Zhang Lili, Zhang Ning, Shang Huishan, Sun Zhiyi, Wei Zihao, Wang Jingtao, Lei Yuanting, Wang Xiaochen, Wang Dan, Zhao Yafei, Sun Zhongti, Zhang Fang, Xiang Xu, Zhang Bing, Chen Wenxing
School of Chemical Engineering, Zhengzhou University, Zhengzhou, 450001, P. R. China.
Changchun Institute of Applied Chemistry Chinese Academy of Sciences, Changchun, P. R. China.
Nat Commun. 2024 Nov 1;15(1):9440. doi: 10.1038/s41467-024-53871-5.
Double-atom catalysts (DACs) have opened distinctive paradigms in the field of rapidly developing atomic catalysis owing to their great potential for promoting catalytic performance in various reaction systems. However, increasing the loading and extending the service life of metal active centres represents a considerable challenge for the efficient utilization of DACs. Here, we rationally design asymmetric nitrogen, sulfur-coordinated diatomic iron centres on highly defective nitrogen-doped carbon nanosheets (denoted A-FeSN/SNC, A: asymmetric), which possess the atomic configuration of the NSFe-FeN moiety. The abundant defects and low-electronegativity heteroatoms in the carbon-based framework endow A-FeSN/SNC with a high loading of 6.72 wt%. Furthermore, A-FeSN/SNC has a low overpotential of 193 mV for the oxygen evolution reaction (OER) at 10 mA cm, outperforming commercial RuO catalysts. In addition, A-FeSN/SNC exhibits extraordinary stability, maintaining > 97% activity for over 2000 hours during the OER process. This work provides a practical scheme for simultaneously balancing the activity and stability of DACs towards electrocatalysis applications.
双原子催化剂（DACs）因其在各种反应体系中提升催化性能的巨大潜力，在快速发展的原子催化领域开创了独特的范例。然而，增加金属活性中心的负载量并延长其使用寿命，对DACs的高效利用而言是一项重大挑战。在此，我们在高度缺陷的氮掺杂碳纳米片上合理设计了不对称氮、硫配位的双原子铁中心（表示为A-FeSN/SNC，A：不对称），其具有NSFe-FeN部分的原子构型。碳基框架中丰富的缺陷和低电负性杂原子赋予A-FeSN/SNC高达6.72 wt%的负载量。此外，A-FeSN/SNC在10 mA cm下的析氧反应（OER）过电位低至193 mV，优于商业RuO催化剂。此外，A-FeSN/SNC表现出非凡的稳定性，在OER过程中超过2000小时保持>97%的活性。这项工作为在电催化应用中同时平衡DACs的活性和稳定性提供了一个切实可行的方案。
