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A C‐S‐C Linkage‐Triggered Ultrahigh Nitrogen‐Doped Carbon and the Identification of Active Site in Triiodide Reduction
Author(s) -
Chang Jiangwei,
Yu Chang,
Song Xuedan,
Tan Xinyi,
Ding Yiwang,
Zhao Zongbin,
Qiu Jieshan
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202012141
Subject(s) - dopant , pyrolysis , carbon fibers , doping , carbonization , adsorption , chemistry , nitrogen , inorganic chemistry , materials science , organic chemistry , optoelectronics , composite number , composite material
An efficient chemical synthesis route, with an aim of reaching an ultrahigh nitrogen (N)‐doping level in carbon materials can provide a platform where the type and amount of N dopant can be tuned over a wide range. We propose a C‐S‐C linkage‐triggered confined‐pyrolysis strategy for the high‐efficiency in situ N‐doping into carbon matrix and an ultrahigh doping level up to 13.5 at %, which is close to the theoretical upper limit (15.2 at %) is realized at a high carbonization temperature of 1000 °C. The pyridinic N is dominant with a maximum percent of 48.7 %. By using I 3 − reduction as an example, the resultant NCM‐5 exhibits the best activity with a power conversion efficiency of 8.77 %. A pyridinic N site‐dependent activity is demonstrated in which the amount of active sites increases with the increase of pyridinic N, and the carbon atom adjacent to electron‐withdrawing pyridinic N at the armchair edge acts as the most favorable site for the adsorption of I 2 .