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Title: Bridging the Homogeneous-Heterogeneous Divide: Modeling Spin for Reactivity in Single Atom Catalysis

Abstract

Single atom catalysts (SACs) are emergent catalytic materials that have the promise of merging the scalability of heterogeneous catalysts with the high activity and atom economy of homogeneous catalysts. Computational, first-principles modeling can provide essential insight into SAC mechanism and active site configuration, where the sub-nm-scale environment can challenge even the highest-resolution experimental spectroscopic techniques. Nevertheless, the very properties that make SACs attractive in catalysis, such as localized d electrons of the isolated transition metal center, make them challenging to study with conventional computational modeling using density functional theory (DFT). For example, Fe/N-doped graphitic SACs have exhibited spin-state dependent reactivity that remains poorly understood. However, spin-state ordering in DFT is very sensitive to the nature of the functional approximation chosen. In this work, we develop accurate benchmarks from correlated wavefunction theory (WFT) for relevant octahedral complexes. We use those benchmarks to evaluate optimal DFT functional choice for predicting spin state ordering in small octahedral complexes as well as models of pyridinic and pyrrolic nitrogen environments expected in larger SACs. Using these guidelines, we determine Fe/N-doped graphene SAC model properties and reactivity as well as their sensitivities to DFT functional choice. Finally, we conclude with broad recommendations for computational modeling ofmore » open-shell transition metal single-atom catalysts.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF)
OSTI Identifier:
1507204
Alternate Identifier(s):
OSTI ID: 1612844
Grant/Contract Number:  
SC0018096; CBET-1704266
Resource Type:
Published Article
Journal Name:
Frontiers in Chemistry
Additional Journal Information:
Journal Name: Frontiers in Chemistry Journal Volume: 7; Journal ID: ISSN 2296-2646
Publisher:
Frontiers Research Foundation
Country of Publication:
Switzerland
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; density functional theory; catalysis; single atom catalysis; spin state crossover; transition metal chemistry

Citation Formats

Liu, Fang, Yang, Tzuhsiung, Yang, Jing, Xu, Eve, Bajaj, Akash, and Kulik, Heather J. Bridging the Homogeneous-Heterogeneous Divide: Modeling Spin for Reactivity in Single Atom Catalysis. Switzerland: N. p., 2019. Web. doi:10.3389/fchem.2019.00219.
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Liu, Fang, Yang, Tzuhsiung, Yang, Jing, Xu, Eve, Bajaj, Akash, & Kulik, Heather J. Bridging the Homogeneous-Heterogeneous Divide: Modeling Spin for Reactivity in Single Atom Catalysis. Switzerland. https://doi.org/10.3389/fchem.2019.00219
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Liu, Fang, Yang, Tzuhsiung, Yang, Jing, Xu, Eve, Bajaj, Akash, and Kulik, Heather J. Tue . "Bridging the Homogeneous-Heterogeneous Divide: Modeling Spin for Reactivity in Single Atom Catalysis". Switzerland. https://doi.org/10.3389/fchem.2019.00219.
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@article{osti_1507204,
title = {Bridging the Homogeneous-Heterogeneous Divide: Modeling Spin for Reactivity in Single Atom Catalysis},
author = {Liu, Fang and Yang, Tzuhsiung and Yang, Jing and Xu, Eve and Bajaj, Akash and Kulik, Heather J.},
abstractNote = {Single atom catalysts (SACs) are emergent catalytic materials that have the promise of merging the scalability of heterogeneous catalysts with the high activity and atom economy of homogeneous catalysts. Computational, first-principles modeling can provide essential insight into SAC mechanism and active site configuration, where the sub-nm-scale environment can challenge even the highest-resolution experimental spectroscopic techniques. Nevertheless, the very properties that make SACs attractive in catalysis, such as localized d electrons of the isolated transition metal center, make them challenging to study with conventional computational modeling using density functional theory (DFT). For example, Fe/N-doped graphitic SACs have exhibited spin-state dependent reactivity that remains poorly understood. However, spin-state ordering in DFT is very sensitive to the nature of the functional approximation chosen. In this work, we develop accurate benchmarks from correlated wavefunction theory (WFT) for relevant octahedral complexes. We use those benchmarks to evaluate optimal DFT functional choice for predicting spin state ordering in small octahedral complexes as well as models of pyridinic and pyrrolic nitrogen environments expected in larger SACs. Using these guidelines, we determine Fe/N-doped graphene SAC model properties and reactivity as well as their sensitivities to DFT functional choice. Finally, we conclude with broad recommendations for computational modeling of open-shell transition metal single-atom catalysts.},
doi = {10.3389/fchem.2019.00219},
journal = {Frontiers in Chemistry},
number = ,
volume = 7,
place = {Switzerland},
year = {Tue Apr 16 00:00:00 EDT 2019},
month = {Tue Apr 16 00:00:00 EDT 2019}
}
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https://doi.org/10.3389/fchem.2019.00219
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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Evidence of two-state reactivity in alkane hydroxylation by Lewis-acid bound copper–nitrene complexes
journal, January 2014

