ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Shiwei Song,Jianbing Zang,Shuyu Zhou,Hongwei Gao,Xueqing Tian,Yungang Yuan,Wei Li,Yanhui Wang
The development of high-efficiency and economical bifunctional electrocatalysts in hydrogen evolution reactions (HER) and oxygen evolution reactions (OER) plays a key role in overall water splitting. In this study, a success was achieved in synthesizing the hollow nanospheres with amorphous nickel-iron phosphorusoxides nanoflakes layer grown on Ni-Fe foam (NiFe-PO x /NFF). Firstly, with the assistance of oxygen bubbles templates, the hollow spheres comprised of NiFe-OH nanosheets were produced through the in-situ chemical oxidation of NFF surface. After phosphorylation, crystalline NiFe-OH nanosheets were transformed into amorphous NiFe-PO x with plenty of defects and disorders, thus improving the density of active sites. The catalytic performance of NiFe-PO x /NFF was further improved by a combination of stable 3D hierarchical nanostructure, effective mass transport and charge transfer, as well as the electrochemical specific surface area expanded by fluffy featherlike nanoflakes. The self-supported electrode of NiFe-PO x /NFF exhibited outstanding catalytic property in the presence of alkaline electrolyte, including a small overpotential of 110 and 247 mV required to achieve 50 mA cm −2 for HER and OER in 1.0 M KOH aqueous solution, respectively. As a bifunctional electrocatalyst, NiFe-PO x /NFF could provide a low cell voltage of 1.52 V to reach 20 mV cm −2 under a two-electrode system as required for the occurrence of overall water electrolysis under alkaline medium, while showing extended durability under continuous electrolysis without degradation.
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高影响因子
Journal of Physical Chemistry C
·
2022
·
IF 4.177
Weifeng Su,Ning Yan,Fan Liu,Zigeng Liu,Guangqi Zhu,Songrui Wang,Xingjiang Liu,Wei Wang
The attenuation process of the oxygen reduction reaction (ORR) catalytic performance for Fe SAC@G catalysts under different discharging conditions, including KOH concentrations, solution temperatures, and discharging potentials, was investigated by electrochemical measurements. The ORR catalytic activity attenuation resulting from the change in KOH concentration and temperature becomes apparent in a negative discharging potential range and elevated discharging temperature. In addition, the more negative discharging potential significantly causes the ORR catalytic activity attenuation. Scanning electron microscopy (SEM), energy-dispersive spectrometry (EDS), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy analyses indicate that, with the prolongation of the discharge time, the nanocolumns of the as-prepared catalyst gradually dissolve, while a flowerlike discharge byproduct composed of elements C and N keeps growing on the surface of the catalyst. The weakest Fe–N bonds first break, resulting in the attenuation of the ORR catalytical performance. Then, the weak C–Cunit bonds connecting the structural units of the catalysts break, leading to the gradual collapse in the structure of the catalysts. The Fe–N4 coordination structure gradually transforms into Fe–N3, Fe–N2, and Fe–N coordination structures. Based on the analyses combined with the density functional theory (DFT) calculations of bond strength, a discharge attenuation mechanism of the structural collapse of the catalyst for the formation of the discharge byproduct with ring structure is proposed.
