SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Jia Deng,Xiang Zhan,Feng Wu,Shuxian Gao,Li-Zhi Huang
Trichloroethylene (TCE), one of the most frequently detected chlorinated organic pollutants (COPs) in groundwater, has potential risks to human health. The bimetallic system consisting of zero-valent iron (ZVI) and a second catalytic metal has been widely investigated for reductive dechlorination of COPs. However, the passivation layer of ZVI inhibits the electron transfer causing a low dechlorination efficiency. In this work, we designed a novel bimetallic system using Fe(OH) 2 and Ni for fast dechlorination of TCE. The reduction efficiency of TCE reaches 94.8 % after 5 h of reaction in the Fe(OH) 2 /Ni system. TCE was completely dechlorinated to nontoxic gas products including ethylene and ethane, which was attributed to the generation of active hydrogen species (H*) in the system. The Ni 2+ cations undergo the process of hydroxylation and olation. Subsequently, electrons of Fe(OH) 2 were transferred to Ni(II) causing the formation of Ni(0). The catalytic Ni(0) sites generate H* for TCE dechlorination via catalytic reduction of H 2 O/H + . A part of Fe(II) in the Fe hydroxide layer of Fe(OH) 2 was oxidized to Fe(III) leading to the formation of green rust with a hexagonal structure. Our work demonstrates Fe(OH) 2 /Ni is a promising composite material for the remediation of TCE-contaminated groundwater.
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Journal of Materials Chemistry B
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2021
·Vol. 9
·期 23
·4726-4734
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IF 6.331
Wenli Zhao,Guangpu Zhang,Yang Du,Shuangqin Chen,You Fu,Fan Xu,Xiangyun Xiao,Wei Jiang,Qingmin Ji
The proportion of Fe2+ and Fe3+ in Fe-based nanozymes is a key point in determining their catalytic activity. However, it is hard to adjust the Fe2+/Fe3+ ratio in nanozyme systems to achieve the best catalytic performance. In this work, we successfully regulate Fe2+/Fe3+ ratios in a wide range of 0.81–1.45 based on a novel porous platform of Fe doped silica hollow spheres. The homogeneous distribution and stable fixation of Fe components in Fe doped silica hollow spheres facilitate the valence regulation of Fe in the reduction heating in H2/Ar. When the Fe doped spheres (FeOx@SHSs) were used as nanozymes, different Fe2+/Fe3+ ratios have shown to influence the peroxidase-like catalytic activity greatly. The highest activity at the ratio of 1.41 should be due to the combined effects of the accelerated reaction rate by Fe2+ and the enhanced catalytic cycle efficiency by Fe3+. The FeOx@SHSs-based nanozyme is further applied to construct a facile colorimetric biosensing system, which exhibited extremely sensitive determination of glucose. This work presents an effective platform for controlling Fe valences and optimizing the peroxidase-like activity for catalytic processes or sensing systems.
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WATER RESEARCH
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2021
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IF 11.236
Shi-Qi Tian,Jing-Yao Qi,Yun-Peng Wang,Yu-Lei Liu,Lu Wang,Jun Ma
After reaction with permanganate or ferrate, the resulted Mn-loaded and Fe-loaded biochar (MnOx/biochar and FeOx/biochar) exhibited excellent catalytic ozonation activity. O 3 (2.5 mg/L) eliminated 48% of atrazine (ATZ, 5 μM) within 30 min at pH 7.0, while under identical conditions, ozonation efficiency of ATZ increased to 83% and 100% in MnOx/biochar and FeOx/biochar (20 mg/L) heterogeneous catalytic systems, respectively. Radical scavenger experiment and electron paramagnetic resonance (EPR) analysis confirmed that hydroxyl radical (•OH) was the dominant oxidant. Total Lewis acid sites on MnOx/biochar and FeOx/biochar were 3.5 and 4.1 times of that on the raw biochar, which induced enhanced adsorption of O 3 and its subsequent decomposition into •OH. Electron transfer via redox pairs on MnOx/biochar and FeOx/biochar was observed by cyclic voltammetry scans, which also functioned in the improved catalytic capacity. Degradation pathways of ATZ in MnOx/biochar and FeOx/biochar ozonation systems were proposed, with 34.6% and 44.8% of dechlorination effect accomplished within 30 min of reaction, which was improved by 4.1 and 5.3 times compared to pure ozonation. After 12-hour treatment, acute toxicity of ATZ oxidation products was reduced from 38.3% of pure ozonation system to 14.5% and 6.3% of activated ozonation systems with MnOx/biochar and FeOx/biochar, respectively. Mn-loaded biochar and Fe-loaded biochar have great potential for heterogeneous catalytic ozonation of polluted water.
