Kinetic Understanding of the Reduction of Oxygen to Hydrogen Peroxide over an N-Doped Carbon Electrocatalyst

Abstract

Nitrogen-doped carbon catalysts for the electrochemical oxygen reduction reaction (ORR) have great potential to substitute precious metal alloy catalysts for the electrochemical synthesis of H 2 O 2 based on a fuel cell setup. Consequently, obtaining a kinetic understanding of nitrogen-doped carbon catalysts in acidic media is essential. In this study, the mathematically modified Damjanovic model and Nabae model were applied to calculate the kinetic constants for an N/C catalyst prepared from polyimide particles. The results show that the N/C catalyst has high selectivity for the two-electron reduction of O 2 , making it a promising catalyst for the electrochemical production of H 2 O 2 . This study gives quantitative insight into the oxygen reduction reaction mechanism over an N/C catalyst prepared by the pyrolysis of polyimide nanoparticles.

Tailoring the Electrochemical Production of H2O2: Strategies for the Rational Design of High‐Performance Electrocatalysts

“…Lastly, Wu et al investigated the kinetics of electrocatalytic ORR to H 2 O 2 over N‐doped carbon catalyst by calculating the individual kinetic rate constants for H 2 O production, H 2 O 2 production, as well as H 2 O 2 reduction by applying a modified Damjanovic model and the Nabae model . The modified Damjanovic model was first used to calculate kinetic constants while the Nabae model was employed to calculate the kinetic rate constants.…”

“…Figure illustrates the mathematical results of their calculations such that k 1 °, k 2 °, and k 3 ° (calculated from the Nabae model) correspond to the kinetic rate constants for the four‐electron pathway, two‐electron pathway, and H 2 O 2 reduction process, respectively. The higher k 2 ° value relative to k 1 ° indicates that the N‐doped carbon catalyst exhibits a high selectivity for the two‐electron pathway compared to the four‐electron pathway, while the negligible k 3 ° value suggests that the N‐doped carbon catalyst exhibited poor catalytic activity for H 2 O 2 reduction …”

“…The values of k 1 °, k 2 °, and k 3 ° correspond to the inherent kinetic rate constants for the four‐electron pathway, two‐electron pathway, and H 2 O 2 reduction process, respectively. Reproduced with permission . Copyright 2019, American Chemical Society.…”

Sustainable Biomass Glucose-Derived Porous Carbon Spheres with High Nitrogen Doping: As a Promising Adsorbent for CO2/CH4/N2 Adsorptive Separation

“…Considering the importance of the heteroatom N, the nature of the N species on the carbon surface of ACSs-N, NCSs, and ACSs was investigated. As shown in Figure 5c-e, three sub-peaks are visible in the deconvoluted XPS N1s spectra: Pyridinic-N (N-6) at 398.5 eV, pyrrolic-/pyridonic-N (N-5) at 399.9 eV, and pyridine-N-oxide (N-X) at 402 eV, respectively [21,30,39,58]. The presence of N can not only provide Lewis basic active sites, but also increase the carbon framework polarity, which is beneficial for CO 2 /CH 4 /N 2 selectivity adsorption [21,23,35,37].…”

“…On the other hand, the polarity of the adsorbent framework could enable weak interactions between the gas molecules and the polar channels, which may further help to separate the gas mixture [23,37]. Nitrogen (N)-doping is an effective method to increase the polarity of carbon frameworks [37,39], which has been reported a lot in CO 2 /CH 4 /N 2 selective adsorption [21,23,37,40,41]. However, nowadays, most porous carbon is fine powder (<30 µm) belonging to Geldart's group C classification [42,43].…”