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Updated: May 14, 2026

Synthesis of Metal Nanoparticles Supported on Carbon Nanotube with Doped Co and N Atoms and its Catalytic Applications in Hydrogen Production
Published on: December 6, 2021
Spin-state engineering of single-atom cobalt catalysts via carbon nanotube supports enhances catalytic activity
Lingyue Liu1, Yuhang Liu2, Zhuodong Lyu1
1Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, China.
Abstract:
Spin-state plays a crucial role in defining the electronic structure and catalytic reactivity of transition metal catalysts. However, precise manipulation of spin states is challenging, and their impact on catalytic mechanisms remains poorly understood. Here, we show that the curvature of carbon nanotubes (CNTs) tunes the spin state of cobalt phthalocyanine (CoPc) anchored on CNTs, thereby affecting the activity and selectivity in the electroreduction of nitric oxide (NORR) to ammonia. As the CNT diameter falls below 3 nm, the Co2+ center spontaneously transitions from a low-spin (LS) to a high-spin (HS) state. Density functional theory calculations and in situ spectroscopic measurements show that the HS state weakens the N=O bond and promotes bent *NO, which favors NH3 generation. As a result, the optimized catalyst achieves a high partial current density with a Faradaic efficiency of >90% at -0.5 V versus the reversible hydrogen electrode (RHE), while maintaining good stability. This work highlights spin-state engineering via support curvature for selective electrochemical transformations.
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