COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
YuXin Zhao,Jiaxian Liu,Tong Zhang,FangXun Liu,Man Zheng,Kun Shi,JinPeng Liu,Yufan Zhang,Huan Wang
The exploration of an inexpensive catalyst with effective oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) activities to replace precious metal electrocatalysts has been of great interest in recent years. In this paper, CNT@Co-Fe/FePc composites were synthesized with high efficiency using a self-assembly strategy. In the synthesis process, carbon nanotubes (CNTs) were synthesized as the base material using crab shells as templates and honey as the carbon and nitrogen source. CoFe alloy nanoparticles derived from CoFe-based prussian blue analogs were self-assembled and anchored on CNTs, and then iron phthalocyanine with Fe-N 4 portion was coupled with CNTs by π-π stacking. Finally formed a homogeneous and stable composite material. The self-assembly method is simple and efficient to achieve good metal loading. The prepared CNT@Co 2 -Fe 1 /FePc exhibits excellent catalytic performance and stability for OER and ORR in alkaline electrolyte . The overpotential at 10 mA cm −2 of CNT@Co 2 -Fe 1 /FePc for OER is 343 mV with a very small Tafel slope of 43.59 mV dec −1 . CNT@Co 2 -Fe 1 /FePc has high methanol tolerance and persistence for ORR. This work provides a strategy for the construction of transition metal-carbon composite electrocatalytic materials with excellent catalytic performance and stability for OER and ORR reactions.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 15
·9761-9770
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IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Lihui Xiao,Lei Du,Xiangyu Lu,Ruopeng Li,Jinqiu Zhang,Maozhong An
Extensive efforts have been devoted to active site designing for non-precious metal electrocatalysts; however, the porous structure engineering has been less emphasized, particularly for catalysts for gas diffusion electrodes, e.g., the cathode (oxygen reduction reaction, ORR) of Zn–air batteries. The desired porous structure is not only important for exposing high-density active sites but also beneficial for boosting mass transfer. Here, a dual-template strategy is proposed for constructing hierarchically porous structural Fe–N–C catalysts with dense active Fe–Nx moieties for the cathode of Zn–air batteries. The dual ZnCl2 and MgO hard templates jointly promote the formation of hierarchically interconnected carbon networks. The experimental results indicated both significantly improved active site accessibility and mass transfer, reasonably leading to enhanced ORR activity in conventional three-electrode cells. Particularly, it is deduced that the microporous structure is beneficial for dense active Fe–Nx moieties, while the ultra-macroporous structure is conducive to mass transfer during the ORR process. We further applied this dual-template-mediated catalyst in a real-world liquid Zn–air battery, which presents a high open-circuit voltage of 1.48 V and a remarkable energy density of 952.8 W h kgZn−1. Such robust battery performance is among the best compared with reported Zn–air batteries using non-precious metal catalysts. Particularly, a peak power density of 116.8 mW cm−2 is achieved in an all-solid-state Zn–air battery.
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ENVIRONMENTAL POLLUTION
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2021
·
IF 8.071
Anqi Huang,Dan Zhi,Yaoyu Zhou
A graphite felt (GF) cathode was firstly modified by Fe–Mn binary oxide (FMBO), active carbon (AC), carbon black (CB), and polytetrafluoroethylene (PTFE), which exhibits satisfactory ciprofloxacin (CIP) removal efficiency at neutral pH value in electro-Fenton (EF) system. Morphological data showed that modified cathodes have larger surface area and volume pore as well as more active sites. And electrochemical properties have proved stronger current response after modification. In compassion to the unmodified GF, the FMBO/AC/CB modified GF (FMBO-GF) has wider pH range and higher CIP removal efficiency due to its unique nanoparticles structure. The CIP removal efficiency achieved 95.40% in 30 min, and the removal efficiency of total organic carbon (TOC) achieved 93.77% in 2 h when conditions were optimal (25 mg/L initial CIP concentration, 2 mA/cm 2 current density, FMBO/AC: CB: PTFE of 1:1:5, and 7 initial pH value) in this study. The results of great degradation and mineralization of CIP in this study indicate that the FMBO-GF cathode has huge potential on antibiotics removals in neutral environment.