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高影响因子
CARBON
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2020
·
IF 8.821
Qingwei Liu,Min Zeng,Jue Liu,Baiyu Guo,Xiaozhu Hao,Qian Cao,Yuchen Shang,Xin Sun,Jinzhang Liu,Xuexu Gao,jiheng Li,Jie Zhu,Xixiang Zhang,Ronghai Yu
Environment-friendly Fe-based material@N-doped carbon nanoparticles imbedded in polylactic acid (PLA) matrix are prepared and applied in microwave absorption field. In the synthesis process, polydopamine (PDA) in the precursor could rationally regulate the phases of the iron-based particles and carbon contents. It turns out that optimizing the chemical composition plays a vital role in modulating microwave absorption performance . For instance, the maximum reflection loss ( R Lmax ) for Fe@N-doped carbon particles (S-120) reaches −61.6 dB (12.56 GHz, 2.1 mm), and the effective bandwidth is 4.48 GHz (from 13.52 GHz to 18 GHz) with a thickness of only 1.7 mm. The excellent microwave absorption performance could be attributed to perfect impedance matching brought by the synergies of multiple components. Moreover, the microwave absorbers display not only high microwave absorption performance but also environment-friendly characteristics that can avoid leaving stubborn waste after failure. The preparation process of the composite is pollution-free and the PLA in the composite can almost be naturally degraded within one month under simulated marine environment. This work may provide a new perspective on preparing high-efficient functional materials which are also harmless to the environment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Wei Wang,Yunlei Zhong,Xinyu Zhang,Sainan Zhu,Yourong Tao,Yanxin Zhang,Hongsen Zhu,Yifei Zhang,Xingcai Wu,Guo Hong
Surface self-reconstruction by the electrochemical activation is considered as an effective strategy to increase the oxygen evolution reaction (OER) performance of transition metal compounds. Herein, uniform Co 2 (OH) 3 Cl microspheres are developed and present an activation-enhanced OER performance caused by the etching of lattice Cl − after 500 cyclic voltammetry (CV) cycles. Furthermore, the OER activity of Co 2 (OH) 3 Cl can be further enhanced after small amounts of Fe modification (Fe 2+ as precursor). Fe doping into Co 2 (OH) 3 Cl lattices can make the etching of surface lattice Cl − easier and generate more surface vacancies to absorb oxygen species. Meanwhile, small amounts of Fe modification can result in a moderate surface oxygen adsorption affinity, facilitating the activation of intermediate oxygen species. Consequently, the 10% Fe-Co 2 (OH) 3 Cl exhibits a superior OER activity with a lower overpotential of 273 mV at 10 mA cm −2 (after 500 CV cycles) along with an excellent stability as compared with commercial RuO 2 .
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ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Lijuan Cao,Xilong Wang,Chen Yang,Jiajia Lu,Xiaoyue Shi,Hongwei Zhu,Han-Pu Liang
The highly active bimetallic single-atom electrocatalysts are desirable for the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) but remain challenging. Herein, Fe/Pt single-atom bifunctional electrocatalysts (Fe1Pt1/NC) are initially fabricated by nitrogen doping during the pyrolysis of porphyra and adsorbed urea at high temperature with subsequent nitrogen anchoring of Pt4+ in aqueous solution with the as-synthesized nitrogen-doped carbon. The as-synthesized Fe1Pt1/NC electrocatalysts have been intensively characterized by HAADF-STEM, XAFS, HRTEM, XRD, and Raman analysis. Particularly, the Fe1Pt1/NC presents excellent electrocatalytic activity toward HER, with relatively low overpotential of 27 mV at 10 mA cm–2 and small Tafel slopes of 28 mV dec–1. Furthermore, the Fe1Pt1/NC electrocatalyst possesses superior ORR activity with an onset potential of 1.04 V and half-wave potential of 0.91 V. This work provides a feasible way to synthesize electrocatalysts with abundant single-atom sites using renewable biomass as a precursor.
