SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Bin Meng,Erping Cao,Liwei Jia,Yuhua Zheng,Yanbin Cui
A variety of Cu-Fe oxide supported on Na 2 CO 3 -modified activated carbon (CuFeNaAC-X) catalysts were prepared via the impregnation and calcination methods and their desulfurization performance was evaluated at low-temperature. By optimizing the loading content of Cu-Fe, the sulfur capacity of the CuFeNaAC-5 reached a maximum of 430.09 mg/g, surpassing most activated carbon (AC) catalysts. EPR testing revealed that the loading of Cu-Fe oxide can activate oxygen to form superoxide radicals ( O 2 - ·), thereby promoting the catalytic oxidation of H 2 S. XPS testing revealed that upon loading of Cu-Fe oxide, the formation of FeOOH can facilitate the catalytic oxidation of H 2 S to sulfur (S) through a chain reaction. Combining EPR and XPS analyses, Na 2 CO 3 modification modulates the content of O 2 - ·, directing the formation of S and then significantly improving the catalyst’s desulfurization efficiency. Furthermore, CO 2 -TPD testing revealed that Na 2 CO 3 modification promotes the ionization of H 2 S to HS - , thereby enhancing the catalyst’s desulfurization performance. Based on the distribution of sulfur species in used catalysts, and the results of characterizations, a possible desulfurization mechanism of CuFeNaAC-X has been proposed.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Xuechang Ren,Ju An,Suying Ding,Zhenyu Yang,Miao Tian,Ning Fu
MoS 2 /MIL-88A (Fe) composite catalyst was prepared by in-situ formation method. The material was characterized by SEM, TEM, XRD and XPS, and the Rhodamine B(RhB) was activated and degraded by persulfate (PMS). The results showed that M-10/M 1:2 had the best degradation effect on RhB, the rate constant was 0.66420 min −1 , and the degradation rate could reach 1.89–14 times that of other doped composite catalysts. The SEM results showed that M − 10 had the least sulfur content, fewer MoS 2 flower layers and more exposed Mo 4+ atoms, which improved the electron transfer efficiency and accelerated the degradation reaction. The XPS spectra before and after M-10/M 1:2 reaction showed that the REDOX reaction of Fe 3+ /Fe 2+ and Mo 4+ /Mo 6+ on the catalyst surface played an important role in the activation of PMS. The results of free radical capture experiment and ESR test showed that the main active substances in M-10/M 1:2 /PMS reaction system were SO 4 •− , 1 O 2 , •O 2 − , and •OH, which only played a role in the degradation of RhB. Finally, based on the ESR results of M-10/M 1:2 /PMS system and the changes of Fe and Mo elements in XPS characterization before and after the reaction, the degradation mechanism of M-10/M 1:2 /PMS system was proposed.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 9
·096518
·
IF 4.386
Xiangyu Meng,Zhihuan Wang,Guoliang Yu,Xinbin Wang,Yingjie Chen,Liyan Yu,Lifeng Dong
Rational design of surface plasmon-enhanced electrocatalysts can effectively integrate solar energy into fuel cells. Herein, iron and nitrogen codoped carbon (Fe/NC) nanoparticles synthesized with microemulsion are used to absorb and photo-reduce Ag ions in solutions to form Ag nanoparticles on Fe/NC (Ag-Fe/NC). Different Ag-Fe/NC materials are prepared by adjusting the concentration of AgNO3 solution. Among them, Ag-Fe/NC obtained with 0.5 mg ml−1 AgNO3 solution shows the highest oxygen reduction reaction (ORR) catalytic performance and light-enhanced ORR characteristics, even better than commercial Pt/C. Besides, Ag-Fe/NC displays excellent long-term stability and high methanol resistance for ORR performances in alkaline medium. Therefore, this study will provide a new method for integrating light to recover Ag ions in solutions and improve electrocatalytic properties.