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高影响因子
Carbon Neutrality
·
2024
·Vol. 3
·期 1
·1-16
·
IF 0
Liu Xinghui,Naraginti Saraschandra,Zhang Fuchun,Sathishkumar Kuppusamy,Saxena Kuldeep K.,Guo Xiang
Environmental contamination by hexavalent chromium (Cr(VI)) and antibiotic drug residues pose significant challenges to public health and ecosystems. This study investigates the application of CoTiO 3 /BiVO 4 @MIL-Fe(53) (CT/BV@Fe-MOF) for the reduction of Cr(VI) and degradation of tetracycline (TCL) under visible light. After grafting an iron-based metal–organic framework MIL-Fe(53) on a modified CoTiO 3 /BiVO 4 composite, the photogenerated electrons could easily be transferred from CoTiO 3 to BiVO 4 /Fe-MOF species via interfacial charge transfer. UV–vis diffuse reflectance spectroscopy showed that charge carriers were formed in response to visible light absorption. The effect of different operating parameters, including catalyst load, pH, initial Cr(VI), and TCL concentration, was systematically evaluated during the photocatalytic process. The CT/BV@Fe-MOF composite exhibited 98.7% reduction efficiency in Cr(VI) (50 ppm) and 97.5% degradation efficiency towards TCL (30 ppm) within 90 min, resulting in a greater efficiency than the pristine CoTiO 3 , BiVO 4 , and Fe-MOF materials. The CT/BV@Fe-MOF composite displayed excellent stability over six cycles, highlighting its potential for practical applications. In addition, the plausible degradation pathway of TCL was evaluated using LC-ESI/MS analysis, while the TEST program was utilized to investigate the toxicity of the products generated during the degradation process.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yi Yang,Minyi Liu,Xintong You,Ying Li,Haowen Lin,J. Paul Chen
Treatment of organic wastewater is of great importance and can be carried out by catalysis technologies such as catalytic wet peroxide oxidation (CWPO). A novel bimetallic Fe-Cu-CNT catalyst was first developed by a facile hydrothermal method; Fe species (Fe (Ⅱ) and Fe (Ⅲ)) and Cu species (Cu (Ⅰ) and Cu (Ⅱ)) were used to fabricate the catalyst with the CNTs, which was stable during testing. Methylene blue (MB) was chosen as model compound for the study; the optimization for treatment by the Box-Behnken design indicated that a combination of low pH, high MB concentration and intermediate temperature led to better treatment performance. The CWPO reaction obeyed the 2 nd -order kinetic equation and the catalyst activity increased with an increase in the Cu content. The reaction induction period was shortened with decreasing Fe:Cu ratio. The cycling reaction between Fe 3+ /Fe 2+ and Cu 2+ /Cu + pairs generated a large number of oxidative radicals and improved the pollutant degradation efficiency. Finally, the reaction rate equation of CWPO over Fe-Cu-CNT was derived, and it was experimentally illustrated that hydroxyl radicals played a crucial role in the treatment. This study demonstrates that the optimized Fe-Cu-CNT has great potentials for treatment of organic wastewater with higher efficiency and lower cost.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Yanyan Wu,Zijuan Xie,Ying Li,Zhe Lv,Lingling Xu,Bo Wei
Developing efficient oxygen evolution reaction (OER) electrocatalysts with earth-abundant elements is very important for sustainable H 2 generation via electrochemical water splitting. Here we design a crystalline-amorphous Ni–Fe–Al hybrid phosphides nanosheet arrays grown on NiFe foam for efficient OER application. Dynamic surface reorganization of phosphides at anodic/cathodic polarizations is probed by in situ Raman spectroscopy . The reconstructed amorphous Ni(Fe)OOH species are determined as the active phases that facilitate the OER process. This unique electrode shows highly catalytic activity toward water oxidation , achieving the current densities of 10 and 100 mA cm −2 at 181 and 214 mV in 1 M KOH, respectively. Meanwhile, it also exhibits excellent stability at a large current density of 100 mA cm −2 for over 60 h. This work reveals the dynamic structural transformation of pre-catalyst in realistic conditions and highlights the important role of oxyhydroxides as real reactive species in OER process with high activity.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yi-long Yan,Qiao-Jun Fang,Jin-kong Pan,Jun Yang,Le-le Zhang,Wei Zhang,Gui-lin Zhuang,Xing Zhong,Sheng-wei Deng,Jian-guo Wang
