Green Energy & Environment
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2021
·
IF 8.207
Ruichang Xue,Mengwei Guo,Zhuoming Wei,Qibo Zhang
Ni–Fe bimetallic electrodes are currently recognized as a kind of benchmark transition metal-based oxygen evolution reaction (OER) electrocatalysts. Facile synthesis of Ni–Fe bimetallic electrode materials with excellent catalytic activity and satisfied stability by a simple and low-cost route is still a big challenge. Herein, well-defined Ni–Fe nanoparticles in-situ developed on a planar Fe substrate (Ni–Fe NPs/Fe) is fabricated via a facile one-step galvanic replacement reaction (GRR) carried out in an Ethaline-based deep eutectic solvent (DES). The prepared Ni–Fe NPs/Fe exhibits outstanding OER performance, which needs an overpotential of only 319 mV to drive a current density of 10 mA cm −2 , with a small Tafel slope of 41.2 mV dec −1 in 1.0 mol L −1 KOH, high mass activity (up to 319.78 A g −1 at an overpotential of 300 mV) and robust durability for 200 h. Impressively, the Ni–Fe bimetallic oxygen-evolution electrode obtained from the Ethaline-based DES is catalytically more active and durable than that of its counterpart derived from the 4.2 mol L −1 NaCl aqueous solution. The reason for this is mainly related to the different morphology and surface state of the Ni–Fe catalysts obtained from these different solvent environments, particularly for the differences in phy–chemical properties, active species formed and deposition kinetics, offered by the Ethaline-based DES.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Chen Hou,Yi-Ran Xing,Le-Le Yu,Yong-Heng Si,Han Lu,Yu-Juan Zhao
Fe–Mn based Li-rich cathode materials are regarded as one of the most promising cathode materials for their low cost and high energy density but possess drawbacks such as high oxygen release, low conductivity, and slow kinetics for lithium-ion transport. To address these issues, herein, we proposed a high-valance cations Nb 5+ doping strategy and synthesized a series of Li 1.26 [Fe 0.22 Mn 0.52 ] 1−x Nb 0.74x O 2 ( x = 0, 0.02, 0.03, 0.04) cathode materials. Using a combination of experimental approaches and density functional theory (DFT) calculations, we found that the doped samples presented expanded interlayer spacing for Li-ion migration and better structural stability due to the large ionic radius of Nb 5+ and the strengthened Nb–O bond. Moreover, Nb doping could not only decrease the band gap and the density of states of the O 2p band but also contribute extra electrons to surrounding O atoms, thereby enhancing electronic conductivity and stabilizing lattice oxygen. Benefit from the underlying mechanisms mentioned above, the Nb 0.022 sample possessed a higher Coulombic efficiency (71.1 vs 65.0%) at 0.2 C, showing more stable cycling performance (90.4 vs 67.7 mAh g −1 ) at 0.5 C and rate capability. These favorable results can assist in the development of Fe–Mn based Li-rich cathode materials with excellent electrochemical properties.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
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IF 8.128
Zhendong Yu,Jiachen Ma,Xiaoyi Huang,Yuancai Lv,Yifan Liu,Chunxiang Lin,Rongni Dou,Xiaoxia Ye,Yongqian Shi,Minghua Liu
In this study, the S modified iron-based catalyst (S-Fe@C) for activating peroxydisulfate (PDS) was fabricated by heating the S-MIL-101 (Fe) precursor at 800 °C. The resulted S-Fe@C composite mainly consisted of carbon, Fe 0 , FeS, FeS 2 , and Fe 3 O 4 , and showed strong magnetism. Compared with Fe@C obtained from MIL-101 (Fe), the S-Fe@C exhibited much higher performance (1.5 times larger) on PDS activation and the S-Fe@C/PDS could rapidly degrade various organic pollutants in 5 min under the attack of the species of SO 4 - · , 1 O 2 , electro-transfer and Fe(IV). The S element in enhancing the PDS activation mainly involved two mechanisms. Firstly, the doped S could speed up the electron transfer efficiency, resulting in a promotion on PDS decomposition; secondly, the S 2- S 2 2- or S 0 could achieve the circulation of Fe 2+ and Fe 3+ , leading to the formation of non-radicals Fe(IV) and 1 O 2 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Qianzhen Fang,Ni Liu,Yanling Gu,Hailan Yang,Shujing Ye,Zhongzhu Yang,Gaobin Chen,Xiaofei Tan,Xinjiang Hu
