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On the Structure and Redox Behavior of Ni and Cu Single Atoms Supported on Carbon Nitride
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DOI：10.1002/anie.2299555.png)
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Abstract
En 中文
Single-atom catalysts (SACs) offer molecular-level control in heterogeneous catalysis, but their activity depends on whether the support can sustain metal-centered redox cycling. Here, Ni and Cu single atoms on carbon nitride (CNx) are compared to determine how coordination geometry governs redox reversibility and photocatalytic performance. EPR/ENDOR spectroscopy, x-ray absorption, and DFT identify a unique edge MN4 site, composed of three sp2 nitrogens and one bridging sp3 nitrogen, as the binding motif for both metals. While Ni and Cu occupy the same MN4 site in the oxidized state, their redox behavior diverges. Ni preserves a distorted square–planar geometry and undergoes fully reversible Ni2+/Ni+ cycling. In contrast, Cu collapses upon reduction to a low-coordinate Cu+ species that cannot be re-oxidized. This structural mismatch suppresses catalytic turnover. Accordingly, Ni@CNx efficiently promotes photoredox C─N, C─O, and C─S couplings, whereas Cu@CNx remains inactive. Catalytic performance thus depends on redox compatibility within a rigid binding pocket, rather than on metal identity alone.
Keywords:
carbon nitride
catalysis
EPR spectroscopy
nickel
single-atom catalysts
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