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Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 11
·1-10
·
IF 4.3
Liang Haoting,Zhao Qiao,Liu Shengkun,Wei Chongyang,Wang Yidan,Wang Yue,Huang Shouying,Ma Xinbin
The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO 2 into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO 2 hydrogenation activity and inhibited CH 4 formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H 2 temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO 2 and the identification of reaction intermediates were analyzed using CO 2 -temperature programed desorption and in situ Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO 2 adsorption and the formation of HCOO* species, ultimately leading to increased CO 2 conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.
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MATERIALS LETTERS
·
2019
·
IF 3.019
Rui Wang,Cong Tang,Ming Zhang,Zhecun Guan,Huanwen Wang,Yansheng Gong,Beibei He
TiO 2 is recognized as a promising anode material for sodium-ion batteries (SIBs) due to its low-cost and high structural stability, but it suffers from intrinsically poor electrical conductivity and low electrochemical activity at high rates. Herein, an in-situ Fe-doping strategy is designed to increase sodium-ion storage performance of TiO 2 /carbon nanofibers by a simple electrospinning method. The combination of Fe-doping with one-dimensional carbon structure could enable fast electron and Na + ion transport of TiO 2 . As a result, the Fe-TiO 2 /carbon nanofiber electrode exhibits high specific capacity (283 mAh g −1 at 0.5 C), excellent rate capability (140 mAh g −1 at 30 C) and long cycling stability (98% retention after 3000 cycles), which is obviously superior to pure TiO 2 /carbon nanofiber and other TiO 2 -based anodes reported in the literatures. These results indicates the powerful effect of in-situ Fe-doping for enhancing the Na-storage property of TiO 2 .
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 8
·10734-10749
·
IF 2.478
Kabir Fazal,Murtaza Adil,Saeed Azhar,Ghani Awais,Ali Anwar,Khan Saleh,Kaili Li,Qizhong Zhao,Kang Yao Kang,Yang Sen
Room temperature ferromagnetism with the doping of magnetic ions in the semiconducting host is the fundamental criterion for the potential use of spintronics material. In the present study, pure and (Fe, Tb) co-doped ZnO nanoparticles were well-prepared via the co-precipitation method, and corresponding microstructural, magnetic, and optical properties were investigated. The formation of Wurtzite hexagonal crystal structure of pure and doped ZnO was confirmed by X-ray diffraction (XRD) studies. No secondary phase was detected in all samples. Microstructural analysis reveals the spherical morphology of synthesized particles with the average size in the nanometer range. Fourier transforms infrared spectra show Tb–Zn–O stretching at 550 cm −1 . Optical absorption spectra show that the bandgap decreases and the absorption band slightly shift toward the visible region with increasing Tb doping, which may be due to the transfer of charge between the Tb ion 4f level and ZnO valance band. The photoluminescence (PL) spectrum exhibits a strong emission in the visible range, and PL emission intensity decreases with increasing Tb concentration and is anticipated to be due to the low recombination rate of electron–hole pairs. Most importantly, the room temperature ferromagnetism (RTFM) was observed in the doped ZnO nanoparticles, ascribed to the bound magnetic polaron (BMP) mechanism. The optical and magnetic outcome demonstrates that prepared (Fe, Tb) co-doped ZnO based dilute magnetic semiconducting (DMS) material are potential candidates for spintronics applications.
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Small
·
2023
·Vol. 19
·期 23
·2300106
·
IF 13.3
Ziqin Liu,Xin Dong,Jing Wen,Pu Hu,Chaoqun Shang
The high reactivity of Li metal and the inhomogeneous Li deposition leads to the formation of Li dendrites and “dead” Li, which impedes the performance of Li metal batteries (LMBs) with high energy density. The regulating and guiding the Li dendrite nucleation is a desirable tactic to realize concentrated distribution of Li dendrites instead of completely inhibiting dendrite formation. Here, a Fe-Co-based Prussian blue analog with hollow and open framework (H-PBA) is employed to modify the commercial polypropylene separator (PP@H-PBA). This functional PP@H-PBA can guide the lithium dendrite growth to form uniform lithium deposition and activate the inactive Li. In details, the H-PBA with macroporous structure and open framework can induce the growth of lithium dendrites via space confinement, while the positive Fe/Co-sites lowered by polar cyanide (−CN) of PBA can reactivate the inactive Li. Thus, the Li|PP@H-PBA|Li symmetric cells exhibit long-term stability at 1 mA cm −2 for 1 mAh cm −2 over 500 h. And the Li-S batteries with PP@H-PBA deliver favorable cycling performance at 500 mA g −1 for 200 cycles.
