journal article·2021-12Open access

Tailoring the d-band center of N-doped carbon nanotube arrays with Co4N nanoparticles and single-atom Co for a superior hydrogen evolution reaction

Bo Cao, Minghao Hu, Yan Cheng, Peng Jing, Baocang Liu, Bo Zhou, Xi Wang, Rui Gao, Xiaolei Sun, Yaping Du, Jun Zhang

NPG Asia Materials· Volume 13· Issue 1

Abstract

Abstract A 3D self-supported integrated electrode, consisting of heteroatomic nitrogen-doped carbon nanotube arrays on carbon cloth with confined ultrafine Co4N nanoparticles and a distribution of anchored single-atom Co, is fabricated via a cobalt-catalyzed growth strategy using dicyandiamide as the nitrogen and carbon source and a layered cobalt hydroxide-nitrate salt as the precursor. The abundance of exposed active sites, namely, the Co4N nanoparticles, single-atom Co, and heteroatomic N-doped carbon nanotubes, and multiple synergistic effects among these components provide suitable tailoring of thed-band center for facilitating vectorial electron transfer and efficient electrocatalysis. Benefiting from the merits of its structural features and electronic configuration, the prepared electrode exhibits robust performance toward the hydrogen evolution reaction with overpotentials of only 78 and 86 mV at 10 mA cm−2in acidic and basic electrolytes, respectively. Density functional theory calculations and X-ray photoelectron spectroscopy valence band measurements reveal that the effective tailoring of thed-band center by Co4N nanoparticles plays a crucial role in optimizing the hydrogen adsorption free energy to a more thermoneutral value for efficient electrocatalysis.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced battery technologies research · Electrochemical Analysis and Applications

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