Geng Zekun, Feng Zhiliang, Kong Haoran, Su Jiaqi, Zhang Kaiyan, Li Jiaxin, Sun Xinzhi, Liu Xiaojuan, Ge Lei, Gai Panpan, Li Feng
College of Chemistry and Pharmaceutical Sciences, Qingdao Agricultural University, Qingdao, 266109, China.
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071, China.
Adv Sci (Weinh). 2024 Oct;11(39):e2406843. doi: 10.1002/advs.202406843. Epub 2024 Aug 13.
Developing effective electrocatalysts for the nitrate reduction reaction (NORR) is a promising alternative to conventional industrial ammonia (NH) synthesis. Herein, starting from a flexible laser-induced graphene (LIG) film with hierarchical and interconnected macroporous architecture, a binder-free and free-standing Ru-modified LIG electrode (Ru-LIG) is fabricated for electrocatalytic NORR via a facile electrodeposition method. The relationship between the laser-scribing parameters and the NORR performance of Ru-LIG electrodes is studied in-depth. At -0.59 V, the Ru-LIG electrode exhibited the optimal and stable NORR performance (NH yield rate of 655.9 µg cm h with NH Faradaic efficiency of up to 93.7%) under a laser defocus setting of +2 mm and an applied laser power of 4.8 W, outperforming most of the reported NORR electrodes operated under similar conditions. The optimized laser-scribing parameters promoted the surface properties of LIG with increased graphitization degree and decreased charge-transfer resistance, leading to synergistically improved Ru electrodeposition with more exposed NORR active sites. This work not only provides a new insight to enhance the electrocatalytic NORR performance of LIG-based electrodes via the coordination with metal electrocatalysts as well as identification of the critical laser-scribing parameters but also will inspire the rational design of future advanced laser-induced electrocatalysts for NORR.
开发用于硝酸盐还原反应（NORR）的高效电催化剂是传统工业合成氨的一种有前景的替代方法。在此，从具有分级互连大孔结构的柔性激光诱导石墨烯（LIG）薄膜出发，通过简便的电沉积方法制备了一种无粘结剂且独立的Ru修饰LIG电极（Ru-LIG）用于电催化NORR。深入研究了激光刻写参数与Ru-LIG电极NORR性能之间的关系。在-0.59 V时，Ru-LIG电极在+2 mm的激光散焦设置和4.8 W的施加激光功率下表现出最佳且稳定的NORR性能（NH₃产率为655.9 μg cm⁻² h⁻¹，NH₃法拉第效率高达93.7%），优于大多数在类似条件下运行的已报道NORR电极。优化后的激光刻写参数促进了LIG的表面性质，提高了石墨化程度并降低了电荷转移电阻，从而协同改善了Ru的电沉积，使更多NORR活性位点得以暴露。这项工作不仅为通过与金属电催化剂配位以及确定关键激光刻写参数来提高基于LIG的电极的电催化NORR性能提供了新的见解，还将激发未来用于NORR的先进激光诱导电催化剂的合理设计。
