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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.