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

Bingqing 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 and Yanwei Lum ()
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Bingqing Wang: National University of Singapore
Meng Wang: National University of Singapore
Ziting Fan: National University of Singapore
Chao Ma: Tsinghua University
Shibo Xi: Agency for Science, Technology and Research (A*STAR)
Lo‐Yueh Chang: National Synchrotron Radiation Research Centre
Mingsheng Zhang: Agency for Science, Technology and Research (A*STAR)
Ning Ling: National University of Singapore
Ziyu Mi: Agency for Science, Technology and Research (A*STAR)
Shenghua Chen: Tsinghua University
Wan Ru Leow: Agency for Science, Technology and Research (A*STAR)
Jia Zhang: Agency for Science, Technology, and Research (A*STAR)
Dingsheng Wang: Tsinghua University
Yanwei Lum: National University of Singapore

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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-N4 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 CO2 reduction in acidic media.

Date: 2024
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DOI: 10.1038/s41467-024-46175-1

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