Multiscale Confinement Engineering for Boosting Overall Water Splitting by One-Step Stringing of a Single Atom and a Janus Nanoparticle within a Carbon Nanotube

作者：Quan, Quan; Zhang, Yuxuan; Li, Shaohai^*; Yip, Senpo; Wang, Wei; Xie, Pengshan; Chen, Dong; Wang, Weijun; Yin, Di; Li, Yezhan; Liu, Bilu; Ho, Johnny C.^*

来源：ACS Nano, 2023, 18(1): 1204-1213.

DOI：10.1021/acsnano.3c11705

• confinement
• single atom
• Janus nanoparticle
• carbon nanotube
• overallwater splitting

Enzyme-mimicking confined catalysis has attracted great interest in heterogeneous catalytic systems that can regulate the geometric or electronic structure of the active site and improve its performance. Herein, a liquid-assisted chemical vapor deposition (LCVD) strategy is proposed to simultaneously confine the single-atom Ru sites onto sidewalls and Janus Ni/NiO nanoparticles (NPs) at the apical nanocavities to thoroughly energize the N-doped carbon nanotube arrays (denoted as Ni/NiO@Ru-NC). The bifunctional Ni/NiO@Ru-NC electrocatalyst exhibits overpotentials of 88 and 261 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at 100 mA cm(-2) in alkaline solution, respectively, all ranking the top tier among the carbon-supported metal-based electrocatalysts. Moreover, once integrated into an anion-exchange membrane water electrolysis (AEMWE) system, Ni/NiO@Ru-NC can act as an efficient and robust bifunctional electrocatalyst to operate stably for 50 h under 500 mA cm(-2). Theoretical calculations and experimental exploration demonstrate that the confinement of Ru single atoms and Janus Ni/NiO NPs can regulate the electron distribution with strong orbital couplings to activate the NC nanotube from sidewall to top, thus boosting overall water splitting.

• 单位
  清华大学