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Engineering Interfacial Pt─O─Ti Site at Atomic Step Defect for Efficient Hydrogen Evolution Catalysis
Lei Wang1, Zhelin Mao1, Xin Mao2
1College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, P. R. China.
Small (Weinheim an Der Bergstrasse, Germany)
|December 14, 2023
Summary
Defect-rich TiO2 nanoparticles with atomic platinum clusters show enhanced hydrogen evolution reaction (HER) activity. This breakthrough in catalysis stems from unique Pt-O-Ti linkages at step defects, boosting efficiency beyond benchmarks.
Area of Science:
- Materials Science
- Catalysis
- Nanotechnology
Background:
- The hydrogen evolution reaction (HER) is crucial for clean energy, with catalyst performance often linked to support material defects.
- Understanding the influence of higher-dimensional defects on supported atomic metal species remains a challenge.
Purpose of the Study:
- To investigate the effect of surface step defects in TiO2 nanoparticles on the HER activity of anchored platinum atomic clusters.
- To elucidate the mechanism behind the enhanced catalytic performance.
Main Methods:
- Synthesis of small TiO2 nanoparticles with abundant surface step defects.
- Anchoring of platinum atomic clusters (Pt-ACs) onto TiO2 via Pt-O-Ti linkages.
- Electrochemical characterization of HER activity (mass activity, turnover frequency).
- Spectroscopic analysis and theoretical calculations to understand electronic structure and interactions.
Main Results:
- Pt-ACs/S-TiO2-NP catalysts demonstrated exceptional intrinsic HER activity, with mass activity of 21.46 A mg(Pt)(-1) and turnover frequency of 21.69 s(-1) at 50 mV overpotential.
- Performance significantly surpassed benchmark Pt/C catalysts and other Pt-ACs/TiO2 samples with fewer step sites.
- Step-defect-located Pt-O-Ti sites were identified as key to enhanced charge transfer and optimized d-band center in Pt.
Conclusions:
- Surface step defects on TiO2 nanoparticles effectively direct uniform anchoring of Pt-ACs, creating highly active catalytic sites.
- The Pt-O-Ti linkage at step defects facilitates both proton reduction and hydrogen desorption, leading to superior HER performance.
- This study provides critical insights into defect-metal interactions for designing advanced atomic catalysts for HER.
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