted in remarkable CL emission, which is contributed by reactive oxygen species (ROS) generated by it. Notably, the CL intensity was inhibited significantly after introducing TPHP. An investigation into the mechanism underlying the effect of CL suppression demonstrated that TPHP competed with luminol to consume ROS from UV-activated MIL-100(Fe) gel, contributing to CL inhibition. The subsequent sensing performance experiments demonstrated the advantages of environmentally friendly, economic efficiency, user-friendly operation, rapid determination, potential for compact size, high selectivity, and sensitivity. Additionally, these investigations confirmed the low limit of detection (210 ng L −1 ) and wide linear range (10–1000 μg L −1 ). Significance In this paper, a green, economical, and oxidant-free CL sensing strategy for TPHP has been established. It has the advantage of being rapid, having the potential for compact size, high selectivity, and sensitivity. This ingenious method has promising applications in real-time and online environmental monitoring, and it paves the way for the rapid and environmentally friendly identification of emerging contaminants that are structurally stable and recalcitrant to remove.
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