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Energy Storage Materials
·
2020
·
IF 16.28
Qiulong Li,Qichong Zhang,Chenglong Liu,Wenbin Gong,Zhengyu Zhou,Ping Man,Jiabin Guo,Bing He,Kai Zhang,Weibang Lu,Yagang Yao
The rational design and construction of high-performance fiber-shaped NiCo//Fe batteries is of great importance for the development of portable and wearable electronics . Electrode materials with all hierarchical core-shell heterostructures have great potential for use in high-performance NiCo//Fe batteries as a result of their good conductivity, high mass loading, and short ion-diffusion paths. Herein is proposed a novel freestanding core-shell positive and negative electrode materials developed by depositing NiCoP nanosheets on nanoflake arrays (NiCoP@NiCoP NFAs) and Fe 2 O 3 nanoneedles on TiN nanowire arrays (TiN@Fe 2 O 3 NWAs) directly grown on carbon nanotube fibers (CNTFs). The fabricated NiCoP@NiCoP NFAs/CNTF was validated to be an ultrahigh capacity cathode (1.07 mAh cm −2 at 2 mA cm −2 ), matching well with the similarly constructed TiN@Fe 2 O 3 NWAs/CNTF anode (0.92 mAh cm −2 at 2 mA cm −2 ). These electrodes were successfully developed into a high-performance NiCo//Fe battery that exhibited an extraordinary capacity of 0.77 mAh cm −2 and a remarkable energy density of 265.2 mWh cm −3 . The flexible battery demonstrated an excellent cycling lifespan with 89.4% capacity retention after 4000 cycles. This pioneering study describes a powerful strategy for the rational construction of high-performance electrode materials with hierarchical core-shell heterostructures and constitutes a novel approach for the development of new-generation wearable aqueous rechargeable batteries.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Dongxu Zhang,Yanhong Liu,Baodong Mao,Haitao Li,Tianyao Jiang,Dongqi Zhang,Weixuan Dong,Weidong Shi
Electrochemical nitrogen reduction reaction (NRR) is considered as one of the most promising methods for NH3 synthesis under room temperature and ambient pressure. A grand challenge of NRR is the development of efficient electrocatalysts, for which the delicate nanostructuring of catalysts plays an important role. Herein, a series of Fe-doped Cu2–xS quantum dots (QDs) are synthesized with multiple active sites and interface engineering, in which the double-phase heterostructure plays a key role for boosting NRR activity. The yield of NH3 was obviously improved with the increase of Fe content from 0 to 3% but started to decrease with Fe from 3 to 9%. The optimized Fe3%–Cu2–xS QDs show an outstanding NH3 yield of 26.4 μg h–1 mg–1cat at −0.7 V (vs the reversible hydrogen electrode), which is 5 times higher than that of Cu2–xS QDs. More importantly, we observed that the highest NRR activity in Fe3%–Cu2–xS QDs was ascribed to the formation of an inherent double-phase heterostructure of Cu2–xS/Cu5FeS4, whereas the complete conversion to single-phase Cu5FeS4 with increased Fe doping (9%) resulted in the activity decrease. Further, N2 temperature-programmed desorption and electrochemical impedance spectra characterizations confirm the stronger chemical adsorption of N2 and faster charge transfer in the Cu2–xS/Cu5FeS4 QDs. A plausible mechanism was proposed for the double-phase Cu2–xS/Cu5FeS4 heterostructure, where the interface provides efficient charge transfer and more active sites of Cu, Fe, and S for the synergetic adsorption and activation of N2. Our work provides a simple strategy for the design of NRR electrocatalysts, which may also bring new inspiration for the preparation of the inherent double-phase heterostructure within other doped QDs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Mang Ma,Anuj Kumar,Danni Wang,Yiyan Wang,Yin Jia,Ying Zhang,Guoxin Zhang,Zifeng Yan,Xiaoming Sun
