Crystalline‐Water/Coordination Induced Formation of 3D Highly Porous Heteroatom‐Doped Ultrathin Carbon Nanosheet Networks for Oxygen Reduction Reaction

Abstract

Development of highly efficient electrocatalysts with low cost for oxygen reduction reaction (ORR) is crucial for their application in fuel cells and metal‐air batteries. In this work, we report a synthesis of 3D heteroatom‐doped ultrathin carbon nanosheet networks directly starting from solid raw materials. This method represents an operationally simple, general, and sustainable strategy to various ultrathin carbon nanosheet networks. Evaporation of crystalline water and coordination interaction are proposed to be responsible for the formation of the 3D carbon nanosheet networks. The carbon nanosheet networks possess high surface area with micro‐ and macropores, large pore volume, ultrathin nanosheet structure, and effective N/S‐co‐doping. The as‐prepared materials show outstanding electrocatalytic ORR performance with more positive onset potential and half‐wave potential, good methanol tolerance, and excellent stability, compared with those of the porous carbons derived from the ZIF counterpart and commercial Pt/C. This work not only provides highly active ORR electrocatalysts via an operationally simple and green process and also demonstrates a general method to prepare 3D ultrathin carbon nanosheet networks without any additional template and solvent.

Regulating carbon work function to boost electrocatalytic activity for the oxygen reduction reaction

“…2(f). The XPS results suggested that the high-resolution N 1s spectrum could be deconvoluted into four types: 398.4 ± 0.2, 400.0 ± 0.2, 401.0 ± 0.2, and 402.0 ± 0.2 eV, corresponding to pyridinic N, pyrrolic N, graphitic N, and oxidized N, respectively [18]. An essential feature of Cs-N/C was that the pyridinic N peak split.…”

Phthalocyanine-induced iron active species in metal–organic framework-derived porous carbon for efficient alkaline zinc–air batteries

“…22,23 Therefore, a large number of ZIF-derived carbon nanomaterials such as carbon nanotubes and carbon nanosheets have been widely utilized in different energy-related applications, because of their large specific surface area, excellent electrical conductivity, high stability and other significant advantages. [24][25][26][27] In this context, the rational design and facile preparation of porous MOF-derived carbon-based catalysts in energy conversion and storage is highly important and desired.…”

Recycling the Catalyst of Atom Transfer Radical Polymerization to Prepare a Cu, N Codoped Mesoporous Carbon Electrocatalyst for Oxygen Reduction

“…Organics containing rich N atoms are ideal precursors for M–N–C. For example, polyacrylonitrile (PAN) is frequently used to synthesize M–N–C catalysts for ORR electrocatalysis. , As for metal-free carbon catalysts, nitrogen , and sulfur have been chosen as heteroatoms doped on carbon materials to facilitate the ORR performance.…”