Enhancing Field Effects of Single-Atom Ru/Lignin Carbon Nanoreactors for Electrocatalytic Hydrogen Evolution by Continuous Heterogeneous Curvature.

Abstract

Local electric fields of the electrocatalysts can modulate adsorbate binding energies based on their polarizability and dipole moment, which directly influence the catalytic performance. Nevertheless, implementing the prevailing strategy remains challenging due to the scarcity of active sites and sluggish catalytic kinetics. Herein, a continuous heterogeneous-curvature nanoreactor (HeterC-LCS) is created to enhance local electric fields by optimizing the uniform-nanocurvature with tip effects. The H+ concentration and H2O transmission rate of HeterC-LCS are improved by about 2.1 and 1.7 times that of the homogeneous curvature structure (HomoC-LCS) during the hydrogen evolution reaction (HER) process. Besides, HeterC-LCS demonstrates a rapid kinetics of intermediate transformation and an extremely low energy barrier. Such HeterC-LCS depicts a lowest overpotential of 9.2 mV at 10 mA cm-2, which outperforms all known carbon- and Ru-based electrocatalysts. And the mass activity is approximately 60 times that of commercial Pt/C. This work proposes a novel strategy of uniform-nanocurvature optimized by tip effects toward industrially electrocatalytic HER.