SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Xiulan Weng,Huijing Ma,Gary Owens,Zuliang Chen
Recently, bimetallic Fe-Pd nanoparticles were integrated with metal organic frameworks (MOFs) to produce a new composite catalyst with significant potential for organic contaminant removal due to enhanced adsorption and reduction. Here, 85.9 % of 2,4-dichlorophenol (2,4-DCP) was successfully removed from aqueous solution within 120 min when using a zinc-based zeolitic imidazolate framework (ZIF-8) embedded with Fe-Pd (Fe-Pd@ZIF-8). In comparison only 77.4 and 48.3 % was removed when using ZIF-8 or Fe-Pd alone. Thus, to better understand the function of composite components (ZIF-8 and Fe-Pd) in the removal of 2,4-DCP, and the specific removal mechanism involved, Fe-Pd@ZIF-8 was characterized before and after exposure to 2,4-DCP. This comparison revealed that 2,4-DCP was adsorbed onto the surface of the composite during exposure. Moreover, while ZIF-8 maintained stability following the removal of 2,4-DCP, Fe 0 was partially oxidized and Pd functioned as a catalyst in the removal process. Furthermore, kinetic studies demonstrated that the initial adsorption of 2,4-DCP conformed to a pseudo-second-order model and the subsequent reduction conformed to a pseudo-first-order model, whereas isothermal adsorption best fit the Freundlich adsorption model. This observation suggested that removal mechanism of 2,4-DCP involved both adsorption and dechlorination. Finally, Fe-Pd@ZIF-8 was applied to practically remove 2,4-DCP from wastewater, showing a 74.4 % removal efficiency which indicated that the composite was a potential new nanomaterial for practically removing organic contaminants from wastewater.
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JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 41
·19490-19501
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IF 4.682
Jin Mengjing,Wu Caixia,Li Xiaopeng,Bai Yunfei,Sun Guowen,Bai Zhaowen,Wang Gang,Wu Hongchang,Zhou Jinyuan,Li Jian,Pan Xiaojun,Xie Erqing
The MOFs materials exist potential application prospects in the energy storage field for their high specific surface area and porosity. However, the MOFs materials also suffer from poor conductivity during the charging and discharging processes. Compared with MOFs, MOFs-derived metal oxides not only inherit the porosity of the MOFs, but also present high conductivity owing to the derived carbon. Herein, an effective approach for encapsulating CoFe 2 O 4 into the derived carbon, which not only increases their conductivity but also restrains the volume expansion, and had excellent reaction kinetics. In this work, CoFe 2 O 4 nanoparticles have been synthesized by one-step annealed process. The electrode is used as the anode for LIBs and found to have long-term stability of 491 mAh g −1 at a current density of 1.0 A g −1 even after 500 cycles. The CoFe 2 O 4 electrode exhibits appreciable electrochemical performance, including 783 and 482 mAh g −1 at the current densities of 0.1 and 2.0 A g −1 , respectively. Such excellent electrochemical properties are ascribed to the porous structure of MOFs, which effectively promotes ion/charge transmission. This will guide material design and optimization of battery communities and electrochemical energy storage applications. Graphical abstract
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ChemSusChem
·
2022
·Vol. 15
·期 16
·e202200741
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IF 9.14
Ziyuan Xiu,Ming Zheng,Jiadong Li,Feng Wei,Changchang Dong,Mingrui Zhang,Xin Zhou,Xiaojun Han
Graphical Nitrogen reduction : A bionic nitrogen fixation system composed of Fe-VS 2 nanosheets and 1-aminoanthraquinone-functionalized polymethacrylic acid (1-AAQ-PA) matrix is fabricated with 1-AAQ-PA as the electron medium to achieved high NH 3 yield rate of 31.6 μg h −1 mg −1 and faradaic efficiency to NH 3 of 23.1 % in 0.05 m Li 2 SO 4 electrolyte at −0.35 V vs. reversible hydrogen electrode. This work provides inspiration and insights for the development of effective catalyst systems for nitrogen reduction. Electrochemical N 2 fixation is considered to be a promising alternative to Haber–Bosch technology. Inspired by the composition and structure of natural nitrogenase, Fe-doped VS 2 nanosheets were prepared via one-step solvothermal method. The electron transfer system mediated by organic conductive polymer (1-AAQ-PA) was constructed to promote the electron transfer between Fe-VS 2 nanosheets and the electrode in electrocatalytic N 2 reduction reaction (NRR). The obtained 1-AAQ-PA−Fe-VS 2 electrode converted N 2 to NH 3 with a yield of 31.6 μg h −1 mg −1 at −0.35 V vs. reversible hydrogen electrode and high faradaic efficiency of 23.5 %. The introduction of Fe dopants favored N 2 adsorption and activation, while the Li−S bond between Fe-VS 2 and Li 2 SO 4 effectively inhibited hydrogen evolution. The highly efficient electron utilization in the electrocatalytic NRR process was realized using the 1-AAQ-PA as the electron transfer medium. Density functional theory calculations showed that N 2 was preferentially adsorbed on Fe and reduced to NH 3 via both distal and alternating mechanism.
