“…Methanol tolerance test was carried out by adapting the method according to the previous report . At constant potential of 0.50 V vs RHE, 5.05 mL of methanol was spiked into 120 mL of KOH electrolyte at a desirable time (at 200 s in our study, as shown Figure S 6c), resulting in a concentration of 1 M.…”
Single-atom catalysts (SACs) possess the potential to involve the merits of both homogeneous and heterogeneous catalysts altogether and thus have gained considerable attention. However, the large-scale synthesis of SACs with rich isolate-metal sites by simple and low-cost strategies has remained challenging. In this work, we report a facile one-step pyrolysis that automatically produces SACs with high metal loading (5.2−15.9 wt %) supported on two-dimensional nitro-oxygenated carbon (M 1 -2D-NOC) without using any solvents and sacrificial templates. The method is also generic to various transition metals and can be scaled up to several grams based on the capacity of the containers and furnaces. The high density of active sites with N/O coordination geometry endows them with impressive catalytic activities and stability, as demonstrated in the oxygen reduction reaction (ORR). For example, Fe 1 -2D-NOC exhibits an onset potential of 0.985 V vs RHE, a half-wave potential of 0.826 V, and a Tafel slope of −40.860 mV/dec. Combining the theoretical and experimental studies, the high ORR activity could be attributed its unique FeO-N 3 O structure, which facilitates effective charge transfer between the surface and the intermediates along the reaction, and uniform dispersion of this active site on thin 2D nanocarbon supports that maximize the exposure to the reactants.
“…Methanol tolerance test was carried out by adapting the method according to the previous report . At constant potential of 0.50 V vs RHE, 5.05 mL of methanol was spiked into 120 mL of KOH electrolyte at a desirable time (at 200 s in our study, as shown Figure S 6c), resulting in a concentration of 1 M.…”
Single-atom catalysts (SACs) possess the potential to involve the merits of both homogeneous and heterogeneous catalysts altogether and thus have gained considerable attention. However, the large-scale synthesis of SACs with rich isolate-metal sites by simple and low-cost strategies has remained challenging. In this work, we report a facile one-step pyrolysis that automatically produces SACs with high metal loading (5.2−15.9 wt %) supported on two-dimensional nitro-oxygenated carbon (M 1 -2D-NOC) without using any solvents and sacrificial templates. The method is also generic to various transition metals and can be scaled up to several grams based on the capacity of the containers and furnaces. The high density of active sites with N/O coordination geometry endows them with impressive catalytic activities and stability, as demonstrated in the oxygen reduction reaction (ORR). For example, Fe 1 -2D-NOC exhibits an onset potential of 0.985 V vs RHE, a half-wave potential of 0.826 V, and a Tafel slope of −40.860 mV/dec. Combining the theoretical and experimental studies, the high ORR activity could be attributed its unique FeO-N 3 O structure, which facilitates effective charge transfer between the surface and the intermediates along the reaction, and uniform dispersion of this active site on thin 2D nanocarbon supports that maximize the exposure to the reactants.
“…However, doping carbon materials with precious metals such as Pt, Ir, and Ru was found not to be a logical solution [8], since the doped metals will still contribute to excessive cost. One of the metals that have been used as an effective dopant is cobalt (Co) and it is known that Co and cobalt oxides can accelerate both ORR and OER in alkaline electrolytes [11][12][13]. Transition metal oxides and hydroxides have exhibited good OER activity [14,15], whereas their sulfides, selenide, nitride, and phosphide counterparts have demonstrated potential as ORR and OER catalysts [16][17][18][19][20].…”
Electrocatalysts with high activity towards both oxygen reduction and evolution reaction are desirable for metal-air batteries. However, most commercially used electrocatalysts result in sluggish kinetics for these oxygen reactions, and different catalysts are usually used for each oxygen reaction. The development of efficient electrocatalysts that can facilitate both reactions, with low overpotentials resulting in less energy consumption is desirable. Herein we report secondary data analysis for materials developed in our previous study, FeS2 electrocatalyst supported on chlorinated carbon nanotubes (ClCNTs) using chemicals that are not harsh chemicals and investigated its catalytic activity towards ORR and OER. FeS2 nanoparticles were produced by thermal annealing of ClCNTs in thiophene at different annealing temperatures. The effect of thiophene volume and reaction time on the growth of FeS2 nanoparticles was also evaluated. The size of FeS2 nanoparticles coated on the surface of ClCNTs increased with an increase in thermal annealing reaction time, and this reduced the catalytic activity of the materials. Whereas as the volume of thiophene was increased during the production of FeS2-loaded ClCNTs, no FeS2 nanoparticles were observed on the surface of the ClCNTs. ClCNTs annealed at 900 °C showed the greatest growth of FeS2 nanoparticles on their surface and provided the greatest enhancement of the ORR and OER activities, evidenced by the low Tafel slope of 63 mV/dec and low overpotential of 252 mV. The number of electrons involved during the reduction of oxygen was found to be 4, which means that the formation of water was favorable when using this electrocatalyst. In our previous study only, cyclic voltammetry was used to evaluate the electrocatalytic activity of the materials toward ORR.
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