  • Abram, Sarah-Luise; Monte-Pérez, Inés; Pfaff, Florian Felix
  • Chem. Commun., Vol. 50, Issue 69
  • DOI: 10.1039/C4CC03754E

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Spectroscopic Characterization and Reactivity of Triplet and Quintet Iron(IV) Oxo Complexes in the Gas Phase
journal, February 2016

  • Andris, Erik; Jašík, Juraj; Gómez, Laura
  • Angewandte Chemie International Edition, Vol. 55, Issue 11
  • DOI: 10.1002/anie.201511374

UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992

  • Rappe, A. K.; Casewit, C. J.; Colwell, K. S.
  • Journal of the American Chemical Society, Vol. 114, Issue 25, p. 10024-10035
  • DOI: 10.1021/ja00051a040

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

Ménage-à-trois: single-atom catalysis, mass spectrometry, and computational chemistry
journal, January 2017

  • Schwarz, Helmut
  • Catalysis Science & Technology, Vol. 7, Issue 19
  • DOI: 10.1039/C6CY02658C

Computational Support for Phillips Catalyst Initiation via Cr–C Bond Homolysis in a Chromacyclopentane Site
journal, January 2018

Auxiliary basis sets to approximate Coulomb potentials
journal, June 1995

Predicting electronic structure properties of transition metal complexes with neural networks
journal, January 2017

  • Janet, Jon Paul; Kulik, Heather J.
  • Chemical Science, Vol. 8, Issue 7
  • DOI: 10.1039/C7SC01247K

Perspective: Treating electron over-delocalization with the DFT+U method
journal, June 2015

  • Kulik, Heather J.
  • The Journal of Chemical Physics, Vol. 142, Issue 24
  • DOI: 10.1063/1.4922693

How to select active space for multiconfigurational quantum chemistry?
journal, April 2011

  • Veryazov, Valera; Malmqvist, Per Åke; Roos, Björn O.
  • International Journal of Quantum Chemistry, Vol. 111, Issue 13
  • DOI: 10.1002/qua.23068

A modified definition of the zeroth-order Hamiltonian in multiconfigurational perturbation theory (CASPT2)
journal, September 2004

Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)]
journal, June 2006

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 124, Issue 21
  • DOI: 10.1063/1.2204597

Identification of catalytic sites in cobalt-nitrogen-carbon materials for the oxygen reduction reaction
journal, October 2017

  • Zitolo, Andrea; Ranjbar-Sahraie, Nastaran; Mineva, Tzonka
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/s41467-017-01100-7

molSimplify: A toolkit for automating discovery in inorganic chemistry
journal, July 2016

  • Ioannidis, Efthymios I.; Gani, Terry Z. H.; Kulik, Heather J.
  • Journal of Computational Chemistry, Vol. 37, Issue 22
  • DOI: 10.1002/jcc.24437

Co-synthesis of atomic Fe and few-layer graphene towards superior ORR electrocatalyst
journal, May 2018

Unifying Exchange Sensitivity in Transition-Metal Spin-State Ordering and Catalysis through Bond Valence Metrics
journal, October 2017

  • Gani, Terry Z. H.; Kulik, Heather J.
  • Journal of Chemical Theory and Computation, Vol. 13, Issue 11
  • DOI: 10.1021/acs.jctc.7b00848

Unveiling the high-activity origin of single-atom iron catalysts for oxygen reduction reaction
journal, June 2018

  • Yang, Liu; Cheng, Daojian; Xu, Haoxiang
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 26
  • DOI: 10.1073/pnas.1800771115

