Zhao Yuanmeng, Cong Hengjiang, Li Peng, Wu Dean, Chen Shengli, Luo Wei
College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, Hubei, 430072, P. R. China.
Angew Chem Int Ed Engl. 2021 Mar 22;60(13):7013-7017. doi: 10.1002/anie.202016207. Epub 2021 Feb 24.
Layered transition metal dichalcogenide (TMD) nanomaterials are promising alternatives to platinum (Pt) for the hydrogen evolution reaction (HER). However, the family of layered TMDs is mainly limited to Group IV-VII transition metals, while the synthesis of layered TMDs based on metals from other groups still remains a challenge. Herein, we demonstrate by atomic-resolution transmission electron microscopy that hexagonal RuSe (h-RuSe ) nanosheets with a mixture of 2H and 1T phases can be obtained by a facile bottom-up colloidal synthetic approach. The obtained h-RuSe , which can be transformed into the thermodynamically favorable phase of cubic RuSe (c-RuSe ) only after annealing at 600 °C, exhibits Pt-like HER performance, with a fivefold turnover frequency enhancement compared to the c-RuSe in alkaline media. Experimental results and density functional theory (DFT) calculations reveal that the enhanced adsorption free energies of H O (ΔG ), optimized adsorption free energies of H (ΔG ), and increased conductivity of h-RuSe contribute to its superior HER activity.
层状过渡金属二硫属化物(TMD)纳米材料是用于析氢反应(HER)的有前景的铂(Pt)替代物。然而,层状TMD家族主要限于IV-VII族过渡金属,而基于其他族金属的层状TMD的合成仍然是一个挑战。在此,我们通过原子分辨率透射电子显微镜证明,具有2H和1T相混合物的六方RuSe(h-RuSe)纳米片可以通过简便的自下而上胶体合成方法获得。所获得的h-RuSe仅在600℃退火后才能转变为热力学上有利的立方RuSe(c-RuSe)相,其表现出类Pt的HER性能,在碱性介质中与c-RuSe相比周转频率提高了五倍。实验结果和密度泛函理论(DFT)计算表明,h-RuSe增强的H₂O吸附自由能(ΔGₐdₛ)、优化的H吸附自由能(ΔGₐdₕ)以及增加的电导率有助于其优异的HER活性。