The photocatalytic conversion of CO 2 into high-value chemicals is an ideal pathway to adjust the energy structure and reduce greenhouse gas emissions. In this work, we reported a facile synthetic strategy of new photocatalyst (ZnFe 2 O 4 /FeP-CTFs), where ZnFe 2 O 4 nanoparticles (NPs) was in situ growth on iron porphyrin covalent triazine-based frameworks (FeP-CTFs) via one-pot ionothermal method. Such strategy can effectively prevent ZnFe 2 O 4 from agglomerating and blocking the pore structure of CTFs . Notably, a series of experiments demonstrated that anchoring sites of FeP-CTFs can effectively promote the crystal-plane ratio of high catalytic performance, in the assistance of Ru(bpy) 3 2+ , promoting higher photocatalytic CO 2 reduction activity (178 μmol h −1 g −1 for CO) of the as-prepared ZnFe 2 O 4 /FeP-CTFs under visible light compared with pure ZnFe 2 O 4 , FeP-CTFs, and their physical mixtures. A combination of experimental measurements and density functional theory calculation reveals that the strong interactions between ZnFe 2 O 4 NPs and FeP-CTFs support can facilitate the charge separation of photogenerated carriers and thereby benefit to photocatalytic CO 2 reduction.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ping Zhang,Guohua Zhang,Yukun Liu,Yuxin Fan,Xinyue Shi,Yiming Dai,Shiwen Gong,Jingrong Hou,Jiwei Ma,Yunhui Huang,Renyuan Zhang
Fe/Mn-based layered oxide cathode is regarded as a competitive candidate for sodium-ion batteries (SIBs) because of its high theoretical capacity, earth abundance and low cost. However, its poor cycling stability still remains a major bottleneck. Herein, P 2/O3 biphasic Na 0.67 Fe 0.425 Mn 0.425 Cu 0.15 O 2 layered oxide is successfully synthesized via a sol–gel method. It is observed that Cu substitution can facilitate the conversion of P 2 to O3 phase, and the P 2/O3 composite structure can be obtained with an appropriate amount of Cu. Meanwhile, in-situ XRD reveals that constructing P 2/O3 composite structure can realize the highly reversible phase transition process of P 2/O3– P 2/ P 3–OP4/OP2 and decrease the lattice mismatch during Na + insertion/extraction. Consequently, the biphasic P 2/O3-Na 0.67 Fe 0.425 Mn 0.425 Cu 0.15 O 2 electrode exhibits 87.1 % capacity retention after 100 cycles at 1C, while the single phase P 2-Na 0.67 Fe 0.5 Mn 0.5 O 2 electrode has only 36.4 %. Therefore, the constructing biphasic structure is proved to be an effective strategy for designing high-performance Fe/Mn-based layered oxide cathodes.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 9
·094506
·
IF 4.386
Wendong Cheng,Shuai Hou,Fen Guo
The traditional electric furnace pyrolysis to produce heteroatom doped carbon faces the time-consuming issue due to the fixed size of furnace chamber and indirect heat transfer. Herein a fast Joule-heating pyrolysis method, viz., powering on the C, N, Fe-containing, conductive polyaniline precursor at fixed direct current (DC) voltage for a specific time, is put forward. The polyaniline precursor begins to decompose thermally when being powered with a DC voltage of 5.0 V upwards. In the pyrolysis products, Fe and N co-doping of carbon material leads to C–N bonding and C-Fe bonding in a certain way. The direct peroxide-peroxide fuel cell (DPPFC) with the optimal Fe, N codoped carbon material as anode and cathode can generate an open circuit voltage of 0.85 V and a peak power density of 29.7 mW cm−2 in ambient temperature, which is highly competitive compared with other DPPFCs with anode and/or cathode made of noble metals.
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高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Biao Li,Zhi-Ying Yan,Xiao-Na Liu,Chen Tang,Jun Zhou,Xia-Yuan Wu,Ping Wei,Hong-Hua Jia,Xiao-Yu Yong
Phenolic compounds are problematic byproducts generated from lignocellulose pretreatment . In this study, the feasibility degradation of syringic acid (SA), vanillic acid (VA), and 4-hydroxybenzoic acid (HBA) by Bio-Electro-Fenton (BEF) system with a novel Fe–Mn/graphite felt (Fe–Mn/GF) composite cathode were investigated. The nano-scale Fe–Mn multivalent composite catalyst with core shell structure distributed more evenly on GF surface to form a catalyst layer with higher oxygen reduction reaction performance. Accordingly, the maximum power density generated with Fe–Mn/GF cathode was 48.1% and 238.9% higher than Fe/GF and GF respectively, which further enhanced the in situ generation of H 2 O 2 due to the superiority of nano-scale core shell structure and synergistic effect of Fe and Mn species. The degradation efficiency of the three phenolic compounds in the BEF system could reached 100% after optimization of influencing parameters. Furthermore, a possible SA degradation pathway by BEF process in the present system was proposed based on the detected intermediates. These results demonstrated an efficient approach for the degradation of phenolic compounds derived from lignocellulose hydrolysates.
