Zhang Huimin, Liu Wenhao, Li Zhenhao, Qiao Liang, Chi Kebin, Guo Xiaoyan, Cao Dong, Cheng Daojian
State Key Laboratory of Organic-Inorganic Composites, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
PetroChina Petrochemical Research Institute, Beijing, 102206, P. R. China.
Adv Sci (Weinh). 2024 Sep;11(35):e2401398. doi: 10.1002/advs.202401398. Epub 2024 Jul 11.
Developing efficient electrocatalysts for water splitting is of great significance for realizing sustainable energy conversion. In this work, Ru sub-nanoclusters anchored on cobalt-nickel bimetallic phosphides (Ru-CoP/NiP) are constructed by an interfacial confinement strategy. Remarkably, Ru-CoP/NiP with low noble metal loading (33.1 µg cm) shows superior activity for hydrogen evolution reaction (HER) in all pH values, whose turnover frequency (TOF) is 8.7, 15.3, and 124.7 times higher than that of Pt/C in acidic, alkaline, and neutral conditions, respectively. Meanwhile, it only requires the overpotential of 171 mV@10 mA cm for oxygen evolution reaction (OER) and corresponding TOF is 20.3 times higher than that of RuO. More importantly, the Ru-CoP/NiP||Ru-CoP/NiP displays superior mass activity of 4017 mA mg at 2.0 V in flowing alkaline water electrolyzer, which is 105.1 times higher than that of Pt/C||IrO. In situ Raman spectroscopy demonstrates that the Ru sites in Ru-CoP/NiP play a key role for water splitting and follow the adsorption evolution mechanism toward OER. Further mechanism studies disclose the confined Ru atom contributes to the desorption of H during HER and the formation of O-O bond during OER, leading to fast reaction kinetics. This study emphasizes the importance of interface confinement for enhancing electrocatalytic activity.
开发用于水分解的高效电催化剂对于实现可持续能源转换具有重要意义。在这项工作中,通过界面限域策略构建了锚定在钴镍双金属磷化物上的钌亚纳米团簇(Ru-CoP/NiP)。值得注意的是,低贵金属负载量(33.1 μg cm)的Ru-CoP/NiP在所有pH值下对析氢反应(HER)均表现出优异的活性,其转换频率(TOF)在酸性、碱性和中性条件下分别比Pt/C高8.7倍、15.3倍和124.7倍。同时,析氧反应(OER)仅需171 mV@10 mA cm的过电位,相应的TOF比RuO高20.3倍。更重要的是,在流动碱性水电解槽中,Ru-CoP/NiP||Ru-CoP/NiP在2.0 V时表现出4017 mA mg的优异质量活性,比Pt/C||IrO高105.1倍。原位拉曼光谱表明,Ru-CoP/NiP中的Ru位点在水分解中起关键作用,并遵循OER的吸附演化机制。进一步的机理研究表明,受限的Ru原子有助于HER过程中H的脱附以及OER过程中O-O键的形成,从而导致快速的反应动力学。这项研究强调了界面限域对增强电催化活性的重要性。