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PubMed
高影响因子
ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Yajie Guo,Xinyu Zhang,Dandan Zhang,Shunlin Li,Hui Wang,Yiyin Peng,Zhaoyong Bian
The present work demonstrates a simple one-step pyrolysis method for the synthesis of a catalytic sludge-based carbon (SBC) biochar containing Fe and Mn from dehydrated sludge with added KMnO 4 and Fe(II). The electrocatalytic degradation of triclosan (TCS) in water was evaluated using an Fe/Mn-SBC cathode to promote a heterogeneous Fenton-like reaction. The catalyst generated at 500 °C exhibited an abundant porous structure and a relatively high surface area, and produced an electrode with better conductivity and electron diffusion . The presence of metal oxides changed the surface structure defects of this biochar and enhanced its catalytic performance while increasing the electrochemically active surface area by 72.68 mF/cm 2 compared with plain SBC. TCS was degraded (91.3%) within 180 min by oxygen species generated in situ on an Fe/Mn-SBC cathode because the activation energy for oxygen reduction was lowered by 4.62 kJ/mol. The degradation of TCS followed pseudo first-order kinetics and was controlled by TCS diffusion and interfacial chemical reactions between adsorbed TCS and the electrode. Possible TCS degradation pathways were devised based on the main intermediates, and 1 O 2 was found to be more important than •OH radicals. Through toxicity test and prediction, the toxicity of degradation was gradually reduced. This study demonstrates a simple and ecofriendly method for the electrocatalytic degradation of organic pollutants.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Tianze Cong,Hui Huang,Hao Zhang,Chengwei Li,Yongpeng Zhao,Zeng Fan,Lujun Pan
In the surface-enhanced Raman scattering (SERS) measurements, it is very important to fabricate “hot spots” and concentrate the analytes into these regions. In this work, a hybrid structure of Au nanostars (NSs) with high SERS sensitivity and metal-organic framework MIL-101(Fe) with high molecular adsorption capability was constructed as high performance SERS substrate. The MIL-101(Fe) shell between AuNSs is several nanometers, promoting the construct of “hot spots” and the aggregation of target molecules. The as-prepared AuNS/MIL-101(Fe) has achieved high SERS sensitivity, long-time stability, reproducibility, and capability of universal detections. The limit of detection for rhodamine 6 G is down to 0.29 nM. Meanwhile, the SERS activity of AuNS/MIL-101(Fe) is kept for at least 30 days. Furthermore, the relative standard deviations of signals on five substrates are all less than 10 %. The as-prepared AuNS/MIL-101(Fe) also exhibit the SERS activities for various molecules including dyes, organic contaminants, pesticides, and amino acids , indicating that the AuNS/MIL-101(Fe) substrates have wide applications in chemical analysis and environmental monitoring.
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Environmental Science-Nano
·
2022
·Vol. 9
·期 9
·3407-3416
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IF 9.473
Han Song,Xinwen Ou,Mengye Wang,Yan Zhang,Zhang Lin
H2 production during the transformation of Fe(OH)2 into magnetite (i.e., Schikorr reaction), has a significant impact on many environmental applications, including the long-term effectiveness of permeable reactive barriers composed of zerovalent iron and the stability of geological radioactive waste repository. However, the reactivity of the Schikorr reaction is not systematically evaluated and its chemical mechanism still remains controversial. Here, we investigate water reduction on the Fe(OH)2 surfaces with the help of an interface-reaction model between water and Fe(OH)2. The Fe(OH)2 hexagonal nanosheets prepared using a coprecipitation method possess dominantly exposed (001) and (100) facets. As unveiled by the DFT simulations, the (001) Fe(OH)2 facet only exposes OH, which is, therefore, inert to water reduction. Moreover, the active Fe-exposed (100) Fe(OH)2 facet is more thermodynamically favourable for water adsorption and dissociation than the (101) and (102) facets. However, the high energy barrier for water dissociation (2.79 eV) may restrict the rate of water reduction on the Fe(OH)2 facet. In addition, the capacity of (100), (101), and (102) Fe(OH)2 facets to adsorb OH− is stronger than that for H2O, which further inhibits water reduction. Furthermore, DOS calculations manifest that Fe d orbitals play a significant role in H2O adsorption, indicating that manipulating the electronic structure of the Fe site is a critical path to mediate water reduction in Fe(OH)2. Our study provides new insights into the understanding of the mechanism of the phase transformation of Fe(OH)2 under anaerobic conditions in environmental and earth sciences.
