Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu, Yuanzhi; Sokolowski, Joshua; Song, Xiancheng; He, Yanghua; Mei, Yi; Wu, Gang

doi:10.1002/aenm.201902844

Title: Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Abstract

Abstract Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO ₂ reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.

Authors:

Zhu, Yuanzhi ^[1]; Sokolowski, Joshua ^[2]; Song, Xiancheng ^[1]; He, Yanghua ^[2]; Mei, Yi ^[1];

^[2]

Faculty of Chemical Engineering Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials The Higher Educational Key Laboratory for Phosphorus Chemical Engineering of Yunnan Province Kunming University of Science and Technology Kunming 650500 China
Department of Chemical and Biological Engineering University at Buffalo The State University of New York Buffalo NY 14260 USA

Publication Date:: Fri Dec 20 00:00:00 EST 2019

Sponsoring Org.:: USDOE

OSTI Identifier:: 1580150

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Advanced Energy Materials

Additional Journal Information:: Journal Name: Advanced Energy Materials Journal Volume: 10 Journal Issue: 11; Journal ID: ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Zhu, Yuanzhi, Sokolowski, Joshua, Song, Xiancheng, He, Yanghua, Mei, Yi, and Wu, Gang. Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion.  Germany: N. p., 2019. 
Web.  doi:10.1002/aenm.201902844.

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                    Zhu, Yuanzhi, Sokolowski, Joshua, Song, Xiancheng, He, Yanghua, Mei, Yi, & Wu, Gang. Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion.  Germany.  https://doi.org/10.1002/aenm.201902844

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                    Zhu, Yuanzhi, Sokolowski, Joshua, Song, Xiancheng, He, Yanghua, Mei, Yi, and Wu, Gang. Fri .  
"Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion".  Germany.  https://doi.org/10.1002/aenm.201902844.

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@article{osti_1580150,

  title        = {Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion},

  author       = {Zhu, Yuanzhi and Sokolowski, Joshua and Song, Xiancheng and He, Yanghua and Mei, Yi and Wu, Gang},

  abstractNote = {Abstract Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO 2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.},

  doi          = {10.1002/aenm.201902844},

  journal      = {Advanced Energy Materials},

  number       = 11,

  volume       = 10,

  place        = {Germany},

  year         = {Fri Dec 20 00:00:00 EST 2019},

  month        = {Fri Dec 20 00:00:00 EST 2019}

}

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Abstract

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Ordered Pt ₃ Co Intermetallic Nanoparticles Derived from Metal–Organic Frameworks for Oxygen Reduction
journal, June 2018

3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media
journal, December 2017

Exclusive Ni–N ₄ Sites Realize Near-Unity CO Selectivity for Electrochemical CO ₂ Reduction
journal, October 2017

Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO2
journal, October 2017

Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MN _x Active Moieties Enable Enhanced ORR Performance
journal, August 2018

Systematic exploration of N,C coordination effects on the ORR performance of Mn–N _x doped graphene catalysts based on DFT calculations
journal, January 2019

Correlating the hydrogen evolution reaction activity in alkaline electrolytes with the hydrogen binding energy on monometallic surfaces
journal, January 2013

Precious metal-free approach to hydrogen electrocatalysis for energy conversion: From mechanism understanding to catalyst design
journal, December 2017

Nitrogen-coordinated single Fe sites for efficient electrocatalytic N2 fixation in neutral media
journal, July 2019

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation
journal, January 2019

Synergetic Contribution of Boron and Fe–N _x Species in Porous Carbons toward Efficient Electrocatalysts for Oxygen Reduction Reaction
journal, November 2017

Microwave-Assisted Rapid Synthesis of Graphene-Supported Single Atomic Metals
journal, July 2018

Advances in Electrocatalytic N ₂ Reduction—Strategies to Tackle the Selectivity Challenge
journal, October 2018

Regulating the coordination environment of Co single atoms for achieving efficient electrocatalytic activity in CO2 reduction
journal, January 2019

One-Pot Pyrolysis to N-Doped Graphene with High-Density Pt Single Atomic Sites as Heterogeneous Catalyst for Alkene Hydrosilylation
journal, September 2018

Kinetics of Oxygen Electroreduction on Me–N–C (Me = Fe, Co, Cu) Catalysts in Acidic Medium: Insights on the Effect of the Transition Metal
journal, August 2017

A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
journal, December 2015

O-, N-Atoms-Coordinated Mn Cofactors within a Graphene Framework as Bioinspired Oxygen Reduction Reaction Electrocatalysts
journal, May 2018

Anchoring zero valence single atoms of nickel and iron on graphdiyne for hydrogen evolution
journal, April 2018

Conversion of Dinitrogen to Ammonia by FeN ₃ -Embedded Graphene
journal, July 2016

Zinc-Coordinated Nitrogen-Codoped Graphene as an Efficient Catalyst for Selective Electrochemical Reduction of CO ₂ to CO
journal, July 2018

Atomically Dispersed Iron Cathode Catalysts Derived from Binary Ligand-Based Zeolitic Imidazolate Frameworks with Enhanced Stability for PEM Fuel Cells
journal, January 2019

