Hao Yixin, Hung Sung-Fu, Tian Cheng, Wang Luqi, Chen Yi-Yu, Zhao Sheng, Peng Kang-Shun, Zhang Chenchen, Zhang Ying, Kuo Chun-Han, Chen Han-Yi, Peng Shengjie
College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing, 210016, China.
Department of Applied Chemistry, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan.
Angew Chem Int Ed Engl. 2024 Apr 24;63(18):e202402018. doi: 10.1002/anie.202402018. Epub 2024 Mar 12.
Developing ruthenium-based heterogeneous catalysts with an efficient and stable interface is essential for enhanced acidic oxygen evolution reaction (OER). Herein, we report a defect-rich ultrathin boron nitride nanosheet support with relatively independent electron donor and acceptor sites, which serves as an electron reservoir and receiving station for RuO, realizing the rapid supply and reception of electrons. Through precisely controlling the reaction interface, a low OER overpotential of only 180 mV (at 10 mA cm) and long-term operational stability (350 h) are achieved, suggesting potential practical applications. In situ characterization and theoretical calculations have validated the existence of a localized electronic recycling between RuO and ultrathin BN nanosheets (BNNS). The electron-rich Ru sites accelerate the adsorption of water molecules and the dissociation of intermediates, while the interconnection between the O-terminal and B-terminal edge establishes electronic back-donation, effectively suppressing the over-oxidation of lattice oxygen. This study provides a new perspective for constructing a stable and highly active catalytic interface.
开发具有高效且稳定界面的钌基多相催化剂对于增强酸性析氧反应(OER)至关重要。在此,我们报道了一种富含缺陷的超薄氮化硼纳米片载体,其具有相对独立的电子供体和受体位点,可作为RuO的电子储存库和接收站,实现电子的快速供应和接收。通过精确控制反应界面,实现了仅180 mV(在10 mA cm时)的低OER过电位和长期运行稳定性(350 h),表明其具有潜在的实际应用价值。原位表征和理论计算验证了RuO与超薄BN纳米片(BNNS)之间存在局部电子循环。富电子的Ru位点加速了水分子的吸附和中间体的解离,而O端和B端边缘之间的相互连接建立了电子回授,有效抑制了晶格氧的过度氧化。这项研究为构建稳定且高活性的催化界面提供了新的视角。