Conductive π-d conjugated metal-organic frameworks (MOFs) have attracted wide concerns in electrocatalysis due to their intrinsic high conductivity. However, the poor electrocatalytic stability is still a major problem that hinders the practical application of MOFs. Herein, we report a novel approach to enhancing the stability of MOF-based electrocatalyst, namely, the introduction of hydrogen bonds (H-bonds). Impressively, the π-d conjugated MOF FeCo₃(DDA)₂ exhibits ultra-high oxygen evolution reaction (OER) stability (up to 2000 h). The experimental studies demonstrate that the presence of H-bonds in FeCo₃(DDA)₂ is responsible for its ultra-high OER stability. Besides that, FeCo₃(DDA)₂ also displays a prominent OER activity (an overpotential of 260 mV versus RHE at a current density of 10 mA cm⁻² and a Tafel slope of 46.86 mV dec⁻¹). Density functional theory (DFT) calculations further indicate that the synergistic effect of the Fe and Co sites in FeCo₃(DDA)₂ contributes to its prominent OER performance. This work provides a new avenue of boosting the electrocatalytic stability of conductive π-d conjugated MOFs.

中文翻译：

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氢键诱导具有高OER活性的导电π-d共轭FeCo3(DDA)2的超长稳定性

导电π-d共轭金属有机骨架（MOF）由于其固有的高导电性而在电催化领域引起了广泛关注。然而，电催化稳定性差仍然是阻碍MOFs实际应用的一大问题。在此，我们报告了一种增强 MOF 基电催化剂稳定性的新方法，即引入氢键（H 键）。令人印象深刻的是，π-d共轭MOF FeCo ₃ (DDA) ₂表现出超高的析氧反应(OER)稳定性（高达2000小时）。实验研究表明，FeCo ₃ (DDA) ₂中氢键的存在是其超高OER稳定性的原因。除此之外，FeCo ₃ (DDA) ₂还表现出显着的OER活性（在10 mA cm ^-2的电流密度下相对于RHE的过电势为260 mV ，塔菲尔斜率为46.86 mV dec ^-1）。密度泛函理论（DFT）计算进一步表明，FeCo ₃ (DDA) ₂中Fe和Co位点的协同效应有助于其突出的OER性能。这项工作为提高导电π-d共轭MOF的电催化稳定性提供了新途径。