Accelerating Surface Reconstruction in Cobalt Carbodiimides through Structural Defects for Enhanced Oxygen Evolution.
basic_science · Level V
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- Record sourced from PubMed, PMID 41325071.
- Also identified by DOI 10.1021/acsnano.5c16842.
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Abstract
The oxygen evolution reaction (OER) is a vital bottleneck for the conversion of water and clean energy into chemical fuels through electrocatalysis. In-depth insights into the surface structural evolution of real active species on catalysts during the OER process are of great significance for knowledge-driven catalyst design. Herein, we developed iron-doped cobalt carbodiimide (Co<sub><i>x</i></sub>Fe<sub>1-<i>x</i></sub>NCN) nanoparticles as efficient OER precatalysts with stable overpotential for at least 290 h. Advanced structural characterizations disclosed the presence of abundant structural defects in low-crystalline (LC) Co<sub><i>x</i></sub>Fe<sub>1-<i>x</i></sub>NCN. <i>Operando</i> X-ray absorption spectroscopy and X-ray diffraction studies revealed that these intrinsic structural defects could accelerate the irreversible surface reconstruction in LC-Co<sub><i>x</i></sub>Fe<sub>1-<i>x</i></sub>NCN. This promoted the generation of high-valent metal oxyhydroxides as the real active OER phases, resulting in a lower overpotential compared to high-crystalline Co<sub><i>x</i></sub>Fe<sub>1-<i>x</i></sub>NCN. The present study highlights the introduction of structural defects as an effective approach for the rational design of efficient OER electrocatalysts.