Abstract

A novel B/N co-doped porous carbon nanosheet with a high heteroatom doping content has been successfully prepared. Using amino-functionalized graphene oxide (GO) as the template, oxidation polymerization of aniline, 3-aminophenylboronic acid, and m-phenylenediamine generates GO-based polyaniline nanosheets functionalized with boronic acid (GO-CBP). After high-temperature treatment, graphene-based B/N co-doped carbon nanosheets (G-CBP) are obtained, which show a typical 2D morphology with a thickness of ∼20 nm. After CO2 activation at 1000 °C, the obtained porous carbon nanosheets (G-CBP-a) have a thickness of ∼17 nm and a high specific surface area of 363 m2 g−1. Benefiting from its high surface area, unique 2D sheet nanostructure, and high heteroatom-doping contents (5.4% B and 5.3% N), G-CBP-a exhibits excellent electrochemical performance for the oxygen reduction reaction under alkaline conditions (0.1 M KOH), with a low half-wave potential (−0.27 V for G-CBP-a versus −0.18 V for Pt/C), a dominant four-electron transfer mechanism (n = 3.78 at −0.45 V), and excellent methanol tolerance and durability (10% current decrease after 20 000 s operation), as well as a high diffusion-limiting current density (JL = −4.5 mA cm−2).

Highlights

  • In the belief that they are the most feasible Pt alternatives, heteroatom (N,1–5 B,6,7 S,8 P9)-doped carbon materials have attracted remarkable attention as metal-free catalysts for oxygen reduction reaction (ORR), which is the key process in fuel cells

  • Bene ting from the high surface area, the unique 2D sheet nanostructure, and the high heteroatom-doping contents (5.4% B and 5.3% N), G-CBPa exhibits excellent electrochemical performance with respect to the oxygen reduction reaction (ORR) under alkaline conditions (0.1 M KOH), with a low half-wave potential (À0.27 V for G-CBPa versus À0.18 V for Pt/C), a dominant four-electron transfer mechanism (n 1⁄4 3.78 at À0.45 V), and excellent methanol tolerance and durability (10% current decrease a er 20 000 s operation), as well as a high diffusion-limiting current density (JL 1⁄4 À4.5 mA cmÀ2)

  • The typical synthesis route towards G-CBP-a is illustrated in Scheme 1

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Summary

Introduction

In the belief that they are the most feasible Pt alternatives, heteroatom (N,1–5 B,6,7 S,8 P9)-doped carbon materials have attracted remarkable attention as metal-free catalysts for oxygen reduction reaction (ORR), which is the key process in fuel cells. After high-temperature treatment, graphene-based B/N co-doped carbon nanosheets (G-CBP) are obtained, which show a typical 2D morphology with a thickness of $20 nm.

Results
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