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ACS Applied Nano Materials
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2020
·
IF 0
Shichuan Su,Long Huang,Shan Su,Chunfeng Meng,Hu Zhou,Liuting Zhang,Ting Bian,Aihua Yuan
The construction of active and durable electrocatalysts based on a high abundance of elements toward oxygen reduction reaction (ORR) is critical for proton-exchange membrane fuel cells and metal–air batteries. Here, a composite nanostructure composed of Fe/Fe3C-NC nanosheets and carbon nanotubes (G-Fe/Fe3C-NC/CNTs) was designed by simply annealing a glucose-chelated Fe-coordinated metal–organic frameworks. The introduction of glucose can not only effectively prevent the collapse of the initial two-dimensional (2D) leaflike zeolitic imidazolate frameworks (ZIFs) during the carbonization process but also boost the growth of carbon nanotubes (CNTs). Benefiting from efficient Fe/Fe3C and Fe–Nx moieties, high specific surface area, and electron-conducting highways provided by the unique composite structure, the obtained G-Fe/Fe3C-NC/CNTs electrocatalysts achieved an impressive ORR activity with a higher positive onset potential of 1.02 V and half-wave potential of 0.87 V over the commercial Pt/C. Significantly, it also exhibits outstanding stability after 6000 cyclic voltammogram (CV) cycles with nearly negligible decay in half-wave potential, which makes it one of the promising Pt-free catalysts for ORR.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Wenjiao Chen,Hui Zhao,Binbin Xu,Qiaorong Jiang,Susu Bao,Zhiyuan Jiang
To satisfy the growing demand for military and civil applications, it is necessary to develop high-efficiency microwave-absorbing materials. Herein, a pyrolysis process was developed to construct FeO x /Fe/C composites using filter papers saturated with ferric nitrate solution as the precursor. The three-dimensional textures of filter paper are well maintained during the pyrolysis process. Ferric nitrate is decomposed to Fe 2 O 3 and subsequently reduced to Fe 3 O 4 and Fe nanoparticles embedded in the carbon matrix via carbothermal reduction. Various gases produced during the pyrolysis process create foam and generate additional nanoscale pores in the carbon matrix. The chemical composition and structure of composites can be tailored by controlling the pyrolysis conditions. The microwave absorption properties of FeO x /Fe/C composites are closely related to the chemical composition and structure. The optimized product shows excellent microwave absorption properties: The strongest reflection loss (RL) is −37 dB at ∼12 GHz; the effective absorption bandwidth (RL < −10 dB) is 6.5 GHz with a thickness of 2.0 mm. The superior absorption properties of the optimized product can be ascribed to the synergies of multiple chemical components, hierarchically porous structures and abundant interfaces. This study also suggests a large-scale synthesis strategy for high-yield carbon-coated magnetic nanoparticles for high-performance microwave absorption materials.