Metal-based materials are widely regarded as promising catalysts for activating peroxymonosulfate (PMS) to remove refractory organic contaminants with high efficiency. In our study, Ni-Fe layered double hydroxide (LDH)-biochar (BC) composite-induced PMS-based advanced oxidation process (AOP) was utilized to elucidate the degradation of tetracycline hydrochloride (TCH). In Ni-Fe LDH-BC/PMS system, more than 99% TCH (45 μM) could be removed effectively at low doses of oxidant (PMS, 0.10 mM) and catalyst (Ni-Fe LDH-BC, 0.10 g/L) addition within 80 min. Besides, the Ni-Fe LDH-BC/PMS system showed high resistance to some inorganic anions, and the Ni-Fe LDH-BC composite possessed excellent reusability in the degradation of TCH (>99% in four cyclic experiments). The reaction mechanisms were investigated via electron paramagnetic resonance detection, chemical quenching tests, probe experiments, and electrochemical measurements. These results indicated that the electron-shuttle mechanism played the dominant role in the removal of TCH. It is worth noting that determination of PMS concentration can reflect the reliability of quenching experiments. In the Ni-Fe LDH-BC composite, BC could not only improve the dispersion of Ni-Fe LDH, but also increase the conductivity of Ni-Fe LDH. Overall, a successful modification strategy was proposed in our study to improve the catalytic property of Ni-Fe LDH, and reaction mechanisms of TCH degradation were discussed deeply and comprehensively.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2019
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IF 2.931
Aiwen Yu,Yiping Tang,Kai Li,Jinwei Gao,Yuhui Zheng,Zhi Zeng
Fluorescence has been well documented and the optical feature of carbon dots generates considerable interests. Here the nitrogen-doped carbon dots with a relative quantum yield of 25% have been prepared. It displays stable blue emission based on the excitation at 355 nm. The carbon nanomaterial is highly dispersible in aqueous solution and can be employed as an effective optical probe for label-free detection of Fe 3+ (0.87 μM) via a switched off change. Additionally, such sensing nanoplatform can be recovered in the presence of pyrophosphate (PPi) and an “off-on” process has been identified. It is expected that this on-off-on strategy will allow new possibilities for developing efficient sensors in industrial fields.
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CHEMOSPHERE
·
2023
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IF 8.8
Yuxin Liu,Qintie Lin,Junli Zheng,Xindan Fan,Kehuan Xu,Yongjie Ma,Jin He
In this work, the magnetic nanocomposite Fe@SiC was prepared by a hydrothermal method and determined by SEM, XRD, XPS, FTIR and VNA. Fe 3 O 4 particles were loaded onto SiC with great success, and the synthesized composites had favorable microwave absorption properties. Fe@SiC was used to activate persulfate in a microwave field for the degradation of BDE209 in soil. Specifically, the synergistic interaction between microwaves and Fe@SiC showed excellent catalytic performance in activating PS to degrade BDE209 (90.1% BDE209 degradation in 15 min). The presence of •OH, O 2 • − and 1 O 2 was demonstrated based on quench trapping and EPR experiments. LC ‒ MS was applied to determine the intermediates and propose the possible degradation pathway for BDE209 in the MW/Fe@SiC/PS system, and it was found that BDE209 produced almost no lower brominated diphenyl ethers. Therefore, the toxicity of BDE209 was found to be reduced using toxicity assessment software. Overall, this work provides an effective approach for the degradation of BDE209 in environmental remediation.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Feijian Xiao,Dezhi Yang,Chun Xun,Haiyan Li,Qiulan Li,Zitao Zhong,Daqiao Wei,Yaling Yang
