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A Heterogeneous Metal‐Free Catalyst for Hydrogenation: Lewis Acid–Base Pairs Integrated into a Carbon Lattice
Author(s) -
Ding Yuxiao,
Huang Xing,
Yi Xianfeng,
Qiao Yunxiang,
Sun Xiaoyan,
Zheng Anmin,
Su Dang Sheng
Publication year - 2018
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201803977
Subject(s) - lewis acids and bases , heteroatom , catalysis , frustrated lewis pair , carbon fibers , chemistry , nanodiamond , electron deficiency , boron , metal , molecule , electron pair , heterogeneous catalysis , inorganic chemistry , materials science , organic chemistry , electron , alkyl , diamond , composite number , composite material , physics , quantum mechanics
Designing heterogeneous metal‐free catalysts for hydrogenation is a long‐standing challenge in catalysis. Nanodiamond‐based carbon materials were prepared that are surface‐doped with electron‐rich nitrogen and electron‐deficient boron. The two heteroatoms are directly bonded to each other to form unquenched Lewis pairs with infinite π‐electron donation from the surrounding graphitic structure. Remarkably, these Lewis pairs can split H 2 to form H + /H − pairs, which subsequently serve as the active species for hydrogenation of different substrates. This unprecedented finding sheds light on the uptake of H 2 across carbon‐based materials and suggests that dual Lewis acidity–basicity on the carbon surface may be used to heterogeneously activate a variety of small molecules.