Issue 10, 2023

Generation of covalent organic framework-derived porous N-doped carbon nanosheets for highly efficient electrocatalytic hydrogen evolution

Abstract

Hydrogen production by electrochemical water splitting is a promising green and renewable hydrogen energy route due to zero pollution, high purity, and abundant water resources. In this context, completely metal-free electrocatalysis is an emerging research area for clean energy production due to its low cost, eco-friendliness, high stability, and high resistance to a wide pH range. However, only a few electrocatalysts like g-C3N4, CNTs, and heteroatom-doped graphene have been reported to date that exhibit robust metal-free hydrogen evolution reaction (HER) performances. Herein, we have developed a triazine-containing polyimide-based covalent organic framework (TP-COF) by a one-pot condensation reaction between pyromellitic dianhydride and melamine under reflux condensation. The polymeric framework exhibited a unique two-dimensional nanosheet morphology with a moderate surface area of 312.6 m2 g−1 and abundant pores of 1.8 nm. The synthesized TP-COF displayed a reasonable electrocatalytic HER performance with excellent long-term stability. Furthermore, the HER performance was further enhanced by pyrolyzing the TP-COF at 700 °C to prepare the N-doped porous carbon nanosheet, TP-COF-C700. The high surface area (672.2 m2 g−1) with uniform mesopores (∼1.98 nm), amplified electrical conductivity of TP-COF-C700, and presence of enriching N as the dopants for improving active sites made the TP-COF-C700 a promising HER electrocatalyst. The TP-COF-C700 showed the HER overpotential of 94 mV@10 mA cm−2 current density with 60 h long-range durability and 98% faradaic efficiency for hydrogen evolution. This report highlights a unique paradigm for preparing highly efficient metal-free electrocatalysts for HER.

Graphical abstract: Generation of covalent organic framework-derived porous N-doped carbon nanosheets for highly efficient electrocatalytic hydrogen evolution

Associated articles

Supplementary files

Article information

Article type
Paper
Submitted
11 júl 2023
Accepted
06 sep 2023
First published
06 sep 2023
This article is Open Access
Creative Commons BY-NC license

Energy Adv., 2023,2, 1713-1723

Generation of covalent organic framework-derived porous N-doped carbon nanosheets for highly efficient electrocatalytic hydrogen evolution

S. Halder, A. K. Pradhan, S. Khan and C. Chakraborty, Energy Adv., 2023, 2, 1713 DOI: 10.1039/D3YA00325F

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