Nanozymes have drawn increasing attention due to unique enzyme-mimic catalytic activities for the treatment of bacterial infections. Herein, a novel tri-metal nanozyme for synergistic eradication of Escherichia coli ( E. coli ) and Staphylococcus aureus ( S. aureus ) was generated by Mo/Fe doped carbon dots (Mo/Fe-CDs) wrapping copper peroxide (CuO 2 ) nanozyme (Mo/Fe@CuO 2 ). Mo/Fe@CuO 2 showed near-infrared (NIR) light-enhanced peroxidase-like catalytic activity, and H 2 O 2 self-supply to promote the generation of reactive oxygen species (ROS) for highly efficient antibacterial photothermal therapy. The CuO 2 could generate H 2 O 2 in the acidic microenvironment, and Mo/Fe-CDs consequently could convert H 2 O 2 to hydroxyl radicals (·OH), resulting in the improvement of sterilization efficiency. Interestingly, Mo/Fe-CDs could activate the transformation of Cu 2+ to Cu + through the co-catalytic reaction based on the Mo 4+ /Mo 6+ and Fe 3+ /Fe 2+ redox couples, and provided photonic hyperthermia (PTT) to enhance the peroxidase-like activity. Meanwhile, Mo/Fe@CuO 2 showed glutathione (GSH) oxidase-like activity, which can achieve the depletion of glutathione (GSH) in bacteria, thus significantly improving the bactericidal effect. The collaborative eradication of bacteria, through innovative metal carbon-based nanozyme technology, provides a powerful and feasible approach to treating bacterial infections that threaten human health.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
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IF 16.6
Chen Da,Xia Zhaoming,Guo Zhixiong,Gou Wangyan,Zhao Junlong,Zhou Xuemei,Tan Xiaohe,Li Wenbin,Zhao Shoujie,Tian Zhimin,Qu Yongquan
Inspired by structures of natural metalloenzymes, a biomimetic synthetic strategy is developed for scalable synthesis of porous Fe-N 3 single atom nanozymes (pFeSAN) using hemoglobin as Fe-source and template. pFeSAN delivers 3.3- and 8791-fold higher oxidase-like activity than Fe-N 4 and Fe 3 O 4 nanozymes. The high catalytic performance is attributed to (1) the suppressed aggregation of atomically dispersed Fe; (2) facilitated mass transfer and maximized exposure of active sites for the created mesopores by thermal removal of hemoglobin (2 ~ 3 nm); and (3) unique electronic configuration of Fe-N 3 for the oxygen-to-water oxidation pathway (analogy with natural cytochrome c oxidase). The pFeSAN is successfully demonstrated for the rapid colorimetric detection of glutathione with a low limit of detection (2.4 nM) and wide range (50 nM–1 mM), and further developed as a real-time, facile, rapid (~6 min) and precise visualization analysis methodology of tumors via glutathione level, showing its potentials for diagnostic and clinic applications.
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高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 48
·18342-18353
·
IF 4
Minghao Dou,Mengjie Yao,Kai Ding,Yuye Cheng,Hongyu Shao,Shenjie Li,Yanyan Chen
Heterostructures formed by combining semiconductor materials with different band structures can provide work functions, d-band positions and electronic properties different from bulk materials and are considered as an effective strategy to improve the catalytic activity through electronic modification. In this study, an efficient MoS2/Fe-Ni3S2/NF heterojunction material was prepared by a two-step hydrothermal method. With the help of flake Ni(OH)2 synthesized in the first step, growth sites were provided for flake Ni3S2. The electronic structure of Ni3S2 was optimized by Fe doping, while the construction of the MoS2/Fe-Ni3S2 heterostructure allowed the catalyst to expose more active sites. MoS2/Fe-Ni3S2/NF exhibited a small charge transfer resistance and excellent electrocatalytic performance. At a current density of 10 mA cm−2, only low overpotentials of 148 mV and 118 mV were required for the oxygen precipitation reaction (OER) and hydrogen precipitation reaction (HER), respectively. Notably, when MoS2/Fe-Ni3S2/NF is used as the anode and cathode for overall hydrolysis, only 1.51 V is required to reach a current density of 10 mA cm−2, demonstrating its great potential for application in hydrolysis. This work provides a feasible idea for the rational construction of non-precious metal bifunctional electrocatalysts with excellent performance.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 48
