Abstract High‐efficiency and low‐cost catalysts for oxygen evolution reaction (OER) are critical for electrochemical water splitting to generate hydrogen, which is a clean fuel for sustainable energy conversion and storage. Among the emerging OER catalysts, transition metal dichalcogenides have exhibited superior activity compared to commercial standards such as RuO2, but inferior stability due to uncontrolled restructuring with OER. In this study, we create bimetallic sulfide catalysts by adapting the atomic ratio of Ni and Co in CoxNi1‐xSyelectrocatalysts to investigate the intricate restructuring processes. Surface‐sensitive X‐ray photoelectron spectroscopy and bulk‐sensitive X‐ray absorption spectroscopy confirmed the favorable restructuring of transition metal sulfide material following OER processes. Our results indicate that a small amount of Ni substitution can reshape the Co local electronic structure, which regulates the restructuring process to optimize the balance between OER activity and stability. This work represents a significant advancement in the development of efficient and noble metal‐free OER electrocatalysts through a doping‐regulated restructuring approach.
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Activating the oxygen electrocatalytic activity of layer-structured Ca 0.5 CoO 2 nanofibers by iron doping
The development of low-cost, highly efficient and stable electrocatalysts for the oxygen evolution reaction (OER) is of great significance for many promising energy storage and conversion applications, including metal–air batteries and water splitting technology. Here we report a layer-structured Ca 0.5 CoO 2 nanofibers composed of interconnected ultrathin nanoplates, synthesized using an electrospinning process. The OER activity of Ca 0.5 CoO 2 can be dramatically improved by iron doping, and the overpotential of Ca 0.5 Co 1− x Fe x O 2 ( x = 0.25) is only 346 mV at a current density of 10 mA cm −2 . The mass activity and intrinsic activity of Ca 0.5 Co 0.75 Fe 0.25 O 2 at 1.6 V are, respectively, ∼18.7 and ∼11.4 times higher than those of Ca 0.5 CoO 2 . Iron doping modifies the electronic structure of Ca 0.5 CoO 2 , resulting in partial oxidation of the surface cobalt and increased amount of highly oxidative species (O 2 2− /O 2 ). Consequently, Ca 0.5 Co 0.75 Fe 0.25 O 2 nanofibers with tuned electronic states have shown great potential as cost-effective and efficient electrocatalysts for OER.
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- Award ID(s):
- 1742828
- PAR ID:
- 10334422
- Date Published:
- Journal Name:
- Dalton Transactions
- Volume:
- 51
- Issue:
- 9
- ISSN:
- 1477-9226
- Page Range / eLocation ID:
- 3636 to 3641
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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