Jung Sieon, Senthil Raja Arumugam, Moon Cheol Joo, Kumar Anuj, Ubaidullah Mohd, Choi Myong Yong
Department of Chemistry (BK21 FOUR), Research Institute of Advanced Chemistry, Gyeongsang National University, Jinju, 52828, Republic of Korea.
Core-Facility Center for Photochemistry & Nanomaterials, Gyeongsang National University, Jinju, 52828, Republic of Korea.
Small. 2025 Aug;21(32):e2502821. doi: 10.1002/smll.202502821. Epub 2025 May 2.
Herein, the design and synthesis of Ru-doped CoFe-layered double hydroxide (CoFeRu─LDH) nanostructures is presented via an innovative yet straightforward pulsed laser method. The CoFeRu─LDH catalyst demonstrates outstanding electrocatalytic performance, achieving a high NH Faradaic efficiency (FE) of 89.65% at -0.7 V versus reversible hydrogen electrode for nitrite reduction reaction (NO RR) and a low overpotential of 297 mV at 10 mA cm for oxygen evolution reaction (OER). Comprehensive in situ and ex situ analyses reveal the electrochemically energetic species formed on the CoFeRu─LDH surface during the NO RR and OER. Theoretical studies confirm that Ru doping plays an imperative role in tuning the electronic structure of CoFeRu─LDH, lowering its reaction barriers, and thereby remarkably enhancing its NO RR and OER performance. Specifically, a galvanic Zn-nitrite battery using CoFeRu─LDH as the cathode efficiently converts NO to NH with an FE of 96.8% while concurrently generating electricity with a power density of 4.14 mV cm. Furthermore, pairing CoFeRu─LDH as the anode with Pt/C as the cathode in water electrolysis enables H production at a low cell voltage of 1.57 V at 10 mA cm. This study presents a new pathway to designing versatile, high-performance electrocatalysts for sustainable energy conversion and the production of carbon-free NH and H fuels.
本文通过一种创新且简便的脉冲激光方法，展示了钌掺杂的钴铁层状双氢氧化物（CoFeRu-LDH）纳米结构的设计与合成。CoFeRu-LDH催化剂表现出卓越的电催化性能，在相对于可逆氢电极-0.7 V的电位下，对于亚硝酸盐还原反应（NO RR）实现了89.65%的高NH法拉第效率（FE），并且在析氧反应（OER）中，在10 mA cm时过电位低至297 mV。全面的原位和非原位分析揭示了在NO RR和OER过程中在CoFeRu-LDH表面形成的电化学活性物种。理论研究证实，钌掺杂在调节CoFeRu-LDH的电子结构、降低其反应势垒方面起着至关重要的作用，从而显著提高其NO RR和OER性能。具体而言，使用CoFeRu-LDH作为阴极的原电池锌-亚硝酸盐电池能以96.8%的FE将NO高效转化为NH，同时以4.14 mV cm的功率密度发电。此外，在水电解中将CoFeRu-LDH作为阳极与Pt/C作为阴极配对，能在10 mA cm时以1.57 V的低电池电压产生氢气。这项研究为设计用于可持续能源转换以及生产无碳NH和H燃料的多功能、高性能电催化剂提供了一条新途径。