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Journal of Cleaner Production
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2022
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IF 11.072
Da Liu,Wenyi Gu,Wenqi Zhou,Ying Xu,Wenjia He,Lizheng Liu,Liang Zhou,Juying Lei,Jinlong Zhang,Yongdi Liu
The activation of hydrogen peroxide (H 2 O 2 ) by Fe/carbon composites has been widely used for the removal of antibiotics. However, the secondary pollution of iron ions limits the application of Fe 2+ /H 2 O 2 system. In this work, three kinds of hydrogel materials combining metal-organic framework (MOF)-derived magnetic Fe/porous carbon (MagFePC) with sodium alginate (SA), polyacrylic acid (PAA) and agarose (AG) were prepared by different methods for removal of norfloxacin (NOR) antibiotics in simulated wastewater. After comparison, MagFePC/SA hydrogels synthesized by a titration forming method were found to have the advantages of good toughness, abundant pores and best Fenton activity. MagFePC/SA can effectively activate H 2 O 2 to remove NOR under neutral conditions, and there was almost no leaching of iron ions, causing no secondary pollution to the environment. The effects of pH, ionic strength and surfactants on the degradation performance for NOR were studied. Mechanism study revealed that ·O 2 − and 1 O 2 were the main active species for the degradation of NOR, and the materials still had good stability and reusability after repeated cycles. More important, we built a simple automated unit for wastewater treatment under laboratory conditions that can completely degrade a 5 mg/L NOR solution at a flow rate of 2 mL/min. Current works showed that MagFePC/SA had the advantages of simple synthesis, outstanding degradability , excellent stability and eco-friendly reaction, which was a wastewater treatment material with good prospect for industrial application.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Zhifeng He,Yuchen Jiang,Xin Cui,Zeyi Liu,Xin Meng,Jiafeng Wan,Fangwei Ma
Recently, molybdenum (Mo)-based catalysts have been proved to be effective NRR catalysts due to the high affinity of nitrogen to Mo. The design of a heterostructure and the introduction of defects, such as vacancies and heteroatom doping, are effective means to regulate the microstructure of catalysts and further improve their electrocatalytic N2 into NH3 performance. In this paper, VS-Fe-doped 1T/2H mixed-phase MoS2/C (VS means sulfur vacancies) heterostructure sphere-like nanoflowers with rich sulfur vacancies are prepared through a pectin-assisted hydrothermal reaction, followed by calcination and treatment with NaBH4 solution. VS-Fe-MoS2/C exhibits good electrocatalytic NRR performance with a high ammonia yield rate of 17.8 ± 0.7 μg h–1 mg–1 at −0.5 V versus reversible hydrogen electrode (vs RHE) and a Faraday efficiency (FE) of 9.2% at −0.3 V (vs RHE) under ambient conditions. Introducing sulfur vacancies, iron doping, and preparing 2H-phase MoS2 have greatly improved the performance of electrocatalytic nitrogen reduction to ammonia.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Linlin Zhang,Jie Wang,Chenglong Zhao,Feijin Zhou,Cheng Yao,Chan Song
The nanozymes-based sensing platforms have been attracted in recent years due to their outstanding performances in the practical applications. In this work, the magnetic Fe nanoparticles (NPs) with peroxidase-like activity was developed for the fast detection of glutathione (GSH). The Fe NPs were facilely prepared through the reduction of iron trichlorrde hexahydrate (FeCl 3 ‧6H 2 O) by sodium borohydride (NaBH 4 ) at room temperature , exhibiting a merit of simplicity. Significantly, the achieved Fe NPs have high peroxidase-like catalytic activity . At the room temperature, the colorimetric substrates such as 3,3′,5,5′-tetramethylbenzidine (TMB) and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) can be rapidly oxidized by Fe NPs with the help of H 2 O 2 . After incubated for just 30 s, the catalytic system could achieve a colored solution. Thus, the Fe NPs-based sensing systems can be employed in the development of the colorimetric biosensors with the naked-eye detection.
