The state-of-the-art alkaline hydrogen evolution catalyst of united ruthenium single atoms and small ruthenium nanoparticles has sparked considerable research interest. However, it remains a serious problem that hydrogen evolution primarily proceeds on the less active ruthenium single atoms instead of the more efficient small ruthenium nanoparticles in the catalyst, hence largely falling short of its full activity potential. Here, we report that by combining highly oxophilic cerium single atoms and fully-exposed ruthenium nanoclusters on a nitrogen functionalized carbon support, the alkaline hydrogen evolution centers are facilely reversed to the more active ruthenium nanoclusters driven by the strong oxophilicity of cerium, which significantly improves the hydrogen evolution activity of the catalyst with its mass activity up to −10.1 A mg⁻¹ at −0.05 V. This finding is expected to shed new light on developing more efficient alkaline hydrogen evolution catalyst by rational regulation of the active centers for hydrogen evolution.

由钌单原子和小钌纳米颗粒组成的最先进的碱性析氢催化剂引起了人们的广泛研究兴趣。然而，仍然存在一个严重的问题，即析氢主要在催化剂中活性较低的钌单原子上进行，而不是在催化剂中更有效的小钌纳米颗粒上进行，因此很大程度上没有达到其全部活性潜力。在这里，我们报告，通过将高度亲氧性的铈单原子和完全暴露的钌纳米团簇结合在氮功能化的碳载体上，碱性析氢中心很容易逆转为由铈的强亲氧性驱动的更活跃的钌纳米团簇，这显着改善了该催化剂的析氢活性在-0.05 V时质量活性高达-10.1 A mg ^-1。这一发现有望为通过合理调控析氢活性中心开发更高效的碱性析氢催化剂提供新的思路。