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A general strategy for preparing pyrrolic-N4 type single-atom catalysts via pre-located isolated atoms

Journal Article · · Nature Communications

Single-atom catalysts (SACs) have been applied in many fields due to their superior catalytic performance. Because of the unique properties of the single-atom-site, using the single atoms as catalysts to synthesize SACs is promising. In this work, we have successfully achieved Co1 SAC using Pt1 atoms as catalysts. More importantly, this synthesis strategy can be extended to achieve Fe and Ni SACs as well. X-ray absorption spectroscopy (XAS) results demonstrate that the achieved Fe, Co, and Ni SACs are in a M1-pyrrolic N4 (M= Fe, Co, and Ni) structure. Density functional theory (DFT) studies show that the Co(Cp)2 dissociation is enhanced by Pt1 atoms, thus leading to the formation of Co1 atoms instead of nanoparticles. These SACs are also evaluated under hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and the nature of active sites under HER are unveiled by the operando XAS studies. These new findings extend the application fields of SACs to catalytic fabrication methodology, which is promising for the rational design of advanced SACs.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1833706
Alternate ID(s):
OSTI ID: 1834901
OSTI ID: 1908826
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
ENGLISH

References (52)

Nitrogen-Doped Porous Carbon Nanosheets Templated from g-C 3 N 4 as Metal-Free Electrocatalysts for Efficient Oxygen Reduction Reaction journal May 2016
Defect-Induced Pt-Co-Se Coordinated Sites with Highly Asymmetrical Electronic Distribution for Boosting Oxygen-Involving Electrocatalysis journal November 2018
Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon journal April 2020
A Single-Site Platinum CO Oxidation Catalyst in Zeolite KLTL: Microscopic and Spectroscopic Determination of the Locations of the Platinum Atoms journal July 2014
A Stable Single-Site Palladium Catalyst for Hydrogenations journal July 2015
Atomic-Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co 1 -N 4 Single-Site Photocatalyst journal August 2017
Rational Design of Single Molybdenum Atoms Anchored on N-Doped Carbon for Effective Hydrogen Evolution Reaction journal November 2017
Charge Polarization from Atomic Metals on Adjacent Graphitic Layers for Enhancing the Hydrogen Evolution Reaction journal June 2019
Unveiling the Nature of Pt Single‐Atom Catalyst during Electrocatalytic Hydrogen Evolution and Oxygen Reduction Reactions journal February 2021
Recent Advances for MOF‐Derived Carbon‐Supported Single‐Atom Catalysts journal February 2019
Ultrastable single-atom gold catalysts with strong covalent metal-support interaction (CMSI) journal July 2015
Single-Atom Catalysts: From Design to Application journal August 2019
Graphene Defects Trap Atomic Ni Species for Hydrogen and Oxygen Evolution Reactions journal February 2018
Precisely-controlled synthesis of Au@Pd core–shell bimetallic catalyst via atomic layer deposition for selective oxidation of benzyl alcohol journal April 2015
The PNC/XOR X-ray microprobe station at APS sector 20
  • Heald, S. M.; Cross, J. O.; Brewe, D. L.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 582, Issue 1 https://doi.org/10.1016/j.nima.2007.08.109
journal November 2007
Atomic layer deposition—Sequential self-limiting surface reactions for advanced catalyst “bottom-up” synthesis journal June 2016
Cobaltocene adsorption and dissociation on Cu(111) journal August 2006
Single-Atom Catalysts across the Periodic Table journal October 2020
Single-Atom Catalysts Based on the Metal–Oxide Interaction journal October 2020
Theoretical Understandings of Graphene-based Metal Single-Atom Catalysts: Stability and Catalytic Performance journal October 2020
O 2 Activation by Metal Surfaces: Implications for Bonding and Reactivity on Heterogeneous Catalysts journal November 2017
Chemical Synthesis of Single Atomic Site Catalysts journal April 2020
Supported Single Fe Atoms Prepared via Atomic Layer Deposition for Catalytic Reactions journal February 2020
Experimental Observation of Redox-Induced Fe–N Switching Behavior as a Determinant Role for Oxygen Reduction Activity journal October 2015
Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis journal April 2013
Single-Atom Pd 1 /Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene journal August 2015
Discovering Partially Charged Single-Atom Pt for Enhanced Anti-Markovnikov Alkene Hydrosilylation journal May 2018
Coordination of Atomic Co–Pt Coupling Species at Carbon Defects as Active Sites for Oxygen Reduction Reaction journal July 2018
Cobalt in Nitrogen-Doped Graphene as Single-Atom Catalyst for High-Sulfur Content Lithium–Sulfur Batteries journal February 2019
A General Strategy for Fabricating Isolated Single Metal Atomic Site Catalysts in Y Zeolite journal May 2019
Highly Active and Stable Metal Single-Atom Catalysts Achieved by Strong Electronic Metal–Support Interactions journal September 2019
Ultrahigh-Loading of Ir Single Atoms on NiO Matrix to Dramatically Enhance Oxygen Evolution Reaction journal March 2020
Single-atom catalysis of CO oxidation using Pt1/FeOx journal July 2011
Identification of catalytic sites in cobalt-nitrogen-carbon materials for the oxygen reduction reaction journal October 2017
Golden single-atomic-site platinum electrocatalysts journal September 2018
Reversible and cooperative photoactivation of single-atom Cu/TiO2 photocatalysts journal April 2019
High temperature shockwave stabilized single atoms journal August 2019
Heterogeneous single-atom catalysis journal May 2018
Atomically dispersed iron hydroxide anchored on Pt for preferential oxidation of CO in H2 journal January 2019
Structural and mechanistic basis for the high activity of Fe–N–C catalysts toward oxygen reduction journal January 2016
Continuous and ultrathin platinum films on graphene using atomic layer deposition: a combined computational and experimental study journal January 2016
Highly stable single Pt atomic sites anchored on aniline-stacked graphene for hydrogen evolution reaction journal January 2019
Atomic site electrocatalysts for water splitting, oxygen reduction and selective oxidation journal January 2020
WinXAS : A New Software Package not only for the Analysis of Energy-Dispersive XAS Data journal April 1997
Theoretical understanding of the stability of single-atom catalysts journal September 2018
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
X-ray absorption near-edge structure calculations beyond the muffin-tin approximation journal March 2001
Generalized Gradient Approximation Made Simple journal October 1996
Theoretical approaches to x-ray absorption fine structure journal July 2000
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal June 2005
Thermally stable single-atom platinum-on-ceria catalysts via atom trapping journal July 2016
Atomic Layer Epitaxy of Copper journal January 1998

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