Lyu Chaojie, Cheng Jiarun, Yang Yuquan, Lau Woon-Ming, Wang Ning, Wu Qi, Zheng Jinlong
Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China; Shunde Innovation School, University of Science and Technology Beijing, Foshan, Guangdong 528000, China.
Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China.
J Colloid Interface Sci. 2023 Dec;651:93-105. doi: 10.1016/j.jcis.2023.07.180. Epub 2023 Jul 28.
Modulation of the electronic interaction between the metal and support has been verified as a feasible strategy to improve the electrocatalytic performance of supported-type catalysts. Here, we have successfully synthesized an electrocatalyst of NiP nanoparticles (NPs) anchored on B, N co-doped graphite-like carbon nanosheets (NiP@B, N-GC), and elucidated the main mechanism by which B atoms doping enhances electrocatalytic hydrogen evolution reaction (HER) performance. The B atoms with electron-rich characteristic not only modulate the electronic structure on carbon skeleton, but also regulate the interfacial electronic interaction between NiP NPs and the carbon skeleton, which can lead to the increased available electron density of Ni sites. Such optimization is conducive to accelerating proton transfer and promoting reactive activity. As revealed, the NiP@B, N-GC catalyst with B atoms doping exhibits superior performance to the NiP@N-GC catalyst in acidic, neutral and alkaline medias. In addition, the assembled Ni(OH)@B, N-GC||NiP@B, N-GC electrolyzer displays prominent overall water splitting performance in alkaline solution, which only demands 1.57 V to reach 10 mA/cm, and in complicated natural seawater electrolyte, as low as 1.59 V. Hence, the B atoms doping strategy shows the significant enhancement for HER electrocatalysis.
调节金属与载体之间的电子相互作用已被证实是提高负载型催化剂电催化性能的一种可行策略。在此,我们成功合成了一种锚定在B、N共掺杂类石墨碳纳米片上的NiP纳米颗粒(NPs)电催化剂(NiP@B,N-GC),并阐明了B原子掺杂提高电催化析氢反应(HER)性能的主要机制。具有富电子特性的B原子不仅调节了碳骨架上的电子结构,还调控了NiP NPs与碳骨架之间的界面电子相互作用,这可导致Ni位点的可用电子密度增加。这种优化有利于加速质子转移并促进反应活性。结果表明,掺杂B原子的NiP@B,N-GC催化剂在酸性、中性和碱性介质中均表现出优于NiP@N-GC催化剂的性能。此外,组装的Ni(OH)@B,N-GC||NiP@B,N-GC电解槽在碱性溶液中表现出突出的全水解性能,达到10 mA/cm仅需1.57 V,在复杂的天然海水电解质中低至1.59 V。因此,B原子掺杂策略对HER电催化表现出显著的增强作用。