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.

中文翻译：

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用于氢化的非均相金属催化剂：路易斯酸-碱对整合到碳晶格中

设计用于氢化的非均相无金属催化剂是催化领域的长期挑战。制备了纳米金刚石基碳材料，这些材料表面掺杂了富电子的氮和缺电子的硼。两个杂原子彼此直接键合，形成非淬灭的路易斯对，周围的石墨结构产生无限的π电子给体。值得注意的是，这些路易斯对可以拆分ħ ₂到生成H ⁺ / H ^-对，其随后用作用于不同的基材的加氢活性种。这一前所未有的发现为H ₂的吸收提供了启示。 跨碳基材料，这表明碳表面的双重路易斯酸碱度可用于异质活化各种小分子。