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Coupling nano and atomic electric field confinement for robust alkaline oxygen evolution
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2024-04-29 , DOI: 10.1002/anie.202405438
Qiyou Wang, Yujie Gong, Xin Zi, Lei Gan, Evangelina Pensa, Yuxiang Liu, Yusen Xiao, Hongmei Li, Kang Liu, Junwei Fu, Jun Liu, Andrei Stefancu, Chao Cai, Shanyong Chen, Shiguo Zhang, Ying-Rui Lu, Ting-Shan Chan, Chao Ma, Xueying Cao, Emiliano Cortes, Min Liu

The alkaline oxygen evolution reaction (OER) is a promising avenue for producing clean fuels and storing intermittent energy. However, challenges such as excessive OH– consumption and strong adsorption of oxygen‐containing intermediates hinder the development of alkaline OER. In this study, we propose a cooperative strategy by leveraging both nano‐scale and atomically local electric fields for alkaline OER, demonstrated through the synthesis of Mn single atom doped CoP nanoneedles (Mn SA‐CoP NNs). Finite element method simulations and density functional theory calculations predict that the nano‐scale local electric field enriches OH‐ around the catalyst surface, while the atomically local electric field improves *O desorption. Experimental validation using in situ attenuated total reflection infrared and Raman spectroscopy confirms the effectiveness of the nano‐scale and atomically electric fields. Mn SA‐CoP NNs exhibit an ultra‐low overpotential of 189 mV at 10 mA cm–2 and stable operation over 100 hours at ~100 mA cm–2 during alkaline OER. This innovative strategy provides new insights for enhancing catalyst performance in energy conversion reactions.

中文翻译:

耦合纳米和原子电场限制以实现稳健的碱性氧气析出

碱性析氧反应(OER)是生产清洁燃料和存储间歇性能源的一种有前景的途径。然而,过量的OH-消耗和含氧中间体的强吸附等挑战阻碍了碱性OER的发展。在这项研究中,我们提出了一种利用纳米级和原子局域电场进行碱性 OER 的合作策略,并通过合成 Mn 单原子掺杂 CoP 纳米针(Mn SA-CoP NN)进行了证明。有限元法模拟和密度泛函理论计算预测纳米级局部电场会富集催化剂表面周围的OH-,而原子局部电场会改善*O的解吸。使用原位衰减全反射红外和拉曼光谱的实验验证证实了纳米级和原子电场的有效性。 Mn SA-CoP NN 在 10 mA cm-2 下表现出 189 mV 的超低过电势,并在碱性 OER 过程中在 ~100 mA cm-2 下稳定运行 100 小时以上。这种创新策略为增强能量转换反应中的催化剂性能提供了新的见解。
更新日期:2024-04-29
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