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Metal–Organic Framework‐Templated Porous Carbon for Highly Efficient Catalysis: The Critical Role of Pyrrolic Nitrogen Species
Author(s) -
Huang Gang,
Yang Li,
Ma Xiao,
Jiang Jun,
Yu ShuHong,
Jiang HaiLong
Publication year - 2016
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201504867
Subject(s) - catalysis , dopant , materials science , pyrolysis , carbon fibers , metal , nitrogen , chemical engineering , porosity , graphene , metal organic framework , amorphous carbon , inorganic chemistry , amorphous solid , nanotechnology , organic chemistry , chemistry , metallurgy , composite material , doping , composite number , optoelectronics , adsorption , engineering
Metal‐free catalysts are of great importance and alternative candidates to conventional metal‐based catalysts for many reactions. Herein, several types of metal–organic frameworks have been exploited as templates/precursors to afford porous carbon materials with various nitrogen dopant forms and contents, degrees of graphitization, porosities, and surface areas. Amongst these materials, the PCN‐224‐templated porous carbon material optimized by pyrolysis at 700 °C (denoted as PCN‐224‐700) is composed of amorphous carbon coated with well‐defined graphene layers, offering a high surface area, hierarchical pores, and high nitrogen content (mainly, pyrrolic nitrogen species). Remarkably, as a metal‐free catalyst, PCN‐224‐700 exhibits a low activation energy and superior activity to most metallic catalysts in the catalytic reduction of 4‐nitrophenol to 4‐aminophenol. Theoretical investigations suggest that the content and type of the nitrogen dopant play crucial roles in determining the catalytic performance and that the pyrrolic nitrogen species makes the dominant contribution to this activity, which explains the excellent efficiency of the PCN‐224‐700 catalyst well.