Highly regenerable carbon-Fe3O4 core–satellite nanospheres as oxygen reduction electrocatalyst and magnetic adsorbent

2017 ◽  
Vol 246 ◽  
pp. 357-362 ◽  
Author(s):  
Wenqiang Zhou ◽  
Minmin Liu ◽  
Chao Cai ◽  
Haijun Zhou ◽  
Rui Liu
Keyword(s):  
Oxygen Reduction ◽  
Magnetic Adsorbent ◽  
Fe3o4 Core

Rational prediction of multifunctional bilayer single atom catalysts for the hydrogen evolution, oxygen evolution and oxygen reduction reactions

Nanoscale ◽  
2020 ◽  
Vol 12 (39) ◽  
pp. 20413-20424
Author(s):  
Riming Hu ◽  
Yongcheng Li ◽  
Fuhe Wang ◽  
Jiaxiang Shang
Keyword(s):  
Oxygen Reduction ◽  
Hydrogen Evolution ◽  
Oxygen Evolution ◽  
Single Atom ◽  
Reduction Reactions ◽  
Oxygen Reduction Reactions

Bilayer single atom catalysts can serve as promising multifunctional electrocatalysts for the HER, ORR, and OER.

A Pyridinic Fe-N4 Macrocycle Effectively Models the Active Sites in Fe/N-Doped Carbon Electrocatalysts

2020 ◽  
Author(s):  
Travis Marshall-Roth ◽  
Nicole J. Libretto ◽  
Alexandra T. Wrobel ◽  
Kevin Anderton ◽  
Nathan D. Ricke ◽  
...  
Keyword(s):  
Oxygen Reduction ◽  
Active Sites ◽  
Catalytic Properties ◽  
Reduction Reaction ◽  
Iron Phthalocyanine ◽  
Electrochemical Studies ◽  
Onset Potential ◽  
Nitrogen Doped Carbon ◽  
Iron Active Sites

Iron- and nitrogen-doped carbon (Fe-N-C) materials are leading candidates to replace platinum in fuel cells, but their active site structures are poorly understood. A leading postulate is that iron active sites in this class of materials exist in an Fe-N<sub>4</sub> pyridinic ligation environment. Yet, molecular Fe-based catalysts for the oxygen reduction reaction (ORR) generally feature pyrrolic coordination and pyridinic Fe-N<sub>4</sub> catalysts are, to the best of our knowledge, non-existent. We report the synthesis and characterization of a molecular pyridinic hexaazacyclophane macrocycle, (phen<sub>2</sub>N<sub>2</sub>)Fe, and compare its spectroscopic, electrochemical, and catalytic properties for oxygen reduction to a prototypical Fe-N-C material, as well as iron phthalocyanine, (Pc)Fe, and iron octaethylporphyrin, (OEP)Fe, prototypical pyrrolic iron macrocycles. N 1s XPS signatures for coordinated N atoms in (phen<sub>2</sub>N<sub>2</sub>)Fe are positively shifted relative to (Pc)Fe and (OEP)Fe, and overlay with those of Fe-N-C. Likewise, spectroscopic XAS signatures of (phen<sub>2</sub>N<sub>2</sub>)Fe are distinct from those of both (Pc)Fe and (OEP)Fe, and are remarkably similar to those of Fe-N-C with compressed Fe–N bond lengths of 1.97 Å in (phen<sub>2</sub>N<sub>2</sub>)Fe that are close to the average 1.94 Å length in Fe-N-C. Electrochemical studies establish that both (Pc)Fe and (phen<sub>2</sub>N<sub>2</sub>)Fe have relatively high Fe(III/II) potentials at ~0.6 V, ~300 mV positive of (OEP)Fe. The ORR onset potential is found to directly correlate with the Fe(III/II) potential leading to a ~300 mV positive shift in the onset of ORR for (Pc)Fe and (phen<sub>2</sub>N<sub>2</sub>)Fe relative to (OEP)Fe. Consequently, the ORR onset for (phen<sub>2</sub>N<sub>2</sub>)Fe and (Pc)Fe is within 150 mV of Fe-N-C. Unlike (OEP)Fe and (Pc)Fe, (phen<sub>2</sub>N<sub>2</sub>)Fe displays excellent selectivity for 4-electron ORR with <4% maximum H<sub>2</sub>O<sub>2</sub> production, comparable to Fe-N-C materials. The aggregate spectroscopic and electrochemical data establish (phen<sub>2</sub>N<sub>2</sub>)Fe as a pyridinic iron macrocycle that effectively models Fe-N-C active sites, thereby providing a rich molecular platform for understanding this important class of catalytic materials.<p><b></b></p>

Chitosan-based Magnetic Composites - Efficient Adsorbents for Removal of Pb(II) and Cu(II) from Aqueous Mono and Bicomponent Solutions

