Open AccessSurface‐Group‐Oriented, Condensation Cyclization‐Driven, Nitrogen‐Doping Strategy for the Preparation of a Nitrogen‐Species‐Tunable, Carbon‐Material‐Supported Pd Catalyst
Author(s) -
Lu Chunshan,
Zhang Xuejie,
Qi Yani,
Ji Haoke,
Zhu Qianwen,
Wang Hao,
Zhou Yebin,
Feng Zhenlong,
Li Xiaonian
Publication year - 2019
Publication title -
chemistryopen
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.644
H-Index - 29
ISSN - 2191-1363
DOI - 10.1002/open.201800227
Subject(s) - nitrogen , catalysis , carbon fibers , desorption , chemistry , molecule , surface modification , electron transfer , inorganic chemistry , selectivity , activated carbon , organic chemistry , materials science , adsorption , composite number , composite material
A nitrogen‐carbon framework with the thickness of several molecules was fabricated through a straightforward nitrogen‐doping strategy, in which specially designed surface‐oxygen‐containing groups (SOGs) first introduced onto the porous carbon support were used to guide the generation of a surface‐nitrogen‐containing structure through condensation reactions between SOGs and the amidogen group of organic amines under hydrothermal conditions. The results indicate that different kinds of SOGs generate different types and abundances of N species. The CO‐releasing groups are apt to form a high proportion of amino groups, whereas the CO 2 ‐releasing groups, especially carboxyl and lactones, are mainly transformed into pyrrolic‐type nitrogen. In the framework with dominant pyrrolic‐type nitrogen, an electron‐rich Pd activated site composed of Pd, pyrrolic‐type N and C is built, in which electron transfer occurs from N to C and Pd atoms. This activated site contributes to the formation of electron‐rich activated hydrogen and desorption of p‐chloroaniline, which work together to achieve the superior selectivity about 99.90 % of p‐chloroaniline and the excellent reusable performance. This strategy not only provides low‐cost, nitrogen‐doped carbon materials, but also develops a new method for the fabrication of different kinds of nitrogen species structures.