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高影响因子
ANALYST
·
2021
·Vol. 146
·期 14
·4557-4565
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IF 4.616
Xiangyu Ma,Kun Qian,Onome Ejeromedoghene,Martha Kandawa-Schulz,Wei Song,Yihong Wang
Taking a composite of a nanomaterial and a signal molecule as a substrate material can provide a label-free electrochemical platform. Besides, the nanomaterial with a high catalytic activity towards the signal molecule can improve the sensitivity of the platform. Herein, a thionine functionalized Fe–N–C nanocomposite was employed as the substrate. Firstly, the electrocatalytic activity of Fe–N–C towards the electroreduction of thionine was explored. Then, an immobilization-free and label-free electrochemical platform for the determination of microRNA-21 based on Fe–N–C–thionine/Fe3O4@AuNPs was constructed. A magnetic glassy carbon electrode (MGCE) was used to keep the magnetic Fe–N–C–thionine/Fe3O4@AuNPs modified onto the surface of the MGCE. Fe–N–C and Fe3O4 nanoparticles can co-catalyze the electroreduction of thionine and a strong electrochemical reduction signal of thionine could be realized in the differential pulse voltammetry (DPV) test. Also, a catalytic hairpin assembly (CHA) reaction was utilized to enhance the sensitivity of the developed electrochemical biosensor. Besides, the developed biosensor shows excellent specificity and reproducibility in the test of human serum samples, indicating its wide application prospects in the early-stage diagnosis of tumors.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 14
·6424-6431
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IF 3.591
Jingjing Ju,Jiajia Lu,Xiaoyue Shi,Hongwei Zhu,Han-Pu Liang
Exploring efficient electrocatalysts with low production costs for the oxygen evolution reaction (OER) is significant for sustainable and scalable production of hydrogen through water electrolysis, while it still remains a challenge. Herein, mesoporous Fe-doped Co–Ni oxide (CoNiFeOx) nanosheets grown on nickel foam are synthesized by a facile two-step strategy (a combination of hydrothermal and post-annealing). Benefiting from the mesoporous nanosheet structure, endowing the catalysts with a high specific surface area (222.6 m2 g−1) and more active sites, and the optimized electronic structure due to the incorporation of Fe, the as-synthesized mesoporous CoNiFeOx nanosheets as a binder-free electrode exhibits remarkable OER activity with an overpotential of only 221 mV at a current density of 10 mA cm−2 and a small Tafel slope of 43.8 mV dec−1 in 1 M KOH solution. Besides, it displays excellent stability for over 250 h and no obvious activity decline is measured after the long-term stability test. Our strategy will provide a potential route to develop low-cost and high-performance electrocatalysts for the OER.
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RSC Advances
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2021
·Vol. 11
·期 43
·26502-26508
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IF 3.361
Meirong Fu,Mingqiang Li,Yingying Zhao,Yunxiang Bai,Xingzhong Fang,Xiaolong Kang,Min Yang,Yanping Wei,Xia Xu
Precious metal nanometric catalysts are widely used in the removal of harmful substances. In the process of synthesis and catalytic reaction, it is particularly important to study green and simple synthesis methods and high catalytic efficiency. In this paper, a green one-step method was used to synthesize the Fe(OH)3/Fe2O3@Au composite catalyst, in which Au was single atom-dispersed. The removal of 4-nitrophenol (4-NP), a typical dangerous chemical widely existing in factory waste gas, waste water and automobile exhaust gas, was catalysed by Fe(OH)3/Fe2O3@Au. The catalytic performance of Fe(OH)3/Fe2O3@Au with different synthesis conditions (different amounts of MES, NaBH4, FeSO4, Au and Pt) on the 4-NP reduction reaction were systematically studied. Finally, the stability and recyclability of Fe(OH)3/Fe2O3@Au composite nanocatalyst were investigated thoroughly.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Chan Zhou,Lei Zhu,Lin Deng,Haojie Zhang,Hanxuan Zeng,Zhou Shi