2018 ◽  
Vol 69 (9) ◽  
pp. 2323-2330 ◽  
Author(s):  
Daniela C. Culita ◽  
Claudia Maria Simonescu ◽  
Rodica Elena Patescu ◽  
Nicolae Stanica
Keyword(s):  
Aqueous Solutions ◽  
Metal Ions ◽  
Chemical Properties ◽  
Order Kinetic ◽  
Mass Ratio ◽  
Magnetic Adsorbent ◽  
Magnetic Composites ◽  
Initial Ph ◽  
Order Kinetic Model ◽  
Physical And Chemical

A series of three chitosan-based magnetic composites was prepared through a simple coprecipitation method. It was investigated the influence of mass ratio between chitosan and magnetite on the physical and chemical properties of the composites in order to establish the optimum conditions for obtaining a composite with good adsorption capacity for Pb(II) and Cu(II) from mono and bicomponent aqueous solutions. It was found that the microspheres prepared using mass ratio chitosan / magnetite 1.25/1, having a saturation magnetization of 15 emu g--1, are the best to be used as adsorbent for the metal ions. The influence of different parameters such as initial pH values, contact time, initial concentration of metal ions, on the adsorption of Pb(II) and Cu(II) onto the chitosan-based magnetic adsorbent was investigated in details. The adsorption process fits the pseudo-second-order kinetic model in both mono and bicomponent systems, and the maximum adsorption capacities calculated on the basis of the Langmuir model were 79.4 mg g--1 for Pb(II) and 48.5 mg g--1 for Cu(II) in monocomponent systems, while in bicomponent systems were 88.3 and 49.5 mg g--1, respectively. The results revealed that the as prepared chitosan-based magnetic adsorbent can be an effective and promising adsorbent for Pb(II) and Cu(II) from mono and bicomponent aqueous solutions.

N and S Co-doped Ordered Mesoporous Carbon: An Efficient Electrocatalyst for Oxygen Reduction Reaction in Microbial Fuel Cells

2020 ◽  
Vol 16 (4) ◽  
pp. 625-638
Author(s):  
Leila Samiee ◽  
Sedigheh Sadegh Hassani
Keyword(s):  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
Microbial Fuel Cells ◽  
Carbon Materials ◽  
Reduction Reaction ◽  
Carbon Substrate ◽  
Promising Candidate ◽  
X Ray ◽  
Carbon Framework ◽  
Co Doped

Background: Porous carbon materials are promising candidate supports for various applications. In a number of these applications, doping of the carbon framework with heteroatoms provides a facile route to readily tune the carbon properties. The oxygen reduction reaction (ORR), where the reaction can be catalyzed without precious metals is one of the common applications for the heteroatom-doped carbons. Therefore, heteroatom doped catalysts might have a promising potential as a cathode in Microbial fuel cells (MFCs). MFCs have a good potential to produce electricity from biological oxidization of wastes at the anode and chemical reduction at the cathode. To the best of our knowledge, no studies have been yet reported on utilizing Sulfur trioxide pyridine (STP) and CMK-3 for the preparation of (N and S) doped ordered porous carbon materials. The presence of highly ordered mesostructured and the synergistic effect of N and S atoms with specific structures enhance the oxygen adsorption due to improving the electrocatalytic activity. So the optimal catalyst, with significant stability and excellent tolerance of methanol crossover can be a promising candidate for even other storage and conversion devices. Methods: The physico-chemical properties of the prepared samples were determined by Small Angle X-ray Diffraction (SAXRD), N2 sorption-desorption, Transmission Electron Microscopy (TEM), Field Emission Scanning Electron Microscopy (FESEM) and X-ray Photoelectron Spectroscopy (XPS). The prepared samples were further applied for oxygen reduction reaction (ORR) and the optimal cathode was tested with the Microbial Fuel Cell (MFC) system. Furthermore, according to structural analysis, The HRTEM, and SAXRD results confirmed the formation of well-ordered hexagonal (p6mm) arrays of mesopores in the direction of (100). The EDS and XPS approved that N and S were successfully doped into the CMK-3 carbon framework. Results: Among all the studied CMK-3 based catalysts, the catalyst prepared by STP precursor and pyrolysis at 900°C exhibited the highest ORR activity with the onset potential of 1.02 V vs. RHE and 4 electron transfer number per oxygen molecule in 0.1 M KOH. The high catalyst durability and fuel-crossover tolerance led to stable performance of the optimal cathode after 5000 s operation, while the Pt/C cathode-based was considerably degraded. Finally, the MFC system with the optimal cathode displayed 43.9 mW·m-2 peak power density showing even reasonable performance in comparison to a Pt/C 20 wt.%.cathode. Conclusions: The results revealed that the synergistic effect of nitrogen and sulfur co-doped on the carbon substrate structure leads to improvement in catalytic activity. Also, it was clearly observed that the porous structure and order level of the carbon substrate could considerably change the ORR performance.

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