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高影响因子
Desalination and Water Treatment
·
2024
·
IF 1
Shuwang Zhang,Luping Zhang,Jialing Zhao,Wenying Yuan,Xing Fang,Qianqian Yu,Jing Cheng,Xinhong Qiu
ABSTRACT In this study, the degradation of bisphenol A (BPA) was enhanced by adding the reducing agent hydroxylamine hydrochloride (HAHC) into the layered double hydroxides (LDH)/peroxymono- sulfate (PMS) system to promote the conversion of ferric iron (Fe(III)) to Fe(II). The results showed that the degradation efficiency exceeded 90% within 120 min after the addition of HAHC. The effects of initial BPA, PMS concentration, and LDH dosage on BPA degradation efficiency were also evaluated in the HAHC/LDH/PMS system. In addition, the catalyst showed high catalytic activity over a wide pH range (2~10) within the experiment. Radical scavenging tests confirmed that the main reactive oxygen species were sulfate radical (SO 4 •– ), hydroxyl radical ( • OH) and superoxide radical (O 2 •– ) in the HAHC/LDH/PMS process. The reaction mechanism was also inferred by using various analytical techniques, including X-ray photoelectron spectroscopy, X-ray diffraction, electron paramagnetic resonance, scanning electron microscopy, transmission electron microscopy, liquid chromatography–mass spectrometry. This work provides a new strategy for the degradation of organic pollutants by the addition of HAHC to promote the activation of PMS by catalysts.
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高影响因子
ChemElectroChem
·
2017
·Vol. 5
·期 3
·471-477
·
IF 4.136
Jingchun Jia,Huijuan Yang,Genxiang Wang,Peng Huang,Pingwei Cai,Zhenhai Wen
Graphical All-round activity : Hybrids of Fe/Fe 3 C embedded in N-doped carbon nanotubes (Fe/Fe 3 C@NCNTs) are prepared by pyrolyzing mixtures of Fe 3 O 4 nanoparticles and dicyandiamide. Fe/Fe 3 C@NCNTs show a highly multifunctional catalytic activity for the oxygen evolution, oxygen reduction, and CO 2 reduction reactions. Hybrids of Fe/Fe 3 C embedded in N-doped carbon nanotubes (Fe/Fe 3 C@NCNTs) are prepared by pyrolyzing mixtures of Fe 3 O 4 nanoparticles and dicyandiamide. The systematic electrochemical study of Fe/Fe 3 C@NCNTs shows a decent catalytic activity toward the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). The sample of Fe/Fe 3 C@NCNTs at 750 °C exhibits a remarkably high activity with an onset potential of 1.47 V for the OER, and an onset potential of 0.96 V and half-wave potential 0.88 V for the ORR, which inspired us to set up a rechargeable Zn-air battery with such Fe/Fe 3 C@NCNT nanohybrids as the cathode materials, showing a maximum power density of 198 mW cm −2 and long-term stability after 500 cycles. We also demonstrate that Fe/Fe 3 C@NCNTs present favorable electrocatalytic activity towards the CO 2 reduction reaction (CO 2 RR) with a low onset potential and good selectivity. The major products are a mixture of H 2 and CO gases that can be used for methanol production in the Fischer−Tropsch process.
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Research
·
2023
·
IF 11
Changsheng Cao,Shenghua Zhou,Shouwei Zuo,Huabin Zhang,Bo Chen,Junheng Huang,Xin-Tao Wu,Qiang Xu,Qi-Long Zhu
Transition metal-based single-atom catalysts (TM-SACs) are promising alternatives to Au- and Ag-based electrocatalysts for CO production through CO2 reduction reaction. However, developing TM-SACs with high activity and selectivity at low overpotentials is challenging. Herein, a novel Fe-based SAC with Si doping (Fe-N-C-Si) was prepared, which shows a record-high electrocatalytic performance toward the CO2-to-CO conversion with exceptional current density (>350.0 mA cm−2) and ~100% Faradaic efficiency (FE) at the overpotential of <400 mV, far superior to the reported Fe-based SACs. Further assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO2 battery delivers an outstanding performance with a maximal power density of 2.44 mW cm−2 at an output voltage of 0.30 V, as well as high cycling stability and FE (>90%) for CO production. Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly accelerate the key pathway involving *CO intermediate desorption, inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO2RR performance. This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on single-atom sites to improve their electrocatalytic performance.
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高影响因子
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