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Endohedral metallofullerenes ([email protected]) as efficient catalysts for highly active hydrogen evolution reaction
Journal of Catalysis ( IF 6.5 ) Pub Date : 2017-09-14 , DOI: 10.1016/j.jcat.2017.08.025
Tianwei He , Guoping Gao , Liangzhi Kou , Geoffrey Will , Aijun Du

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 (ΔGH = 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.



中文翻译:

内表面金属富勒烯([电子邮件保护])作为高效活性氢释放反应的有效催化剂

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。

更新日期:2017-09-14
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