Dipole correction for surface supercell calculations
journal, May 1999

Isolated Single Iron Atoms Anchored on N-Doped Porous Carbon as an Efficient Electrocatalyst for the Oxygen Reduction Reaction
journal, April 2017

  • Chen, Yuanjun; Ji, Shufang; Wang, Yanggang
  • Angewandte Chemie, Vol. 129, Issue 24
  • DOI: 10.1002/ange.201702473

Accurate Coulomb-fitting basis sets for H to Rn
journal, January 2006

  • Weigend, Florian
  • Physical Chemistry Chemical Physics, Vol. 8, Issue 9
  • DOI: 10.1039/b515623h

On the zeroth-order hamiltonian for CASPT2 calculations of spin crossover compounds: Spin State Energetics of FeN
journal, December 2015

  • Vela, Sergi; Fumanal, Maria; Ribas-Ariño, Jordi
  • Journal of Computational Chemistry, Vol. 37, Issue 10
  • DOI: 10.1002/jcc.24283

Where Does the Density Localize? Convergent Behavior for Global Hybrids, Range Separation, and DFT+U
journal, November 2016

  • Gani, Terry Z. H.; Kulik, Heather J.
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 12
  • DOI: 10.1021/acs.jctc.6b00937

Multiconfiguration perturbation theory with imaginary level shift
journal, August 1997

A universal principle for a rational design of single-atom electrocatalysts
journal, April 2018

Communication: Evaluating non-empirical double hybrid functionals for spin-state energetics in transition-metal complexes
journal, January 2018

  • Wilbraham, Liam; Adamo, Carlo; Ciofini, Ilaria
  • The Journal of Chemical Physics, Vol. 148, Issue 4
  • DOI: 10.1063/1.5019641

A theoretical study of spin states in Ni-S4 complexes and models of the [NiFe] hydrogenase active site
journal, September 2004

  • Bruschi, Maurizio; De Gioia, Luca; Zampella, Giuseppe
  • JBIC Journal of Biological Inorganic Chemistry, Vol. 9, Issue 7
  • DOI: 10.1007/s00775-004-0588-2

Comparison of two efficient approximate Hartee–Fock approaches
journal, October 2009

Spin States and Other Ligand–Field States of Aqua Complexes Revisited with Multireference ab Initio Calculations Including Solvation Effects
journal, June 2018

  • Radoń, Mariusz; Drabik, Gabriela
  • Journal of Chemical Theory and Computation, Vol. 14, Issue 8
  • DOI: 10.1021/acs.jctc.8b00200

Graphene Defects Trap Atomic Ni Species for Hydrogen and Oxygen Evolution Reactions
journal, February 2018

Understanding and Breaking Scaling Relations in Single-Site Catalysis: Methane to Methanol Conversion by Fe IV ═O
journal, January 2018

Challenges for Density Functional Theory
journal, December 2011

  • Cohen, Aron J.; Mori-Sánchez, Paula; Yang, Weitao
  • Chemical Reviews, Vol. 112, Issue 1
  • DOI: 10.1021/cr200107z

Assessment of electronic structure methods for the determination of the ground spin states of Fe( ii ), Fe( iii ) and Fe( iv ) complexes
journal, January 2017

  • Verma, Pragya; Varga, Zoltan; Klein, Johannes E. M. N.
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 20
  • DOI: 10.1039/C7CP01263B

Single-Atom Electrocatalysts
journal, October 2017

  • Zhu, Chengzhou; Fu, Shaofang; Shi, Qiurong
  • Angewandte Chemie International Edition, Vol. 56, Issue 45
  • DOI: 10.1002/anie.201703864

Two-State Reactivity as a New Concept in Organometallic Chemistry §
journal, March 2000

  • Schröder, Detlef; Shaik, Sason; Schwarz, Helmut
  • Accounts of Chemical Research, Vol. 33, Issue 3
  • DOI: 10.1021/ar990028j

Optimized accurate auxiliary basis sets for RI-MP2 and RI-CC2 calculations for the atoms Rb to Rn
journal, January 2007

  • Hellweg, Arnim; Hättig, Christof; Höfener, Sebastian
  • Theoretical Chemistry Accounts, Vol. 117, Issue 4
  • DOI: 10.1007/s00214-007-0250-5

Software update: the ORCA program system, version 4.0: Software update
journal, July 2017

  • Neese, Frank
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 8, Issue 1
  • DOI: 10.1002/wcms.1327

