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Quantification of Hydrogen Concentrations in Surface and Interface Layers and Bulk Materials through Depth Profiling with Nuclear Reaction Analysis
Published on: March 29, 2016
Site-Dependent Hydrogen Adsorption of Pt Single Atoms for Ampere-Level Alkaline Hydrogen Evolution
Peiyu Ma1,2, Jilong Xu2, Qi Hao3
1School of Chemistry and Chemical Engineering, Anhui University, Hefei, Anhui, People's Republic of China.
Abstract:
The intermediate adsorption on single-atom sites critically governs the catalytic performance of single-atom catalysts. Site-specific single atoms exhibit distinct intrinsic properties that modulate their intermediate adsorption behaviors. Herein, we elucidate the site-dependent hydrogen adsorption of Pt single atoms by anchoring them at oxygen vacancies (PtV/CoOOH), three-fold hollow sites (PtT/CoOOH), and lattice sites (PtL/CoOOH), respectively. Electrochemical measurements demonstrate PtT/CoOOH achieves an overpotential of 8 mV at a current density of 10 mA cm-2 and long-term stability for 1000 h. Anion exchange membrane water electrolyzer (AEMWE) integrated PtT/CoOOH just required 1.90 V to reach the industrial current density of 1.0 A cm-2 with 1000 h stability time. In situ/operando x-ray absorption fine structure (XAFS), ambient pressure x-ray photoelectron spectroscopy (AP-XPS), attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), and theoretical calculations collectively demonstrate that PtT/CoOOH exhibits moderate H2O dissociation kinetics and near-thermoneutral hydrogen binding energy. The optimal hydrogen adsorption facilitated a balanced H adsorption-H2 desorption kinetics, thereby contributing to a superior alkaline hydrogen evolution reaction (HER) activity compared to PtV/CoOOH with weaker hydrogen adsorption and PtL/CoOOH with stronger hydrogen adsorption. This work proposes a precise synthesis strategy to anchor single atoms at diverse sites and elucidates the influence of site-dependent intermediate adsorption on catalytic performance.
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