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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics

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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

This summary is machine-generated.

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.

Keywords:

Pt clusters Pt─O─Ti site TiO2 nanoparticles atomic step defects hydrogen evolution reaction

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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.