Nanocurvature-induced field effects enable control over the activity of single-atom electrocatalysts

作者：B.X. Wang, Meng Wang, Ziting Fan, Chao Ma, Shibo Xi, Lo‐Yueh Chang, Mingsheng Zhang, Ning Ling, Ziyu Mi, Shenghua Chen, Wan Ru Leow, Jia Zhang, Dingsheng Wang, Yanwei Lum · 发表于：Nature Communications · 年份：2024 · DOI：10.1038/s41467-024-46175-1 · 被引用次数：138 · 研究领域：Electrocatalysts for Energy Conversion、Electrochemical Analysis and Applications、CO2 Reduction Techniques and Catalysts

Abstract Tuning interfacial electric fields provides a powerful means to control electrocatalyst activity. Importantly, electric fields can modify adsorbate binding energies based on their polarizability and dipole moment, and hence operate independently of scaling relations that fundamentally limit performance. However, implementation of such a strategy remains challenging because typical methods modify the electric field non-uniformly and affects only a minority of active sites. Here we discover that uniformly tunable electric field modulation can be achieved using a model system of single-atom catalysts (SACs). These consist of M-N 4 active sites hosted on a series of spherical carbon supports with varying degrees of nanocurvature. Using in-situ Raman spectroscopy with a Stark shift reporter, we demonstrate that a larger nanocurvature induces a stronger electric field. We show that this strategy is effective over a broad range of SAC systems and electrocatalytic reactions. For instance, Ni SACs with optimized nanocurvature achieved a high CO partial current density of ~400 mA cm −2 at >99% Faradaic efficiency for CO 2 reduction in acidic media.