Self-Size-Limiting Nanoscale Perforation of Graphene for Dense Heteroatom Doping

Abstract

A scalable and controllable nanoscale perforation method for graphene is developed on the basis of the two-step thermal activation of a graphene aerogel. Different resistance to the thermal oxidation between graphitic and defective domains in the weakly reduced graphene oxide is exploited for the self-limiting nanoscale perforation in the graphene basal plane via selective thermal degradation of the defective domains. The resultant nanoporous graphene with a narrow pore-size distribution addresses the long-standing challenge for the high-level doping of graphene with lattice-mismatched large-size heteroatoms (S and P). Noticeably, this novel heteroatom doping strategy is demonstrated to be highly effective for oxygen reduction reaction (ORR) catalysis. Not only the higher level of heteroatom doping but also favorable spin and charge redistribution around the pore edges leads to a strong ORR activity as supported by density functional theory calculations.

Voltage gated inter-cation selective ion channels from graphene nanopores

“…Graphene nanopores have been explored for applications in sensing and separations, and are a promising material for a solid-state ion channel. Aside from graphene being atomically thin 8 , mechanically strong 9 , and relatively inert 10 , it has been shown that well-defined nanometer and sub-nanometer pores can be controllably introduced into the material [11][12][13][14][15][16][17] . Nanopores in graphene have been shown to exhibit ion selectivity 12,[18][19][20][21][22][23][24] and gated nanopores in graphene have been used in sensing biomolecules such as DNA and proteins [25][26] .…”

Free‐Standing 3D Nanoporous Duct‐Like and Hierarchical Nanoporous Graphene Films for Micron‐Level Flexible Solid‐State Asymmetric Supercapacitors

“…The pore size lies in 30–200 nm and 2–30 nm is fairly consistent with that of the NPC substrate and the gap among hollow 3D‐npG, respectively. Some hydrophilic groups such as NO 2 , NH 2 , CO, and CO will be introduced onto the surface of the 3D‐npG after acidulated by concentrated nitric, which can increase the wettability of 3D‐npG with electrolyte and improve its capacitance as the electrode due to the existence of N‐doping groups . The electrochemical properties of the acidulated 3D‐npG film were investigated in a three‐electrode cell in 2.0 m LiNO 3 aqueous electrolyte.…”

“…Some hydrophilic groups such as NO 2 , NH 2 , C O, and C O will be introduced onto the surface of the 3D-npG after acidulated by concentrated nitric, [ 53 ] which can increase the wettability of 3D-npG with electrolyte and improve its capacitance as the electrode due to the existence of N-doping groups. [54][55][56] The electrochemical properties of the acidulated 3D-npG fi lm were investigated in a three-electrode cell in 2.0 M LiNO 3 aqueous electrolyte. The electrode displayed rectanglelike CV curves, even at a high scan rate of 500 mV s −1 , inferring an ideal capacitive behavior ( Figure S13a, Supporting Information).…”

Production of Metal‐Free Composites Composed of Graphite Oxide and Oxidized Carbon Nitride Nanodots and Their Enhanced Photocatalytic Performances

“…2D materials such as graphene, graphene oxide, hexagonal boron nitride, and metal dichalcogenides, have been intensively studied due to their unique physical, chemical, and morphological properties . Hybridization of different 2D materials often enhances their properties for various applications such as energy storage materials, photocatalytic reactions, and photovoltaic systems …”

“…GN showse nhanced photocatalytic performance for degrading an organic pollutant, Rhodamine B, under visible light.2D materials such as graphene, graphene oxide,h exagonal boron nitride, and metal dichalcogenides, have been intensively studied due to their unique physical, chemical, and morphological properties. [1][2][3][4][5][6][7][8][9] Hybridization of different2 Dm aterials often enhances their properties for variousa pplicationss uch as energys torage materials, photocatalytic reactions, and photovoltaic systems. [10][11][12][13][14] Photocatalysts use solar energy to trigger chemicalr eactions, such as H 2 evolution, CO 2 reduction, and degradation of organic pollutants, whicha re important to solve energy and environmental problems.…”