Li Bolin, Deng Fulin, Wang Hanlu, Li Zesheng, Yan Fanfei, Yu Changlin
College of Chemistry Engineering, Guangdong University of Petrochemical Technology, Maoming, 525000, China.
Small. 2025 Feb;21(5):e2409542. doi: 10.1002/smll.202409542. Epub 2024 Dec 12.
It is of great significance for the development of hydrogen energy technology by exploring the new-type and high-efficiency electrocatalysts (such as single atom catalysts (SACs)) for water splitting. In this paper, by combining interface engineering and doping engineering, a unique single atom iron (Fe)-doped carbon-coated nickel sulfide (NiS) quantum wires (NiS@Fe-SACs) is prepared as a high-performance bi-functional electrocatalyst for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Theoretical calculation and experimental results show that the addition of atomic Fe species can effectively adjust the electronic structure of sulfide, the interfacial electron transfer modulates the d-band center position, optimizing the transient state of the catalytic process and adsorption energy of hydrogen/oxygen intermediates, and greatly accelerates the kinetics of HER and OER. The results show that the NiS@Fe-SACs core-shell quantum wires array exhibit overpotentials of 46 and 219 mV for HER and OER at 10 mA cm in 1 m KOH, respectively. In addition, the two-electrode electrolyzer assembled by the NiS@Fe-SACs requires a voltage as low as 1.465 V to achieve alkaline overall water splitting of 10 mA cm. This work holds great promise for the development of highly active and highly stable electrocatalysts for future hydrogen energy conversion applications.
探索用于水分解的新型高效电催化剂（如单原子催化剂（SACs））对氢能技术的发展具有重要意义。本文通过结合界面工程和掺杂工程，制备了一种独特的单原子铁（Fe）掺杂碳包覆硫化镍（NiS）量子线（NiS@Fe-SACs）作为用于析氢反应（HER）和析氧反应（OER）的高性能双功能电催化剂。理论计算和实验结果表明，原子级Fe物种的加入可有效调节硫化物的电子结构，界面电子转移调节d带中心位置，优化催化过程的瞬态状态以及氢/氧中间体的吸附能，并极大地加速HER和OER的动力学。结果表明，NiS@Fe-SACs核壳量子线阵列在1 m KOH中，10 mA cm下HER和OER的过电位分别为46和219 mV。此外，由NiS@Fe-SACs组装的双电极电解槽实现10 mA cm碱性全水解所需电压低至1.465 V。这项工作对未来氢能转换应用中高活性和高稳定性电催化剂的开发具有巨大潜力。