Atomically dispersed metal-nitrogen-carbon complexes on carbon supports have drawn tremendous attention in the electrocatalysis fields. Herein, we managed the synthesis of atomically dispersed binary Ni x Fe 100-x -NC (x = 0–100) materials with tunable Ni/Fe ratios and investigated their underneath synergy effects for the enhancement of oxygen reduction (ORR) and oxygen evolution reactions (OER). EXAFS revealed the abundant presence of Ni(N 3 )-Fe(N 3 )-C n moieties in Ni 66 Fe 34 -NC sample. XPS fine scans indicated deep synergy of dual-site Ni/Fe that favored more charge localized over Ni/Fe sites. Electrochemical measurments showed that the Ni 66 Fe 34 -NC delivered a very high ORR half-wave potential ( E 1/2 ) of 0.85 V and a low OER overpotential of 467 mV at ∼10 mA cm −2 ( E j=10). The Fe site with Ni neighboring, as suggested by DFT simulations and in-situ Raman, was the responsible site for both ORR and OER. Furthermore, the Ni 66 Fe 34 -NC-assembled Zn-air battery afforded large specific power density and extraordinary cycling stability.
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NANOTECHNOLOGY
·
2019
·Vol. 30
·期 30
·305402
·
IF 3.399
Tong Wu,Yaying Li,Yuntong Li,Jing Hong,Haiyang Wu,Jie Mao,Yuzhe Wu,Qipeng Cai,Conghui Yuan,Lizong Dai
Simultaneous introduction of both transition metal and other inorganic elements into the carbon matrix has attracted great attention in the fabrication of carbon materials with high electrochemical properties. Herein, rational design of ligand-iron coordinative supramolecular precursors is achieved for the fabrication of Fe-N/C catalysts, which possess high oxygen reduction reaction (ORR) performance. A series of precursors are prepared by a simple coordination reaction between a three armed catechol monomer and iron ions. Particular interest is focused on tuning the doping species, surface area and morphology of the Fe-N/C catalysts through a simple selection of iron resources. We show that an Fe-N/C catalyst derived from Fe2(SO4)3 at a carbonization temperature of 800 °C, has the optimized ORR performance with an onset potential of 0.930 V and half-wave potential of 0.801 V. Detailed investigation indicates that the synergistic effect among doping elements of nitrogen and sulfur and the unique carbon structure determines the performance of the Fe-N/C catalysts. Our findings may be of significance for the fabrication of doped carbon materials using coordinative supramolecular polymers as precursors.
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CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Hang Cui,Xiaogang Gu,Shuguang Lu,Xiaori Fu,Xiang Zhang,George Y. Fu,Zhaofu Qiu,Qian Sui
Ethylbenzene (EB) degradation performance in (S,S)-ethylenediamine-N,N-disuccinic acid (EDDS) chelated Fe(III) activated sodium percarbonate (SPC) system was investigated in this study. The effects of various factors, such as the dosages of SPC and Fe(III), molar ratio of EDDS/Fe(III), anions (Cl − , HCO 3 − , SO 4 2− , and NO 3 − ) concentration, natural organic matters (NOM), and initial solution pH were evaluated. The results showed that the addition of EDDS remarkably improved the EB removal in Fe(III)/SPC system. Both HCO 3 − anions and NOM had significantly inhibitive effect, while the influence of SO 4 2− , Cl − and NO 3 − could be negligible on EB degradation. The EB removal was inhibited at extremely low and high initial solution pH. Moreover, the results of free radical probe tests, scavenger tests and electron paramagnetic resonance (EPR) detection indicated that OH was the predominant species responsible for EB degradation even though both OH and O 2 − were generated in the SPC/EDDS–Fe(III) system. The oxidation products were analyzed and possible EB degradation pathways were proposed. In conclusion, this study provides an important insight into the application of SPC/EDDS–Fe(III) system in the removal of EB contaminant, especially for in situ remediation of BTEX-contaminated groundwater.
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