For improving the catalytic activity and recyclability of CuS in Fenton-like reaction processes, novel sulfur vacancies-enriched CuS@MIL-101(Fe) was constructed, characterized, and examined as heterogeneous catalysts for activating peroxymonosulfate (PMS) to degrade coumarin (COU). Thanks to the redox pairs of Fe 3+ /Fe 2+ , Cu + /Cu 2+ , S 2− /S 2 2− /S 0 /sulfate species, copper-iron synergistic effect and sulfur vacancies, the CuS@MIL-101(Fe) realized a complete removal of COU (30 μM) in 10 min with reaction rate constant of 0.577 min −1 , which was 11.1 and 17.0 times of CuS and MIL-101(Fe), respectively. The effect of various experimental conditions (i.e., initial pH, CuS@MIL-101(Fe) dosage, PMS concentration, and background anions) on COU degradation was discussed, and the stability and versatility of CuS@MIL-101(Fe) was studied as well. Radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy identified • OH and 1 O 2 as the main reactive oxygen species (ROS). Finally, the possible mechanism of higher COU degradation efficiency in the CuS@MIL-101(Fe) activated PMS system and the degradation pathways were also deeply explored. Consequently, this work provided a novel insight into construction of sulfur vacancies-enriched heterogeneous catalysts for efficiently activating PMS for refractory organic pollutants elimination.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Miao,Ying Liu,Dandan Wang,Ningjie Du,Ziwei Ye,Yang Hou,Shun Mao,Kostya (Ken) Ostrikov
Transition-metal and nitrogen co-doped carbon-based catalysts receive much attention in peroxymonosulfate (PMS) activation. However, the contribution of doped metal and the kinetic mechanisms of the emerging nonradical pathways especially enabled by reactive singlet oxygen species remain unclear. Herein, we report Fe-N-co-doped carbon-based catalysts (FeCNx) for peroxymonosulfate activation. The catalysts achieve fast removal of a broad spectrum of organic pollutants in a wide pH range without the common Fe leaching. Both catalyst surface-activated PMS complex (catalyst-PMS*), surface-bound radicals, and singlet oxygen are identified. The new mechanism is enabled by the Fe-Nx single-atomic-site that enhances the adsorption of PMS and facilitates the formation of catalyst-PMS*. The formation route of singlet oxygen species is elucidated for the first time for Fe, N-co-doped carbon-based catalysts with density functional theory simulation. This study reveals the intrinsic role of Fe-Nx site in catalysts and provides new insights into the origin and kinetics of non-radical pathways for peroxymonosulfate activation.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Yun Pei,Junxian Qin,Jun Wang,Yun Hu
A series of Fe-based metal organic framework derived materials were prepared by thermal treating MIL-100(Fe) in nitrogen atmosphere for adsorption removal of oxygenated volatile organic compounds (OVOCs) such as methanol, formaldehyde and acetone under dynamic conditions. The experimental results showed that the partially carbonized M-350 material obtained by calcining MIL-100(Fe) at 350 °C exhibited the best adsorption performance and high stability. The breakthrough adsorption capacity of M-350 for methanol was 61.5% higher than that of pure MIL-100 (Fe), and it was 24.7, 6.5 and 2.6 times higher than that of commercial activated carbon, ZSM-5 and SAPO-34 adsorbents, respectively. The excellent adsorption performance was attributed to the exposure of abundant coordinatively unsaturated iron metal sites acting as Lewis acid sites through high temperature calcination, which had a strong affinity for OVOCs. Meanwhile, a hierarchical porous structure and high specific surface area further promoted the adsorption. This work provides new insights into the further development of metal organic frameworks based functional materials for VOCs removal and purification.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Katam Srinivas,Yuanfu Chen,Bin Wang,Bo Yu,Yingjiong Lu,Zhe Su,Wanli Zhang,Dongxu Yang