Nitrogen and Iron-Codoped Carbon Hollow Nanotubules as High-Performance Catalysts toward Oxygen Reduction Reaction: A Combined Experimental and Theoretical Study
journal, June 2017

Atomically dispersed platinum supported on curved carbon supports for efficient electrocatalytic hydrogen evolution
journal, June 2019

A specific demetalation of Fe–N ₄ catalytic sites in the micropores of NC_Ar + NH ₃ is at the origin of the initial activity loss of the highly active Fe/N/C catalyst used for the reduction of oxygen in PEM fuel cells
journal, January 2018

Computational Evaluation of Electrocatalytic Nitrogen Reduction on TM Single-, Double-, and Triple-Atom Catalysts (TM = Mn, Fe, Co, Ni) Based on Graphdiyne Monolayers
journal, July 2019

Carbon‐Supported Divacancy‐Anchored Platinum Single‐Atom Electrocatalysts with Superhigh Pt Utilization for the Oxygen Reduction Reaction
journal, December 2018

Synergistic Effects between Atomically Dispersed Fe−N−C and C−S−C for the Oxygen Reduction Reaction in Acidic Media
journal, September 2017

Doping of Carbon Materials for Metal-Free Electrocatalysis
journal, December 2018

Engineering the Coordination Environment of Single-Atom Platinum Anchored on Graphdiyne for Optimizing Electrocatalytic Hydrogen Evolution
journal, June 2018

Ultralow-temperature photochemical synthesis of atomically dispersed Pt catalysts for the hydrogen evolution reaction
journal, January 2019

Graphitic carbon nitride supported single-atom catalysts for efficient oxygen evolution reaction
journal, January 2016

Fe–N–C Catalyst Graphitic Layer Structure and Fuel Cell Performance
journal, June 2017

In Situ Polymer Graphenization Ingrained with Nanoporosity in a Nitrogenous Electrocatalyst Boosting the Performance of Polymer-Electrolyte-Membrane Fuel Cells
journal, December 2016

Atomic cobalt on nitrogen-doped graphene for hydrogen generation
journal, October 2015

Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
journal, January 2018

Ruthenium atomically dispersed in carbon outperforms platinum toward hydrogen evolution in alkaline media
journal, February 2019

Facile Ammonia Synthesis from Electrocatalytic N ₂ Reduction under Ambient Conditions on N-Doped Porous Carbon
journal, January 2018

Transition metal (Fe, Co, Ni, and Mn) oxides for oxygen reduction and evolution bifunctional catalysts in alkaline media
journal, October 2016

Molecule-Level g-C ₃ N ₄ Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions
journal, February 2017

Carbon‐Rich Nonprecious Metal Single Atom Electrocatalysts for CO ₂ Reduction and Hydrogen Evolution
journal, May 2019

3D porous graphitic nanocarbon for enhancing the performance and durability of Pt catalysts: a balance between graphitization and hierarchical porosity
journal, January 2019

An Isolated Zinc–Cobalt Atomic Pair for Highly Active and Durable Oxygen Reduction
journal, January 2019

Ru nanoassembly catalysts for hydrogen evolution and oxidation reactions in electrolytes at various pH values
journal, December 2019

X‐Ray Absorption Spectroscopy Characterizations on PGM‐Free Electrocatalysts: Justification, Advantages, and Limitations
journal, December 2018

Building Up a Picture of the Electrocatalytic Nitrogen Reduction Activity of Transition Metal Single-Atom Catalysts
journal, April 2019

Facile synthesis of single-nickel-atomic dispersed N-doped carbon framework for efficient electrochemical CO2 reduction
journal, February 2019

Electrochemical CO ₂ Reduction with Atomic Iron-Dispersed on Nitrogen-Doped Graphene
journal, March 2018

Heat-Treated Fe/N/C Catalysts for O₂ Electroreduction: Are Active Sites Hosted in Micropores?
journal, March 2006

Single-atomic cobalt sites embedded in hierarchically ordered porous nitrogen-doped carbon as a superior bifunctional electrocatalyst
journal, November 2018

Surface functionalization of ZIF-8 with ammonium ferric citrate toward high exposure of Fe-N active sites for efficient oxygen and carbon dioxide electroreduction
journal, August 2017

A general route via formamide condensation to prepare atomically dispersed metal–nitrogen–carbon electrocatalysts for energy technologies
journal, January 2019

−60 °C solution synthesis of atomically dispersed cobalt electrocatalyst with superior performance
journal, February 2019

Nitrogen-Doped Graphene-Rich Catalysts Derived from Heteroatom Polymers for Oxygen Reduction in Nonaqueous Lithium–O ₂ Battery Cathodes
journal, October 2012

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction
journal, November 2016

Fe–N–C electrocatalyst with dense active sites and efficient mass transport for high-performance proton exchange membrane fuel cells
journal, March 2019

Single Fe Atom on Hierarchically Porous S, N‐Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn‐Air Batteries
journal, May 2019