Comparison of density functionals for differences between the high- (T2g5) and low- (A1g1) spin states of iron(II) compounds. IV. Results for the ferrous complexes [Fe(L)(‘NHS4’)]
journal, June 2005

  • Ganzenmüller, Georg; Berkaïne, Nabil; Fouqueau, Antony
  • The Journal of Chemical Physics, Vol. 122, Issue 23
  • DOI: 10.1063/1.1927081

Spin Propensities of Octahedral Complexes From Density Functional Theory
journal, April 2015

  • Mortensen, Sara R.; Kepp, Kasper P.
  • The Journal of Physical Chemistry A, Vol. 119, Issue 17
  • DOI: 10.1021/acs.jpca.5b01626

A Theoretical Study on the Mechanism of Camphor Hydroxylation by Compound I of Cytochrome P450
journal, April 2003

  • Kamachi, Takashi; Yoshizawa, Kazunari
  • Journal of the American Chemical Society, Vol. 125, Issue 15
  • DOI: 10.1021/ja0208862

Drug Metabolism by Cytochrome P450 Enzymes: What Distinguishes the Pathways Leading to Substrate Hydroxylation Over Desaturation?
journal, April 2015

  • Ji, Li; Faponle, Abayomi S.; Quesne, Matthew G.
  • Chemistry - A European Journal, Vol. 21, Issue 25
  • DOI: 10.1002/chem.201500329

Spin-forbidden reactions: computational insight into mechanisms and kinetics: Spin-forbidden reactions
journal, June 2013

  • Harvey, Jeremy N.
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 4, Issue 1
  • DOI: 10.1002/wcms.1154

Assessment of density functional theory for iron(II) molecules across the spin-crossover transition
journal, September 2012

  • Droghetti, A.; Alfè, D.; Sanvito, S.
  • The Journal of Chemical Physics, Vol. 137, Issue 12
  • DOI: 10.1063/1.4752411

Structure of graphite by neutron diffraction
journal, November 1975

A ?Level-Shifting? method for converging closed shell Hartree-Fock wave functions
journal, July 1973

  • Saunders, V. R.; Hillier, I. H.
  • International Journal of Quantum Chemistry, Vol. 7, Issue 4
  • DOI: 10.1002/qua.560070407

Low-Spin versus High-Spin Ground State in Pseudo-Octahedral Iron Complexes
journal, May 2012

  • Bowman, David N.; Jakubikova, Elena
  • Inorganic Chemistry, Vol. 51, Issue 11
  • DOI: 10.1021/ic202344w

Molcas 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table : Molcas 8
journal, November 2015

  • Aquilante, Francesco; Autschbach, Jochen; Carlson, Rebecca K.
  • Journal of Computational Chemistry, Vol. 37, Issue 5
  • DOI: 10.1002/jcc.24221

Embedding Transition-Metal Atoms in Graphene: Structure, Bonding, and Magnetism
journal, March 2009

Direct oxidation of methane to methanol on Fe–O modified graphene
journal, January 2014

  • Impeng, Sarawoot; Khongpracha, Pipat; Warakulwit, Chompunuch
  • RSC Adv., Vol. 4, Issue 24
  • DOI: 10.1039/C3RA47826B

Optimized pseudopotentials
journal, January 1990

  • Rappe, Andrew M.; Rabe, Karin M.; Kaxiras, Efthimios
  • Physical Review B, Vol. 41, Issue 2
  • DOI: 10.1103/PhysRevB.41.1227

Density Functional Theory in Transition-Metal Chemistry: A Self-Consistent Hubbard U Approach
journal, September 2006

Efficient and accurate local approximations to coupled-electron pair approaches: An attempt to revive the pair natural orbital method
journal, March 2009

  • Neese, Frank; Wennmohs, Frank; Hansen, Andreas
  • The Journal of Chemical Physics, Vol. 130, Issue 11
  • DOI: 10.1063/1.3086717

Where Does the Density Localize in the Solid State? Divergent Behavior for Hybrids and DFT+U
journal, January 2018

  • Zhao, Qing; Kulik, Heather J.
  • Journal of Chemical Theory and Computation, Vol. 14, Issue 2
  • DOI: 10.1021/acs.jctc.7b01061

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

  • Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9668

A Simple Approach for Predicting the Spin State of Homoleptic Fe(II) Tris-diimine Complexes
journal, April 2017