Strategic design and fabrication of a highly efficient and cost-effective bifunctional electrocatalyst is of great significance in water electrolysis in order to produce sustainable hydrogen fuel in a large scale. However, it is still challenging to develop a stable, inexpensive, and efficient bifunctional electrocatalyst that can overcome the sluggish oxygen evolution kinetics in water electrolysis. To address the aforementioned concerns, a metal–organic framework-derived Fe-doped Ni3Fe/NiFe2O4 heterostructural nanoparticle-embedded carbon nanotube (CNT) matrix (Fe(0.2)/Ni-M@C-400-2h) is synthesized via a facile hydrothermal reaction and subsequent carbonization of an earth-abundant Ni/Fe/C precursor. With a novel porous nanoarchitecture fabricated by a Ni3Fe/NiFe2O4 heterostructure on a highly conductive CNT matrix, this catalyst exhibits exceptional bifunctional activity during water electrolysis over the Ni/Fe-based electrocatalysts reported recently. It delivers a low overpotential of 250 mV to achieve a current density of 10 mA/cm2 with a small Tafel slope of 43.4 mV/dec for oxygen evolution reaction. It requires a low overpotential of 128 mV (η10) for hydrogen evolution reaction and displays a low overpotential of 1.62 V (η10) for overall water splitting. This study introduces a facile and straightforward synthesis strategy to develop transition metal-based nanoarchitectures with high performance and durability for overall water-splitting catalysis.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Junlei Zhang,Wei Zhao,Zhi Li,Gang Lu,Mingshan Zhu
Advanced oxidation processes involving the visible-light-assisted peroxymonosulfate (PMS) are emerging as promising approaches for treating antibiotic pollutants. Here, Fe(II)/V(IV) self-doped FeVO 4 nanobelts were synthesized and employed to build a visible-light-assisted PMS activation system for degrading antibiotic sulfamethoxazole (SMX). Compared with PMS/FeVO 4 , PMS/Visible light (VL), or PMS system, the PMS/FeVO 4 /VL system showed 3.9, 14.0, or 14.1 times improved for the removal of SMX, respectively. The reason behind this is the organic combination of the VL photocatalysis and transformation of Fe(II)/V(IV) to Fe(III)/V(V) over FeVO 4 , namely when photocatalytic behavior over FeVO 4 can produce electrons (e - ) and holes (h + ) to activate PMS or directly degrade SMX, the transformation of Fe(II)/V(IV) to Fe(III)/V(V) will also happen to donate some e - for PMS activation simultaneously. Such a system can also effectively remove SMX from actual water bodies such as medicine wastewater, river water, tap water, and rainwater. This work not only provides an effective system for treating SMX polluted wastewater, but also gives some new insights to understanding the mechanism involving Fe-based binary metal oxide activating peroxymonosulfate.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Ruzhen Xie,Yanbin Jiang,Andac Armutlulu,Ziye Shen,Bo Lai,Hui Wang
In this work, cost-effective, magnetic carbon-supported Fe@Ti composite (Fe@Ti/Cs) with abundant active sites was synthesized by one-step carbothermal reduction of ilmenite with the assistance of microwave oven and utilized as a highly efficient persulfate (PS) activator for the wastewater purification. The coexistence of Fe 0/2+/3+ , Ti 3+/4+ and oxygen vacancies on Fe@Ti/Cs was found to favor for the electron transfer to PS, which facilitate the generation of reactive oxygen species (ROS). Catalytic experiment results showed that the Fe@Ti/C-4 produced from ilmenite/carbon with a mass ratio of 4:1 exhibited the best catalytic activation performance towards PS for the degradation of Rhodamine B (RhB). Usage of merely 0.12 g/L Fe@Ti/C-4 enabled the removal of 94.01% RhB (200 mg/L) within 30 min in the PS containing system, significantly outperforming ilmenite + PS (29.29%) and carbon + PS (49.91%) systems tested under the same conditions. The physico-chemical properties of the produced Fe@Ti/Cs before and after the reaction were carefully characterized. Radical scavenging experiments and electron paramagnetic resonance (EPR) analysis were carried out to better understand the underlying mechanism. The results indicate that oxygen vacancies in Fe@Ti/C-4 promoted the electron transfer and participated in the transition metal redox cycle to generate ROS in the PS-containing system, which was highly efficient for degrading RhB into small molecules and finally enabling mineralization. This work offers a new perspective for designing highly efficient and stable PS activators with long life derived from natural ore for environmental remediation.
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