Lin Lingtong, Zhang Caiyun, Liang Congcong, Zhang Honggang, Wang Zeyan, Wang Peng, Zheng Zhaoke, Cheng Hefeng, Xing Danning, Dai Ying, Huang Baibiao, Liu Yuanyuan
State Key Laboratory of Crystal Materials, Shandong University, Jinan, 250100, China.
Shandong Institute of Advanced Technology, Shandong, 250100, P. R. China.
Adv Mater. 2024 Jul;36(30):e2402388. doi: 10.1002/adma.202402388. Epub 2024 May 16.
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, a novel approach to enhancing the stability of MOF-based electrocatalyst, namely, the introduction of hydrogen bonds (H-bonds), is reported. Impressively, the π-d conjugated MOF FeCo(DDA) (DDA = 1,5-diamino-4,8-dihydroxy-9,10-anthraceneedione) exhibits ultrahigh oxygen evolution reaction (OER) stability (up to 2000 h). The experimental studies demonstrate that the presence of H-bonds in FeCo(DDA) is responsible for its ultrahigh OER stability. Besides that, FeCo(DDA) also displays a prominent OER activity (an overpotential of 260 mV vs reversible hydrogen electrode (RHE) at a current density of 10 mA cm and a Tafel slope of 46.86 mV dec). Density functional theory (DFT) calculations further indicate that the synergistic effect of the Fe and Co sites in FeCo(DDA) contributes to its prominent OER performance. This work provides a new avenue of boosting the electrocatalytic stability of conductive π-d conjugated MOFs.
导电π-d共轭金属有机框架材料（MOFs）因其固有的高导电性在电催化领域引起了广泛关注。然而，较差的电催化稳定性仍然是阻碍MOFs实际应用的一个主要问题。在此，报道了一种提高基于MOF的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（DDA）（DDA = 1,5-二氨基-4,8-二羟基-9,10-蒽二酮）表现出超高的析氧反应（OER）稳定性（长达2000小时）。实验研究表明FeCo（DDA）中H键的存在是其超高OER稳定性的原因。除此之外，FeCo（DDA）还表现出显著的OER活性（在电流密度为10 mA cm时相对于可逆氢电极（RHE）的过电位为260 mV，塔菲尔斜率为46.86 mV dec）。密度泛函理论（DFT）计算进一步表明FeCo（DDA）中Fe和Co位点的协同效应有助于其显著的OER性能。这项工作为提高导电π-d共轭MOFs的电催化稳定性提供了一条新途径。