  • Phan, Hoa; Hrudka, Jeremy J.; Igimbayeva, Dilyara
  • Journal of the American Chemical Society, Vol. 139, Issue 18
  • DOI: 10.1021/jacs.7b02098

On some approximations in applications of X α theory
journal, October 1979

  • Dunlap, B. I.; Connolly, J. W. D.; Sabin, J. R.
  • The Journal of Chemical Physics, Vol. 71, Issue 8
  • DOI: 10.1063/1.438728

The Power of Single-Atom Catalysis
journal, August 2015

Quantum Mechanics/Molecular Mechanics Study on the Oxygen Binding and Substrate Hydroxylation Step in AlkB Repair Enzymes
journal, December 2013

  • Quesne, Matthew G.; Latifi, Reza; Gonzalez-Ovalle, Luis E.
  • Chemistry - A European Journal, Vol. 20, Issue 2
  • DOI: 10.1002/chem.201303282

Ligand-Field-Dependent Behavior of Meta-GGA Exchange in Transition-Metal Complex Spin-State Ordering
journal, October 2016

  • Ioannidis, Efthymios I.; Kulik, Heather J.
  • The Journal of Physical Chemistry A, Vol. 121, Issue 4
  • DOI: 10.1021/acs.jpca.6b11930

Support effects on adsorption and catalytic activation of O 2 in single atom iron catalysts with graphene-based substrates
journal, January 2018

  • Gao, Zheng-yang; Yang, Wei-jie; Ding, Xun-lei
  • Physical Chemistry Chemical Physics, Vol. 20, Issue 10
  • DOI: 10.1039/C7CP08301G

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011

Quantum electrodynamical corrections to the fine structure of helium
journal, January 1974

Second‐order perturbation theory with a complete active space self‐consistent field reference function
journal, January 1992

  • Andersson, Kerstin; Malmqvist, Per‐Åke; Roos, Björn O.
  • The Journal of Chemical Physics, Vol. 96, Issue 2
  • DOI: 10.1063/1.462209

Main Group Atoms and Dimers Studied with a New Relativistic ANO Basis Set
December 2003

Coulombic potential energy integrals and approximations
journal, May 1973

  • Whitten, J. L.
  • The Journal of Chemical Physics, Vol. 58, Issue 10
  • DOI: 10.1063/1.1679012

Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis
journal, April 2013

  • Yang, Xiao-Feng; Wang, Aiqin; Qiao, Botao
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar300361m

Towards quantifying the role of exact exchange in predictions of transition metal complex properties
journal, July 2015

  • Ioannidis, Efthymios I.; Kulik, Heather J.
  • The Journal of Chemical Physics, Vol. 143, Issue 3
  • DOI: 10.1063/1.4926836

Auxiliary basis sets for main row atoms and transition metals and their use to approximate Coulomb potentials
journal, October 1997

  • Eichkorn, Karin; Weigend, Florian; Treutler, Oliver
  • Theoretical Chemistry Accounts: Theory, Computation, and Modeling (Theoretica Chimica Acta), Vol. 97, Issue 1-4
  • DOI: 10.1007/s002140050244

Single-atom catalysis of CO oxidation using Pt1/FeOx
journal, July 2011

  • Qiao, Botao; Wang, Aiqin; Yang, Xiaofeng
  • Nature Chemistry, Vol. 3, Issue 8
  • DOI: 10.1038/nchem.1095

Single-atom catalysts for CO 2 electroreduction with significant activity and selectivity improvements
journal, January 2017

  • Back, Seoin; Lim, Juhyung; Kim, Na-Young
  • Chemical Science, Vol. 8, Issue 2
  • DOI: 10.1039/C6SC03911A

Absorption Spectra of Co-ordination Compounds. I
journal, May 1938

  • Tsuchida, Ryutaro
  • Bulletin of the Chemical Society of Japan, Vol. 13, Issue 5
  • DOI: 10.1246/bcsj.13.388

Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium
journal, June 2017

Catalytic Mechanism of Cofactor-Free Dioxygenases and How They Circumvent Spin-Forbidden Oxygenation of Their Substrates
journal, June 2015

  • Hernández-Ortega, Aitor; Quesne, Matthew G.; Bui, Soi
  • Journal of the American Chemical Society, Vol. 137, