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Title: Two-dimensional materials as catalysts for energy conversion

Abstract

Although large efforts have been dedicated to studying two-dimensional materials for catalysis, a rationalization of the associated trends in their intrinsic activity has so far been elusive. In the present work we employ density functional theory to examine a variety of two-dimensional materials, including, carbon based materials, hexagonal boron nitride ( h-BN), transition metal dichalcogenides (e.g. MoS 2, MoSe 2) and layered oxides, to give an overview of the trends in adsorption energies. By examining key reaction intermediates relevant to the oxygen reduction, and oxygen evolution reactions we find that binding energies largely follow the linear scaling relationships observed for pure metals. Here, this observation is very important as it suggests that the same simplifying assumptions made to correlate descriptors with reaction rates in transition metal catalysts are also valid for the studied two-dimensional materials. By means of these scaling relations, for each reaction we also identify several promising candidates that are predicted to exhibit a comparable activity to the state-of-the-art catalysts.

Authors:
 [1];  [2];  [1];  [3];  [2];  [4];  [4];  [4];  [2];  [5]
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Zurich, Zurich (Switzerland)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States); Karlsruhe Inst. of Technology (KIT), Eggenstein-Leopoldshafen (Germany); Karlsruhe Inst. of Technology (KIT), Karlsruhe (Germany)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1348397
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Catalysis Letters
Additional Journal Information:
Journal Volume: 146; Journal Issue: 10; Journal ID: ISSN 1011-372X
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Siahrostami, Samira, Tsai, Charlie, Karamad, Mohammadreza, Koitz, Ralph, García-Melchor, Max, Bajdich, Michal, Vojvodic, Aleksandra, Abild-Pedersen, Frank, Nørskov, Jens K., and Studt, Felix. Two-dimensional materials as catalysts for energy conversion. United States: N. p., 2016. Web. doi:10.1007/s10562-016-1837-z.
Siahrostami, Samira, Tsai, Charlie, Karamad, Mohammadreza, Koitz, Ralph, García-Melchor, Max, Bajdich, Michal, Vojvodic, Aleksandra, Abild-Pedersen, Frank, Nørskov, Jens K., & Studt, Felix. Two-dimensional materials as catalysts for energy conversion. United States. doi:10.1007/s10562-016-1837-z.
Siahrostami, Samira, Tsai, Charlie, Karamad, Mohammadreza, Koitz, Ralph, García-Melchor, Max, Bajdich, Michal, Vojvodic, Aleksandra, Abild-Pedersen, Frank, Nørskov, Jens K., and Studt, Felix. Wed . "Two-dimensional materials as catalysts for energy conversion". United States. doi:10.1007/s10562-016-1837-z. https://www.osti.gov/servlets/purl/1348397.
@article{osti_1348397,
title = {Two-dimensional materials as catalysts for energy conversion},
author = {Siahrostami, Samira and Tsai, Charlie and Karamad, Mohammadreza and Koitz, Ralph and García-Melchor, Max and Bajdich, Michal and Vojvodic, Aleksandra and Abild-Pedersen, Frank and Nørskov, Jens K. and Studt, Felix},
abstractNote = {Although large efforts have been dedicated to studying two-dimensional materials for catalysis, a rationalization of the associated trends in their intrinsic activity has so far been elusive. In the present work we employ density functional theory to examine a variety of two-dimensional materials, including, carbon based materials, hexagonal boron nitride (h-BN), transition metal dichalcogenides (e.g. MoS2, MoSe2) and layered oxides, to give an overview of the trends in adsorption energies. By examining key reaction intermediates relevant to the oxygen reduction, and oxygen evolution reactions we find that binding energies largely follow the linear scaling relationships observed for pure metals. Here, this observation is very important as it suggests that the same simplifying assumptions made to correlate descriptors with reaction rates in transition metal catalysts are also valid for the studied two-dimensional materials. By means of these scaling relations, for each reaction we also identify several promising candidates that are predicted to exhibit a comparable activity to the state-of-the-art catalysts.},
doi = {10.1007/s10562-016-1837-z},
journal = {Catalysis Letters},
issn = {1011-372X},
number = 10,
volume = 146,
place = {United States},
year = {2016},
month = {8}
}

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Cited by: 4 works
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Works referenced in this record:

Benchmarking Hydrogen Evolving Reaction and Oxygen Evolving Reaction Electrocatalysts for Solar Water Splitting Devices
journal, March 2015

  • McCrory, Charles C. L.; Jung, Suho; Ferrer, Ivonne M.
  • Journal of the American Chemical Society, Vol. 137, Issue 13
  • DOI: 10.1021/ja510442p

New directions in science and technology: two-dimensional crystals
journal, July 2011


The New Skinny in Two-Dimensional Nanomaterials
journal, May 2013


The role of defects and doping in 2D graphene sheets and 1D nanoribbons
journal, May 2012


Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction
journal, February 2009


Graphene based new energy materials
journal, January 2011

  • Sun, Yiqing; Wu, Qiong; Shi, Gaoquan
  • Energy & Environmental Science, Vol. 4, Issue 4
  • DOI: 10.1039/c0ee00683a

Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene
journal, March 2013

  • Butler, Sheneve Z.; Hollen, Shawna M.; Cao, Linyou
  • ACS Nano, Vol. 7, Issue 4, p. 2898-2926
  • DOI: 10.1021/nn400280c

Transition-metal doped edge sites in vertically aligned MoS2 catalysts for enhanced hydrogen evolution
journal, January 2015


QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

Graphene: Status and Prospects
journal, June 2009


Functionalization of Graphene for Efficient Energy Conversion and Storage
journal, September 2012


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Cobalt–Iron (Oxy)hydroxide Oxygen Evolution Electrocatalysts: The Role of Structure and Composition on Activity, Stability, and Mechanism
journal, March 2015

  • Burke, Michaela S.; Kast, Matthew G.; Trotochaud, Lena
  • Journal of the American Chemical Society, Vol. 137, Issue 10
  • DOI: 10.1021/jacs.5b00281

Scaling Relationships for Adsorption Energies on Transition Metal Oxide, Sulfide, and Nitride Surfaces
journal, June 2008

  • Fernández, Eva M.; Moses, Poul G.; Toftelund, Anja
  • Angewandte Chemie International Edition, Vol. 47, Issue 25
  • DOI: 10.1002/anie.200705739

Understanding the Reactivity of Layered Transition-Metal Sulfides: A Single Electronic Descriptor for Structure and Adsorption
journal, October 2014

  • Tsai, Charlie; Chan, Karen; Nørskov, Jens K.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 21
  • DOI: 10.1021/jz5020532

Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation
journal, June 2012


Graphene photonics and optoelectronics
journal, August 2010


Boron Nitride Nanosheet on Gold as an Electrocatalyst for Oxygen Reduction Reaction: Theoretical Suggestion and Experimental Proof
journal, April 2014

  • Uosaki, Kohei; Elumalai, Ganesan; Noguchi, Hidenori
  • Journal of the American Chemical Society, Vol. 136, Issue 18
  • DOI: 10.1021/ja500393g

Graphene-based nanomaterials for energy storage
journal, January 2011


Density-Functional-Theory Calculation Analysis of Active Sites for Four-Electron Reduction of O 2 on Fe/N-Doped Graphene
journal, October 2014

  • Liang, Wei; Chen, Junxiang; Liu, Yuwen
  • ACS Catalysis, Vol. 4, Issue 11
  • DOI: 10.1021/cs501170a

Synthesis of MoS2 and MoSe2 Films with Vertically Aligned Layers
journal, February 2013

  • Kong, Desheng; Wang, Haotian; Cha, Judy J.
  • Nano Letters, Vol. 13, Issue 3, p. 1341-1347
  • DOI: 10.1021/nl400258t

Recent Advances in Heteroatom-Doped Metal-Free Electrocatalysts for Highly Efficient Oxygen Reduction Reaction
journal, January 2015


Three dimensional graphene based materials: Synthesis and applications from energy storage and conversion to electrochemical sensor and environmental remediation
journal, July 2015

  • Wang, Hou; Yuan, Xingzhong; Zeng, Guangming
  • Advances in Colloid and Interface Science, Vol. 221
  • DOI: 10.1016/j.cis.2015.04.005

Measurement of the Elastic Properties and Intrinsic Strength of Monolayer Graphene
journal, July 2008


Biomimetic Hydrogen Evolution:  MoS 2 Nanoparticles as Catalyst for Hydrogen Evolution
journal, April 2005

  • Hinnemann, Berit; Moses, Poul Georg; Bonde, Jacob
  • Journal of the American Chemical Society, Vol. 127, Issue 15
  • DOI: 10.1021/ja0504690

Vertical 2D Heterostructures
journal, July 2015


N-doped graphene as catalysts for oxygen reduction and oxygen evolution reactions: Theoretical considerations
journal, May 2014


Theory of multiple proton–electron transfer reactions and its implications for electrocatalysis
journal, January 2013


Molybdenum Sulfides and Selenides as Possible Electrocatalysts for CO 2 Reduction
journal, July 2014


The Oxygen Reduction Reaction on Nitrogen-Doped Graphene
journal, October 2012


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
journal, March 2011

  • Man, Isabela C.; Su, Hai‐Yan; Calle‐Vallejo, Federico
  • ChemCatChem, Vol. 3, Issue 7
  • DOI: 10.1002/cctc.201000397

Electrolysis of water on oxide surfaces
journal, September 2007


Rational design of MoS 2 catalysts: tuning the structure and activity via transition metal doping
journal, January 2015

  • Tsai, Charlie; Chan, Karen; Nørskov, Jens K.
  • Catalysis Science & Technology, Vol. 5, Issue 1
  • DOI: 10.1039/C4CY01162G

Nitrogen-Doped Graphene as Efficient Metal-Free Electrocatalyst for Oxygen Reduction in Fuel Cells
journal, February 2010

  • Qu, Liangti; Liu, Yong; Baek, Jong-Beom
  • ACS Nano, Vol. 4, Issue 3, p. 1321-1326
  • DOI: 10.1021/nn901850u

One-Dimensional Metallic Edge States in MoS 2
journal, October 2001


An overview of graphene in energy production and storage applications
journal, June 2011


Electric Field Effect in Atomically Thin Carbon Films
journal, October 2004


Superior Thermal Conductivity of Single-Layer Graphene
journal, March 2008

  • Balandin, Alexander A.; Ghosh, Suchismita; Bao, Wenzhong
  • Nano Letters, Vol. 8, Issue 3, p. 902-907
  • DOI: 10.1021/nl0731872

Beyond Graphene: Progress in Novel Two-Dimensional Materials and van der Waals Solids
journal, July 2015


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Scaling Properties of Adsorption Energies for Hydrogen-Containing Molecules on Transition-Metal Surfaces
journal, July 2007


Materials for Flexible, Stretchable Electronics: Graphene and 2D Materials
journal, July 2015


Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction
journal, October 2013

  • McCrory, Charles C. L.; Jung, Suho; Peters, Jonas C.
  • Journal of the American Chemical Society, Vol. 135, Issue 45
  • DOI: 10.1021/ja407115p

Homogeneously dispersed multimetal oxygen-evolving catalysts
journal, March 2016


Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting
journal, January 2015

  • Friebel, Daniel; Louie, Mary W.; Bajdich, Michal
  • Journal of the American Chemical Society, Vol. 137, Issue 3
  • DOI: 10.1021/ja511559d

Exploring the active sites of nitrogen-doped graphene as catalysts for the oxygen reduction reaction
journal, September 2014


Gold-supported cerium-doped NiOx catalysts for water oxidation
journal, April 2016

  • Ng, Jia Wei Desmond; García-Melchor, Max; Bajdich, Michal
  • Nature Energy, Vol. 1, Issue 5
  • DOI: 10.1038/nenergy.2016.53

The rise of graphene
journal, March 2007

  • Geim, A. K.; Novoselov, K. S.
  • Nature Materials, Vol. 6, Issue 3, p. 183-191
  • DOI: 10.1038/nmat1849

Recent development in 2D materials beyond graphene
journal, August 2015


Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004

  • Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 46
  • DOI: 10.1021/jp047349j

The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets
journal, April 2013

  • Chhowalla, Manish; Shin, Hyeon Suk; Eda, Goki
  • Nature Chemistry, Vol. 5, Issue 4, p. 263-275
  • DOI: 10.1038/nchem.1589

Universality in Oxygen Reduction Electrocatalysis on Metal Surfaces
journal, July 2012

  • Viswanathan, Venkatasubramanian; Hansen, Heine Anton; Rossmeisl, Jan
  • ACS Catalysis, Vol. 2, Issue 8
  • DOI: 10.1021/cs300227s

Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts
journal, July 2007

  • Jaramillo, T. F.; Jorgensen, K. P.; Bonde, J.
  • Science, Vol. 317, Issue 5834, p. 100-102
  • DOI: 10.1126/science.1141483

A metal-free bifunctional electrocatalyst for oxygen reduction and oxygen evolution reactions
journal, April 2015

  • Zhang, Jintao; Zhao, Zhenghang; Xia, Zhenhai
  • Nature Nanotechnology, Vol. 10, Issue 5
  • DOI: 10.1038/nnano.2015.48

Origin of the Electrocatalytic Oxygen Reduction Activity of Graphene-Based Catalysts: A Roadmap to Achieve the Best Performance
journal, March 2014

  • Jiao, Yan; Zheng, Yao; Jaroniec, Mietek
  • Journal of the American Chemical Society, Vol. 136, Issue 11
  • DOI: 10.1021/ja500432h

Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
journal, September 2009

  • Greeley, J.; Stephens, I. E. L.; Bondarenko, A. S.
  • Nature Chemistry, Vol. 1, Issue 7, p. 552-556
  • DOI: 10.1038/nchem.367