The cage structure of C60 fullerenes with encapsulated metal atoms, i.e. endohedral fullerenes ([email protected]) possess unique electronic properties with novel applications. By using density functional theory (DFT), we for the first time predict endohedral [email protected] (M = Na, K, Rb, Cs, Sc, Ti, Mn, Fe) fullerenes from 20 possible candidates as promising high performance hydrogen evolution reaction (HER) catalysts. For the pristine C60, the Gibbs free energy is too positive to prevent the adsorption of H-atoms on surface carbon atoms. However, when a metal atom is embedded in the C60 cage, the H-atom binding free energy on [email protected] can be optimized to ideal value for HER (ΔG_H = 0). The catalytic active site is non-metal C-atom and the HER performance of [email protected] are even better than those of the state-of-the-art Pt and MoS₂ catalysts. The excellent catalytic activities are attributed to the charge transfer between the metal atom and C60 cage. Since the endohedral fullerenes can be easily realized in experiment, our findings highlight a new class of low-cost and efficient HER catalyst for experimental validation studies toward hydrogen production.

具有被包封的金属原子的C60富勒烯的笼状结构，即内表面富勒烯（[受电子邮件保护]）具有独特的电子性质，并具有新颖的应用。通过使用密度泛函理论（DFT），我们首次从20种可能的候选物中预测了内面体（受电子邮件保护）（M = Na，K，Rb，Cs，Sc，Ti，Mn，Fe）富勒烯作为有前途的高性能氢生成反应（HER）催化剂。对于原始的C60而言，吉布斯自由能太大，无法阻止H原子在表面碳原子上的吸附。然而，当金属原子被嵌入在C60笼，H-原子上[电子邮件保护]结合自由能可以被优化到理想值对HER（ΔG _ħ = 0）。催化活性位点是非金属C原子，[受电子邮件保护]的HER性能甚至优于最新的Pt和MoS ₂催化剂。优异的催化活性归因于金属原子与C60笼之间的电荷转移。由于内层富勒烯可以在实验中轻松实现，因此我们的发现突出了一种新型的低成本高效HER催化剂，可用于制氢的实验验证研究。