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Anion Structure Regulation of Cobalt Silicate Hydroxide Endowing Boosted Oxygen Evolution Reaction
Yang Wang1, Longmei Li1, Shengguo Wang1
1School of Chemistry, Dalian University of Technology, Dalian, 116024, China.
Introducing silicate vacancies in cobalt silicate hydroxide (CoSi) enhances its performance as an electrocatalyst for the oxygen evolution reaction (OER). This anionic regulation boosts catalytic activity and conductivity, offering a new path for non-noble metal catalysts.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Transition metal silicates (TMSs) show promise as electrocatalysts for the oxygen evolution reaction (OER) due to their layered structures.
- However, limitations in theoretical activity and conductivity hinder their practical application.
- Current strategies often involve compositing TMSs with other materials, neglecting intrinsic structural modifications.
Purpose of the Study:
- To investigate the impact of intrinsic anionic structure regulation on the electrocatalytic activity of cobalt silicate hydroxide (CoSi) for OER.
- To introduce and characterize silicate vacancies in CoSi to enhance catalytic site availability and activity.
- To elucidate the mechanism behind the improved OER performance through computational analysis.
Main Methods:
- Interference hydrolysis and vacancy reserve methods were employed to synthesize silicate vacancy-modified cobalt silicate hydroxide (SV-CoSi).
- Electrochemical performance for OER was evaluated, including overpotential measurements at a current density of 10 mA cm⁻².
- Density functional theory (DFT) was utilized to analyze the electronic structure and understand the origin of enhanced catalytic activity.
Main Results:
- The synthesized SV-CoSi exhibited a significantly reduced overpotential of 301 mV at 10 mA cm⁻², compared to 438 mV for pristine CoSi.
- The improvement in OER performance was attributed to both an increased number of active sites and enhanced intrinsic activity.
- DFT calculations confirmed that the anion structure variation, specifically the introduction of silicate vacancies, strengthens cobalt-oxygen covalence.
Conclusions:
- Intrinsic anionic structure regulation, specifically the introduction of silicate vacancies, is an effective strategy to improve the OER performance of transition metal silicates.
- SV-CoSi demonstrates superior electrocatalytic activity for OER compared to unmodified CoSi.
- This work provides a novel approach for designing efficient non-noble metal electrocatalysts for OER by manipulating the intrinsic anionic structure.
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