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Processes
·
2022
·Vol. 10
·期 4
·751
·
IF 3.352
Zixuan Tang,Zehui Bai,Xin Li,Le Ding,Bin Zhang,Xinghua Chang
Cu-based bimetallic materials have been widely reported as efficient catalysts for electrocatalytic nitrate reduction. However, the faradaic efficiency and selectivity are still far from satisfactory. Herein, Cu-Fe bimetallic nanoalloys with adjustable Cu/Fe ratios are successfully prepared through a reactive mechanical milling approach with CuCl2, FeCl3and Na as the starting materials. The optimized Cu3Fe exhibits excellent nitrate conversion efficiency of 81.1% and 70.3% ammonia selectivity at −0.7 V vs. RHE within 6 h under 0.1 M Na2SO4and 100 ppm NO3−. The Fe-introduction-induced upshift of thed-band center is identified to be beneficial for promoting nitrate adsorption on Cu3Fe. Moreover, favorable H generation under the assistance of Fe could effectively accelerate the stepwise hydrogenation during electrocatalytic nitrate reduction, resulting in significantly improved NH4+selectivity. This work supplies valuable insights for the rational design of transition-metal-based bimetallic catalysts for electrocatalytic nitrate reduction.Keywords:Cu-Fe bimetallic catalysts;nitrate to ammonia;d-band center regulation
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Liangyu Tong,Yunpeng Liu,Chenyu Song,Yuqing Zhang,Sanjay S. Latthe,Shanhu Liu,Ruimin Xing
Hollow hybrid heterostructures are regarded to be promising materials as bifunctional electrocatalysts for highly efficient water electrolysis due to their intriguing morphological features and remarkable electrochemical properties . Herein, with FeNi-PBA as both a precursor and morphological template, we demonstrate the rational construct of cost-effective (Fe,Ni)S 2 @MoS 2 /NiS 2 hollow hybrid heterostructures as bifunctional electrocatalysts for alkaline overall water splitting. Microstructural analysis shows that the hybrid is a kind of hierarchical heterostructure composed of MoS 2 /NiS 2 nanosheets/nanoparticles in situ grown on hollow (Fe,Ni)S 2 nanocubes with abundant heterointerfaces, which effectively maximizes the electrochemical active sites to the accessible electrolyte ions , leading to the promoted charge transfer. As expected, the hybrid shows remarkable alkaline electrocatalytic performance, such as hydrogen evolution overpotential of 176 mV and oxygen evolution overpotential of 342 mV at 50 mA cm −2 , as well a cell voltage of 1.65 V at 20 mA cm −2 . Moreover, the stability and durability are greatly enhanced under harsh electrochemical conditions. This study opens a new venue for developing earth-abundant bifunctional electrocatalysts with hollow hybrid heterostructures for alkaline water electrolysis in the future.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Peng Chu,Hailei Zhao,Jie Wang,Hongliang Xie,Chongqi Han,Zhao Yang
Negative current collectors play vital roles in the electrochemical performance of liquid metal batteries (LMBs). Employing a three-dimensional (3D) current collector is an effective approach to host molten lithium and reduce the effective current density. The Ni-Fe foam is a frequently used 3D current collector for the negative electrode. However, the corrosion of molten lithium towards the Ni-Fe foam skeleton devastates the 3D structure of the current collector and so deteriorates seriously the electrochemical performance of LMB. To enhance the corrosion resistivity, herein, the graphite layer coated Ni-Fe foam (Graphite@Ni-Fe) is prepared by the chemical vapor deposition method. The prepared scaly-like graphite layer plays a bifunctional role in chemistry, preventing corrosion as an effective barrier and improving remarkably the surface lithiophilicity of Ni-Fe foam. The assembled Li||Bi batteries with Graphite@Ni-Fe foam as negative current collector exhibit stable cycling performance with capacity retention of 98.10% and high Coulombic efficiencies over 98.3% at 0.4 A cm −2 over 100 cycles at 500 °C. More importantly, outstanding rate capability is achieved and almost no capacity degradation is observed upon current density change from 0.2 to 2.0 A cm −2 . This work highlights the importance of the lithiophilicity and the corrosion resistance ability of the negative current collectors for LMBs.
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