Solution Plasma Synthesis of Nitrogen-Doped Carbon Nanoballs as Effective Metal-Free Electrocatalysts for Oxygen Reduction Reaction

2014 ◽  
Vol 1641 ◽  
Author(s):  
Gasidit Panomsuwan ◽  
Satoshi Chiba ◽  
Nagahiro Saito ◽  
Takahiro Ishizaki
Keyword(s):  
Thermal Annealing ◽  
Organic Liquid ◽  
Reduction Reaction ◽  
Limiting Current ◽  
Plasma Synthesis ◽  
Plasma Process ◽  
Onset Potential ◽  
Nitrogen Doped ◽  
Before And After ◽  
Nitrogen Doped Carbon

ABSTRACTNitrogen-doped carbons nanoballs were synthesized from an organic liquid precursor (a mixture of benzene and pyrazine) by solution plasma process. After synthesis, they were further annealed at 700 and 900 °C under N2 atmosphere. The nitrogen-doped carbon nanoballs before and after thermal annealing process exhibit a similar morphological feature, and their diameters are in the range between 20 and 40 nm. With higher annealing temperature, the graphitization of the nitrogen-doped carbon nanoballs increases. For the electrocatalytic activity in an alkaline solution, the limiting current density and onset potential for the ORR activity can be significantly improved for the samples after thermal annealing at 900 °C. We anticipate that solution plasma process will be a viable alternative way for synthesizing heteroatom-doped carbon electrocatalysts for broad application in the field of fuel cells, metal-air batteries, and supercapacitors.

In situ solution plasma synthesis of nitrogen-doped carbon nanoparticles as metal-free electrocatalysts for the oxygen reduction reaction

2014 ◽  
Vol 2 (43) ◽  
pp. 18677-18686 ◽  
Author(s):  
Gasidit Panomsuwan ◽  
Satoshi Chiba ◽  
Youta Kaneko ◽  
Nagahiro Saito ◽  
Takahiro Ishizaki
Keyword(s):  
Carbon Nanoparticles ◽  
Organic Liquid ◽  
Liquid Mixtures ◽  
Reduction Reaction ◽  
Plasma Synthesis ◽  
Plasma Process ◽  
Nitrogen Doped ◽  
Metal Free ◽  
Nitrogen Doped Carbon

Nitrogen-doped carbon nanoparticles were successfully synthesized by a facile solution plasma process without the addition of metal catalysts. Organic liquid mixtures of benzene and pyrazine were used as the precursors for the synthesis.

scholarly journals Cobalt Nanoparticles on Plasma-Controlled Nitrogen-Doped Carbon as High-Performance ORR Electrocatalyst for Primary Zn-Air Battery

Nanomaterials ◽  
2020 ◽  
Vol 10 (2) ◽  
pp. 223 ◽  
Author(s):  
Seonghee Kim ◽  
Hyun Park ◽  
Oi Lun Li
Keyword(s):  
High Performance ◽  
Synergetic Effect ◽  
Carbon Support ◽  
Reduction Reaction ◽  
Cobalt Nanoparticles ◽  
Limiting Current ◽  
Onset Potential ◽  
Nitrogen Doped ◽  
Air Battery ◽  
Nitrogen Doped Carbon

Metal–air batteries and fuel cells have attracted much attention as powerful candidates for a renewable energy conversion system for the last few decades. However, the high cost and low durability of platinum-based catalysts used to enhance sluggish oxygen reduction reaction (ORR) at air electrodes prevents its wide application to industry. In this work, we applied a plasma process to synthesize cobalt nanoparticles catalysts on nitrogen-doped carbon support with controllable quaternary-N and amino-N structure. In the electrochemical test, the quaternary-N and amino-N-doped carbon (Q-A)/Co catalyst with dominant quaternary-N and amino-N showed the best onset potential (0.87 V vs. RHE) and highest limiting current density (−6.39 mA/cm2). Moreover, Q-A/Co was employed as the air catalyst of a primary zinc–air battery with comparable peak power density to a commercial 20 wt.% Pt/C catalyst with the same loading, as well as a stable galvanostatic discharge at −20 mA/cm2 for over 30,000 s. With this result, we proposed the synergetic effect of transitional metal nanoparticles with controllable nitrogen-bonding can improve the catalytic activity of the catalyst, which provides a new strategy to develop a Pt-free ORR electrocatalyst.