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Journal of Cleaner Production
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2020
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IF 7.246
Runyuan Zhang,Xiaoxian Zheng,Bohan Chen,Jinlin Ma,Xiaojun Niu,Dongqing Zhang,Zhang Lin,Mingli Fu,Shaoqi Zhou
An increasing amount of antibiotics has been released into the aquatic environment and caused a serious threat to public health. In this study, a series of magnetic biochars (MBCs) were prepared via one-step graphitization and magnetization for sulfamethoxazole (SMX) removal. The effects of pyrolysis temperature and impregnated FeCl 3 concentration on SMX adsorption were investigated. Characterization of MBC were carried out through SEM, BET, XRD, FTIR, Raman and XPS analyses. The performance for sulfamethoxazole removal was evaluated with the adsorption kinetics and isotherms studies, and the influence of pH, temperature, ion and NOM on SMX adsorption capacity was also examined in batch studies. The results show that the physicochemical properties of the MBCs were dominated by the pyrolysis temperatures and the iron weight ratio. The iron species in MBCs contributed significantly to the enhancement of SMX adsorptive capacity , including increasing the carbonization degree, promoting the formation of oxygen-rich functional groups and providing more adsorption sites. The prepared MBCs was proved to be highly efficient for SMX removal, and the 300-MBC800 was the optimal sorbent with the maximum adsorption capacity of 187.31 mg g −1 , which was 5.3 times of the pristine biochar. The primary mechanisms for SMX adsorption include electrostatic interaction, π-π electron-donor-acceptor (EDA) interaction, hydrogen bonding, and Lewis acid-base electron interactions , mainly resulting from the graphitized structures and enriched functional groups on MBCs. This study demonstrated promise of MBC as an effective and environmentally friendly sorbent for removing SMX from wastewater with high adsorption capacity and cost effectiveness.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Yu Kang,Yujia Han,Ming Tian,Chuande Huang,Chaojie Wang,Jian Lin,Baolin Hou,Yang Su,Lin Li,Junhu Wang,Xiaodong Wang
Fe-based oxygen carries (OCs) have attracted wide attention due to the low cost and environmental compatibility for chemical looping methane partial oxidation. However, they usually suffer from low CH 4 reactivity mainly due to insufficient synergy between catalytic CH 4 activation and lattice oxygen mobility. In this work, Fe ions with different amount were incorporated into a novel garnet structure (Y 3 Fe x Al 5-x O 12 ), which exhibited drastically increased CH 4 conversion with reduction time. This resulted from in-situ formed Fe 0 sites at the early stage of reduction, which led to a more efficient reaction route involving methane catalytic decomposition on Fe 0 and the resulted carbon oxidation easier by lattice oxygen, compared with methane directly oxidized by OCs. Moreover, the amount of Fe ions in garnet influenced surface exposed Fe 0 sites and oxygen mobility, inducing Y 3 Fe 2 Al 3 O 12 performed the best with almost 94 % methane conversion thanks to the combined advantages of larger surface exposed Fe 0 and higher lattice oxygen mobility.
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INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
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2020
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IF 3.407
Youhong Sun,Jinhao Wu,Linkai He,Baochang Liu,Chi Zhang,Qingnan Meng,Xuliang Zhang
Diamond/WC-Fe-Ni composite is a potential composition for impregnated diamond drill bits. It is necessary to avoid the graphitization of the diamond from Fe and Ni under the powder metallurgy process. Boron carbide (B 4 C) was coated on diamond, and diamond/WC-Fe-Ni composites were consolidated by hot pressing at different temperatures. The influences of sintering temperature and interfacial structure on bending strength and wear behavior were investigated. The bending strength for diamond/WC-Fe-Ni composite was dependent on matrix densification and interfacial graphitization. Un-coated diamond was eroded by Fe-Ni matrix and partially converted to graphite during the sintering process at all sintering temperatures. In opposite, B 4 C coating was beneficial to matrix densification at a lower sintering temperature, and delayed the appearance of graphitization to around 1300 °C. Therefore, the diamond/WC-Fe-Ni composites with B 4 C coating exhibited larger bending strength and better wear behavior at a relative low sintering temperature.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Dan Mu,Wenshen Wang,Jianhui Li,Pin Lv,Renyuan Liu,Ying Tan,Chongxia Zhong,Yu Qi,Xuan Sun,Yihai Liu,Song Shen,Yuyu Li,Biao Xu,Bing Zhang
Macrophage accumulation is central to the pathogenesis of atherosclerotic plaques. Reducing macrophages in plaques is an appealing approach to attenuate the development of atherosclerosis. Chemodynamic therapy, specifically inhibiting hydrogen peroxide (H2O2)-rich cells in slightly acidic microenvironment, has emerged as a new method in tumor treatment. Herein, we manufactured ultrasmall dopamine-modified hyaluronic acid (HD)-stabilized Fe(III)-tannic acid nanoparticles (HFTNPs). HFTNPs can specifically accumulate in inflammatory macrophages in atherosclerotic plaques, provide brighter magnetic resonance images, promote reactive oxygen species (ROS) generation, and induce the death of inflammatory macrophages without damaging normal cells and tissues. In conclusion, HFTNPs have a tremendous potential as safe and effective diagnostic and therapeutic reagents for atherosclerosis.
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