·26573-26579
·
IF 11.9
Zhiwen Li,Yan Xie,Jianxin Gao,Xiaoke Zhang,Jia Zhang,Yu Liu,Gao Li
The in-depth understanding of the functions and interactions of multiple transition metal-based species in non-noble metal electrocatalysts is still obscure and challenges the oxygen reduction reaction (ORR). Herein, we rationally developed a Hm/Cy@C-900 electrocatalyst comprising multiple iron active sites of FeSx and Fe3C clusters and FeNx sites, which was characterized using XRD, S/TEM, and Mössbauer analyses. Hm/Cy@C-900 exhibited a high ORR performance (E1/2 0.845 V vs. RHE) in an O2-saturated KOH electrolyte, which outperformed the Hm/TCA@C-900 counterpart and commercial Pt–C electrocatalysts. Furthermore, the equipped zinc–air battery (ZAB) of Hm/Cy@C-900 could reach a power density of 192 mW cm−2@260.7 mA cm−2, which is much more efficient than that of Hm/TCA@C-900 (131 mW cm−2@201.2 mA cm−2) and a 20 wt% Pt–C catalyst (109 mW cm−2@221.3 mA cm−2). The superior ORR performance of Hm/Cy@C-900 was attributed to the promotional effect of FeSx and Fe3C clusters with FeNx active sites. Our work provides a rational design for and in-depth synthesis of FeNSC electrocatalysts for promoting the ZAB activity.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Jiaxing Zhang,Ajuan Zhou,Limin Ren,Min Yang,Guangjin Hou,Anfeng Zhang,Chunshan Song,Xinwen Guo
A clear understanding of the acidity-activity relationship is an important prerequisite for designing functional materials in alkylation of benzene with methanol. Herein, a series of b -axis-oriented [Fe/Al]-MFI nanosheets with similar thickness but varied acidities were prepared by tuning Fe incorporation to systematically study the effect of acidity on their alkylation performance. Comprehensive physiochemical studies demonstrate that tetrahedral framework type Fe species are dominated. The incorporation of Fe significantly weakens the strong acid strength of zeolite thus endowing the samples with proper acidity, consequently showing a strong inhibition effect on the by-product ethylbenzene. Moreover, a long-term stable operation (>300 h) is further achieved over the [Fe]-S-1 nanosheets by optimizing the content of framework Fe. This work elucidates the important relationship between acidity and alkylation activity.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·
IF 5.8
Wang Lanbin,Chen Yu,Xu Yangming,Ma Yanping,Du Yaguang
With the shortage of high-quality raw materials and increasingly strict environmental regulations, the recovery of metals from copper slag and pyrolusite has become a research hotspot. A novel method for simultaneously extracting Mn and Fe from pyrolusite and copper slag has been proposed. Under the optimal conditions (Copper slag / Pyrolusite = 2, H 2 SO 4 = 2 M, liquid—solid ratio = 10, T = 90 ℃, holding time = 60 min), the leaching efficiencies of Mn and Fe can reach 98.28% and 99.04%, respectively. In addition, the treated residue containing 60.04 wt% SiO 2 can be used as a raw building material. Through chemical kinetics and mineralogical transformation analyses, Fe 2 SiO 4 in copper slag decomposes to release Fe 2+ , which can reduce and leach Mn from pyrolusite. The unreacted shrinkage nuclear reaction model under the control of the surface chemical reaction is the most suitable model to describe the process, and when the apparent activation energy is 35.50 kJ/mol, the apparent rate equation is:
$$1-{\left(1-\times \right)}^{1/3}=979.65{\left[\mathrm{CS}/\mathrm{Pyrolusite}\right]}^{2.6072}{\left[{\mathrm{H}}_{4}{\mathrm{SO}}_{4}\right]}^{1.3143}{\left[\mathrm{L}/\mathrm{S}\right]}^{0.5649}e\mathrm{xp}\left(-35.50/\mathrm{RT}\right)$$ Graphical Abstract
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高影响因子
危险品化学品经营许可证（带存储）