A Heterogeneous Metal‐Free Catalyst for Hydrogenation: Lewis Acid–Base Pairs Integrated into a Carbon Lattice. Issue 42 (19th June 2018)

• Record Type: Journal Article
• Authors: Ding, Yuxiao; Huang, Xing; Yi, Xianfeng; Qiao, Yunxiang; Sun, Xiaoyan; Zheng, Anmin; Su, Dang Sheng
• Is Part Of: Angewandte Chemie international edition. Volume 57:Issue 42(2018)
• Page Start: 13800
• Page End: 13804
• Publication Date: 2018-06-19
• Subjects: heterogeneous catalysis -- hydrogenation -- Lewis pairs -- metal-free catalysis -- nanocarbons; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201803977
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: 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 H2 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 H2 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. Abstract : Lewis in the sky with diamonds : Solid‐phase metal‐free Lewis pairs, comprised of electron‐rich nitrogen and electron‐deficient boron, were dispersed on sp 2 ‐hybridized diamond surfaces. The unquenched Lewis pairs split H2 into H + and H − and can be used to catalytically hydrogenate a range of substrates.