Unveiling the Nature of Pt Single‐Atom Catalyst during Electrocatalytic Hydrogen Evolution and Oxygen Reduction Reactions
Top Cited Papers
- 19 February 2021
- Vol. 17 (11), 2007245
- https://doi.org/10.1002/smll.202007245
Abstract
Single‐atom catalysts (SACs) have attracted significant attention due to their superior catalytic activity and selectivity. However, the nature of active sites of SACs under realistic reaction conditions is ambiguous. In this work, high loading Pt single atoms on graphitic carbon nitride (g‐C3N4)‐derived N‐doped carbon nanosheets (Pt1/NCNS) is achieved through atomic layer deposition. Operando X‐ray absorption spectroscopy (XAS) is performed on Pt single atoms and nanoparticles (NPs) in both the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). The operando results indicate that the total unoccupied density of states of Pt 5d orbitals of Pt1 atoms is higher than that of Pt NPs under HER condition, and that a stable Pt oxide is formed during ORR on Pt1/NCNS, which may suppress the adsorption and activation of O2. This work unveils the nature of Pt single atoms under realistic HER and ORR conditions, providing a deeper understanding for designing advanced SACs.Keywords
Funding Information
- Ballard Power Systems
- Canada Research Chairs
- Canada Foundation for Innovation
- Western University
- Higher Education Discipline Innovation Project ((D17003))
This publication has 37 references indexed in Scilit:
- Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalystNature Communications, 2016
- Single‐Atom Catalyst of Platinum Supported on Titanium Nitride for Selective Electrochemical ReactionsAngewandte Chemie, 2015
- Synchrotron-Based In Situ Characterization of Carbon-Supported Platinum and Platinum Monolayer ElectrocatalystsACS Catalysis, 2015
- Single-Atom Pd1/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-ButadieneJournal of the American Chemical Society, 2015
- Electronic Metal–Support Interactions in Single‐Atom CatalystsAngewandte Chemie, 2014
- Chemical Structure of Nitrogen-Doped Graphene with Single Platinum Atoms and Atomic Clusters as a Platform for the PEMFC ElectrodeThe Journal of Physical Chemistry C, 2014
- Single-Atom Catalysts: A New Frontier in Heterogeneous CatalysisAccounts of Chemical Research, 2013
- Single-atom catalysis of CO oxidation using Pt1/FeOxNature Chemistry, 2011
- In situ X-ray probing reveals fingerprints of surface platinum oxidePhysical Chemistry Chemical Physics, 2010
- Determination of d-band occupancy in pure metals and supported catalysts by measurement of the LIII X-ray absorption thresholdJournal of Catalysis, 1976