A Thermally Decomposable Template Route to Synthesize Nitrogen-Doped Wrinkled Carbon Nanosheets as Highly Efficient and Stable Electrocatalysts for the Oxygen Reduction Reaction

Abstract

We successfully developed a thermally decomposable template route to prepare wrinkled carbon nanosheets with a high level of nitrogen functional moieties by direct carbonization of biomass glucose and dicyandiamide as the renewable feedstocks. Confined pyrolysis of glucose within the interlayers of dicyandiamide-derived g-C3N4 as a thermally removable template results in the formation of two-dimensional (2D) wrinkled carbon nanosheets as well as simultaneous high-level nitrogen doping. The textural properties and nitrogen contents could be controlled by adjusting the mass ratio of glucose/dicyandiamide. Among various samples, the sample prepared with the dicyandiamide/glucose mass ratio of 7/1 has optimal activity for the electrocatalytic oxygen reduction (onset potential −0.12 V vs saturated calomel electrode (SCE); limiting current density 4.73 mA/cm2) in 0.1 M KOH solution, the half-wave potential of which is only 67 mV larger than that for 20 wt % Pt/C. Moreover, it demonstrates a highly efficient four-electron reaction process, as well as superior durability and tolerance to MeOH crossover to Pt/C. The excellent activity is mainly attributed to the high content of pyridinic and graphitic-N groups, highly graphitized structures, and wrinkled 2D nanostructures, efficiently promoting the increased exposure of actives sites and fast mass/electron transfer.

FeCo alloy/N, S dual-doped carbon composite as a high-performance bifunctional catalyst in an advanced rechargeable zinc-air battery

“…The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are key electrochemical processes of air electrodes for rechargeable ZABs [10][11][12]. However, the inherent sluggish kinetics of the ORR and OER impede battery development [13][14][15]. Noble metal-based catalysts (e.g.…”

Environmental Catalysis: Present and Future

“…The biomaterials displayed one of the highest current densities values reported in the literature for laccases functionalized nanoparticles systems. As a relevant example, N‐doped wrinkled graphene materials were synthesized through a one‐pot thermal treatment of glucose and dicyandiamide as the renewable precursors towards oxygen reduction reaction . The synthetic route could significantly revolutionize the current methodologies for the chemical synthesis of N‐doped graphene nanosheets since it promotes the confined growth of graphene within the interlayers of dicyandiamide‐derived g‐C 3 N 4 as well as the simultaneous nitrogen doping into the graphene layers (Figure C).…”

“…Enzymes are powerful bio-entities which are able to catalyze at electrode surfaces a number of redox reactions of technological importance that usually require high overpotential values to render significant yields. [120] Importantly, they provide many advantages such as high electrocatalytic currents and the possibility to carry out the electrocatalytic processes in a reversible way.…”

“…Electrocatalytic enzymes systems composed of (A) dehydrogenases, (B) multicopper oxidases, (C) carbon monoxide deshydrogenases and (D) peroxidases. Adapted with permission of ref [120]. Copyright, Amercan Chemical Society.…”

Ice/Salt‐Assisted Synthesis of Ultrathin Two‐Dimensional Micro/Mesoporous Iron and Nitrogen Co‐Doped Carbon as an Efficient Electrocatalyst for Oxygen Reduction

“…Recently,t wo-dimensional (2D) carbonm aterials have drawn increasing interestf or their application in electrocatalysis owingt ot heir high conductivity,l arge specific area,a nd highly open and exposed surfaces. [19][20][21][22][23][24] Compared to the previously reported3 Dp orousc arbon-based electrocatalytic materials in the literature, [25,26] 2D carbon materials theoretically possess a more accessible surface area and significantly higher percentage of exposed catalytic active sites for ORR reactants, thereby offering ap ortfolio of highly attractive electrocatalysts towards ORR. [27,28] Severalapproaches to synthesize 2D carbon materials have been reported, including hard-ands oft-template synthesis as well as the constructiono f2 Ds tructured carbonization precursors.…”