Moradi Kayvan, Ashrafi Maysam, Salimi Abdollah, Melander Marko M
Department of Chemistry, Nanoscience Center, University of Jyväskylä, P.O. Box 35, Jyväskylä, FI-40014, Finland.
Department of Chemistry, University of Kurdistan, Sanandaj, 66177-15175, Iran.
Small. 2025 Feb;21(8):e2409097. doi: 10.1002/smll.202409097. Epub 2025 Jan 20.
Designing cost-effective electrocatalysts with fast reaction kinetics and high stability is an outstanding challenge in green hydrogen generation through overall water splitting (OWS). Layered double hydroxide (LDH) heterostructure materials are promising candidates to catalyze both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), the two OWS half-cell reactions. This work develops a facile hydrothermal route to synthesiz hierarchical heterostructure MoS@NiFeCo-LDH and MoS@NiFeCo-Mo(doped)-LDH electrocatalysts, which exhibit extremely good OER and HER performance as witnessed by their low IR-corrected overpotentials of 156 and 61 mV with at a current density of 10 mA cm under light assistance. The MoS@NiFeCo-Mo(doped)-LDH-MoS@NiFeCo-LDH OWS cell achieves a low cell voltage of 1.46V at 10 mA cm during light-assisted water electrolysis. Both materials exhibited exceptional stability under industrially relevant HER and OER conditions, maintaining a current density of 1 A cm with minimal alterations in their potential and performance. The experimental and computational results demonstrate that doping the LDH matrix with high-valence Mo atoms and MoS quantum dots improves the electrocatalytic activity by 1) enhancing electron transfer, 2) making the electrocatalyst metallic, 3) increasing the number of active sites, 4) lowering the thermodynamic overpotential, and 5) changing the OER mechanism. Overall, this work develops a facile synthesis method to design highly active and stable MoS@NiFeCo-Mo(doped)-LDH heterostructure electrocatalysts.
设计具有快速反应动力学和高稳定性的经济高效的电催化剂，是通过全水解（OWS）制绿氢过程中的一项重大挑战。层状双氢氧化物（LDH）异质结构材料有望催化析氧反应（OER）和析氢反应（HER）这两个OWS半电池反应。这项工作开发了一种简便的水热路线，以合成分级异质结构的MoS@NiFeCo-LDH和MoS@NiFeCo-Mo（掺杂）-LDH电催化剂，在光辅助下，其在10 mA cm的电流密度下具有156和61 mV的低红外校正过电位，展现出极佳的OER和HER性能。MoS@NiFeCo-Mo（掺杂）-LDH-MoS@NiFeCo-LDH OWS电池在光辅助水电解过程中，在10 mA cm下实现了1.46V的低电池电压。两种材料在工业相关的HER和OER条件下均表现出卓越的稳定性，在电位和性能变化极小的情况下保持1 A cm的电流密度。实验和计算结果表明，用高价Mo原子和MoS量子点掺杂LDH基体，通过以下方式提高了电催化活性：1）增强电子转移；2）使电催化剂具有金属性；3）增加活性位点数量；4）降低热力学过电位；5）改变OER机理。总体而言，这项工作开发了一种简便的合成方法，用于设计高活性和稳定的MoS@NiFeCo-Mo（掺杂）-LDH异质结构电催化剂。
