Yong Feng, Huan Wang, Kun Feng, Chengyu Li, Shuo Li, Cheng Lu, Youyong Li, Ding Ma, Jun Zhong
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引用次数: 0
摘要
在原子水平上操纵催化剂的电子结构是提高催化性能的一种有效但具有挑战性的方法。在这里,通过用插入的 Mo 原子拉伸 FeOOH 中的 Fe-O 键,可以创建一个 Fe-O-Mo 单元,从而在碱性氧进化反应(OER)中诱导形成高价的 Fe4+。原位 X 射线吸收光谱清楚地揭示了高活性 Fe4+ 状态,它既能增强氧化能力,又能为 OER 提供高效稳定的吸附剂进化机制(AEM)途径。因此,所获得的铁-钼-镍-3S2 催化剂具有优异的 OER 活性和出色的稳定性,能在 259 mV 的低过电位(60 °C)下达到 1 A cm-2 的工业级电流密度,并能在大电流下稳定工作 2000 小时以上。此外,通过与商用 Pt/C 的耦合,Fe-Mo-Ni3S2∥Pt/C 系统可用于阴离子交换膜电池,在 1.68 V(4 A cm-2 时为 2.03 V)的电压下获得 1 A cm-2 的整体水分离效果,优于基准 RuO2∥Pt/C 系统。通过操纵原子结构实现的高效、低成本和超稳定 OER 催化剂可能为未来的实用水分离提供潜在的机会。
Atomic Manipulation to Create High-Valent Fe4+ for Efficient and Ultrastable Oxygen Evolution at Industrial-Level Current Density.
Manipulating the electronic structure of a catalyst at the atomic level is an effective but challenging way to improve the catalytic performance. Here, by stretching the Fe-O bond in FeOOH with an inserted Mo atom, a Fe-O-Mo unit can be created, which will induce the formation of high-valent Fe4+ during the alkaline oxygen evolution reaction (OER). The highly active Fe4+ state has been clearly revealed by in situ X-ray absorption spectroscopy, which can both enhance the oxidation capability and lead to an efficient and stable adsorbate evolution mechanism (AEM) pathway for the OER. As a result, the obtained Fe-Mo-Ni3S2 catalyst exhibits both superior OER activity and outstanding stability, which can achieve an industrial-level current density of 1 A cm-2 at a low overpotential of 259 mV (at 60 °C) and can stably work at the large current for more than 2000 h. Moreover, by coupling with commercial Pt/C, the Fe-Mo-Ni3S2∥Pt/C system can be used in the anion exchange membrane cell to acquire 1 A cm-2 for overall water splitting at 1.68 V (2.03 V for 4 A cm-2), outperforming the benchmark RuO2∥Pt/C system. The efficient, low-cost, and ultrastable OER catalyst enabled by manipulating the atomic structure may provide potential opportunities for future practical water splitting.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.