Synthesis of graphitic-N and amino-N in nitrogen-doped carbon via a solution plasma process and exploration of their synergic effect for advanced oxygen reduction reaction

2017 ◽  
Vol 5 (5) ◽  
pp. 2073-2082 ◽  
Author(s):  
Oi Lun Li ◽  
Satoshi Chiba ◽  
Yuta Wada ◽  
Gasidit Panomsuwan ◽  
Takahiro Ishizaki
Keyword(s):  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
Room Temperature ◽  
Reduction Reaction ◽  
Synergic Effect ◽  
Plasma Process ◽  
Temperature Plasma ◽  
Nitrogen Doped ◽  
Orr Activity ◽  
Nitrogen Doped Carbon

N-doped carbon synthesized by a room temperature plasma process demonstrated the synergic effect of amino-N and graphitic-N towards advanced ORR activity.

Selective nitrogen bonding states in nitrogen-doped carbon via a solution plasma process for advanced oxygen reduction reaction

RSC Advances ◽  
2016 ◽  
Vol 6 (111) ◽  
pp. 109354-109360 ◽  
Author(s):  
Oi Lun Li ◽  
Satoshi Chiba ◽  
Yuta Wada ◽  
Hoonseung Lee ◽  
Takahiro Ishizaki
Keyword(s):  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
Carbon Nanoparticles ◽  
Reduction Reaction ◽  
Plasma Process ◽  
Nitrogen Doped ◽  
Nitrogen Doped Carbon

Selective nitrogen bonding within nitrogen-doped carbon nanoparticles was achieved by altering linear and heterocyclic precursor via solution plasma.

scholarly journals A pyridinic Fe-N4 macrocycle models the active sites in Fe/N-doped carbon electrocatalysts

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Travis Marshall-Roth ◽  
Nicole J. Libretto ◽  
Alexandra T. Wrobel ◽  
Kevin J. Anderton ◽  
Michael L. Pegis ◽  
...  
Keyword(s):  
Active Site ◽  
Active Sites ◽  
Catalytic Properties ◽  
Molecular Model ◽  
Reduction Reaction ◽  
Electrochemical Studies ◽  
Onset Potential ◽  
Nitrogen Doped ◽  
Nitrogen Doped Carbon ◽  
Excellent Selectivity

Abstract Iron- and nitrogen-doped carbon (Fe-N-C) materials are leading candidates to replace platinum catalysts for the oxygen reduction reaction (ORR) in fuel cells; however, their active site structures remain poorly understood. A leading postulate is that the iron-containing active sites exist primarily in a pyridinic Fe-N4 ligation environment, yet, molecular model catalysts generally feature pyrrolic coordination. Herein, we report a molecular pyridinic hexaazacyclophane macrocycle, (phen2N2)Fe, and compare its spectroscopic, electrochemical, and catalytic properties for ORR to a typical Fe-N-C material and prototypical pyrrolic iron macrocycles. N 1s XPS and XAS signatures for (phen2N2)Fe are remarkably similar to those of Fe-N-C. Electrochemical studies reveal that (phen2N2)Fe has a relatively high Fe(III/II) potential with a correlated ORR onset potential within 150 mV of Fe-N-C. Unlike the pyrrolic macrocycles, (phen2N2)Fe displays excellent selectivity for four-electron ORR, comparable to Fe-N-C materials. The aggregate spectroscopic and electrochemical data demonstrate that (phen2N2)Fe is a more effective model of Fe-N-C active sites relative to the pyrrolic iron macrocycles, thereby establishing a new molecular platform that can aid understanding of this important class of catalytic materials.

Modifying nitrogen species of nitrogen-doped carbon nanotubes by thermal annealing to explore their role in the triiodide reduction reaction

Carbon ◽  
2020 ◽  
Vol 167 ◽  
pp. 209-218 ◽  
Author(s):  
Jose Manuel Ruiz-Marizcal ◽  
Enrique Contreras ◽  
Maricela Diaz ◽  
David Dominguez ◽  
Hugo A. Borbon-Nuñez ◽  
...  
Keyword(s):  
Carbon Nanotubes ◽  
Thermal Annealing ◽  
Reduction Reaction ◽  
Nitrogen Species ◽  
Nitrogen Doped ◽  
Nitrogen Doped Carbon

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>

Sign in / Sign up

Export Citation Format

Share Document