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Accelerating Surface Reconstruction in Cobalt Carbodiimides through Structural Defects for Enhanced Oxygen Evolution
Chong Huang1, Carlos A Triana1, Bingquan Jia2
1Department of Chemistry, University of Zurich, Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.
None:
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 (CoxFe1-xNCN) 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) CoxFe1-xNCN. Operando X-ray absorption spectroscopy and X-ray diffraction studies revealed that these intrinsic structural defects could accelerate the irreversible surface reconstruction in LC-CoxFe1-xNCN. This promoted the generation of high-valent metal oxyhydroxides as the real active OER phases, resulting in a lower overpotential compared to high-crystalline CoxFe1-xNCN. The present study highlights the introduction of structural defects as an effective approach for the rational design of efficient OER electrocatalysts.
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