Conductive Metal-Organic Frameworks with Extra Metallic Sites as an Efficient Electrocatalyst for the Hydrogen Evolution Reaction.,Advanced Science

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Conductive Metal-Organic Frameworks with Extra Metallic Sites as an Efficient Electrocatalyst for the Hydrogen Evolution Reaction.
Advanced Science ( IF 14.3 ) Pub Date : 2020-03-16 , DOI: 10.1002/advs.202000012
Hao Huang ₁ , Yue Zhao ₂ , Yimin Bai ₁ , Fumin Li ₁ , Ying Zhang ₁ , Yu Chen ₂

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The 2D conductive metal-organic frameworks (MOFs) are expected to be an ideal electrocatalyst due to their high utilization of metal atoms. Exploring a new conjugated ligand with extra active metallic center can further boost the structural advantages of conductive MOFs. In this work, hexaiminohexaazatrinaphthalene (HAHATN) is employed as a conjugated ligand to construct bimetallic sited conductive MOFs (M23(M13∙HAHATN)2) with an extra M-N2 moiety. Density functional theory (DFT) calculations demonstrate that the 2D conjugated framework renders M23(M13∙HAHATN)2 a high electric conductivity with narrow bandgap (0.19 eV) for electron transfer and a favorable in-plane porous structure (2.7 nm) for mass transfer. Moreover, the metal atom at the extra M-N2 moiety has a higher unsaturation degree than that at M-N4 linkage, resulting in a stronger ability to donate electrons for enhancing electroactivity. These characteristics endow the new conductive MOFs with an enhanced electroactivity for hydrogen evolution reaction (HER) electrocatalysis. Among the series of M23(M13∙HAHATN)2 MOF, Ni3(Ni3∙HAHATN)2 nanosheets with the optimal structure exhibit a small overpotential of 115 mV at 10 mA cm-2, low Tafel slope of (45.6 mV dec-1), and promising electrocatalytic stability for HER. This work provides an effective strategy for designing conductive MOFs with a favorable structure for electrocatalysis.

中文翻译：

具有额外金属位点的导电金属有机框架作为析氢反应的有效电催化剂。

二维导电金属有机框架（MOF）由于其对金属原子的高利用率而有望成为理想的电催化剂。探索具有额外活性金属中心的新型共轭配体可以进一步增强导电MOF的结构优势。在这项工作中，六亚氨基六氮杂萘 (HAHATN) 被用作共轭配体，构建具有额外 M-N2 部分的双金属位点导电 MOF (M23(M13∙HAHATN)2)。密度泛函理论 (DFT) 计算表明，二维共轭框架使 M23(M13∙HAHATN)2 具有高电导率，窄带隙 (0.19 eV) 用于电子传递，并具有良好的面内多孔结构 (2.7 nm) 用于传质。此外，额外的M-N2部分的金属原子比M-N4键的金属原子具有更高的不饱和度，从而具有更强的贡献电子的能力，从而增强电活性。这些特性赋予新型导电 MOF 增强析氢反应 (HER) 电催化的电活性。在M23(M13∙HAHATN)2 MOF系列中，具有最佳结构的Ni3(Ni3∙HAHATN)2纳米片在10 mA cm-2下表现出115 mV的小过电势，低塔菲尔斜率(45.6 mV dec-1) ，并且有望实现 HER 的电催化稳定性。这项工作为设计具有良好电催化结构的导电 MOF 提供了有效的策略。

更新日期：2020-03-16

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