Xuemin Wang, Ming Liu, Na Li, Zhigang Li, Cui Zhang, Shuangxi Liu
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引用次数: 0
摘要
监测活性物种的动态行为并调节其电子结构对于开发高效催化剂至关重要。本文战略性地合成了一种具有 "自我优化效应 "的三维有序多孔 Ni2P/CeO2 异质结催化剂,用于高效氧进化反应(OER)。这种催化剂在 1.0 m KOH 中 20 mA cm-2 的过电位很低,仅为 235 mV。在 OER 过程中,异质结催化剂经历了一个独特的相变过程,其中涉及 P 元素的浸出,这引发了 PO43--NiOOH/CeO2 催化剂的形成,PO43- 吸附在重构产物 NiOOH/CeO2 的表面。密度泛函理论计算表明,自我优化结构中的 CeO2 和吸附的 PO43- 分别是提高催化活性的关键和次要因素。它们共同促进了表面 Ni 和 O 中电子密度的重新分布,增加了 d/p 带中心差。这一现象优化了*OOH 等关键中间产物的吸附/解吸,提高了催化性能。总之,这项研究凸显了 d/p 带调制在合理设计经济高效的电催化剂方面的潜力。
Swelling the d/p-Band Center Difference Induced by Heterostructure Self-Optimization Engineering for Enhanced Water Oxidation
Monitoring the dynamic behavior of active species and modulating their electronic architecture are crucial for the development of efficient catalysts. Here, a 3D ordered multi-level porous Ni2P/CeO2 heterojunction catalyst with a “self-optimization effect” is strategically synthesized for efficient oxygen evolution reaction (OER). This catalyst exhibits a low overpotential of 235 mV at 20 mA cm−2 in 1.0 m KOH. During the OER process, the heterojunction catalyst specifically undergoes a unique phase transition involving the leaching of the P element, which triggers the formation of the PO43−-NiOOH/CeO2 catalyst with PO43− adsorbed on the surface of the reconstructed product NiOOH/CeO2. Density functional theory calculations reveal that the CeO2 and adsorbed-PO43− in the self-optimized structure are essential and minor factors for enhancing catalytic activity, respectively. They collaborate to promote the redistribution of electron density in surface Ni and O, increasing the d/p-band center difference. This phenomenon results in optimized adsorption/desorption of the key intermediates such as *OOH and improved catalytic performance. Overall, this research highlights the potential of d/p-band modulation for the rational design of cost-effective and high-efficiency electrocatalysts.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.