Wang Rui, Li Shuhui, Hu Yang, Wu Shanshan, Zhu Jiamin, An Li, Xi Pinxian, Yan Chun-Hua
State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, Frontiers Science Center for Rare Isotopes, College of Chemistry and Chemical Engineering, Lanzhou University Lanzhou 730000 China
Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University Beijing 100871 China.
Chem Sci. 2025 May 15. doi: 10.1039/d5sc02417j.
The pursuit of sustainable energy solutions has identified water oxidation as a crucial reaction, with the oxygen evolution reaction (OER) serving as a decisive efficiency determinant in water technologies. This study presents a novel van der Waals (vdW) heterostructure catalyst, synthesized through a spontaneous self-restacking of nickel-iron-based phosphorus-sulfur compounds (NiPS and FePS). Density Functional Theory (DFT) calculations underpinned the thermodynamic spontaneity of the restacking process, uncovering an electronic transition that significantly amplifies electrocatalytic functionality. The catalyst demonstrates a remarkable OER performance, achieving a low overpotential of 257 mV at 20 mA cm and a Tafel slope of 49 mV dec and demonstrates remarkable durability sustaining 500 mA cm for 140 hours. In addition to its high performance, the material's rapid reconstruction facilitated by surface electron enrichment and the release of phosphate and sulfate during the OER underscores a dual enhancement in both activity and stability. The universality of the synthesis method is further demonstrated by extending the approach to other MPS materials (M = Mn, Co, Zn), establishing a generalized platform for developing high-performance OER catalysts. This work represents a significant advancement in the application of restacked vdW heterostructures as a foundation for advanced electrocatalytic materials.
对可持续能源解决方案的追求已将水氧化确定为关键反应，其中析氧反应（OER）是水技术中决定性的效率决定因素。本研究提出了一种新型范德华（vdW）异质结构催化剂，它是通过镍铁基磷硫化合物（NiPS和FePS）的自发自堆叠合成的。密度泛函理论（DFT）计算支持了堆叠过程的热力学自发性，揭示了一种显著增强电催化功能的电子跃迁。该催化剂表现出卓越的OER性能，在20 mA cm时过电位低至257 mV，塔菲尔斜率为49 mV dec，并且在500 mA cm下可持续140小时，展现出出色的耐久性。除了高性能外，表面电子富集促进的材料快速重构以及OER过程中磷酸盐和硫酸盐的释放突出了活性和稳定性的双重增强。通过将该方法扩展到其他MPS材料（M = Mn、Co、Zn），进一步证明了合成方法的通用性，建立了一个开发高性能OER催化剂的通用平台。这项工作代表了将堆叠vdW异质结构应用于先进电催化材料基础的重大进展。
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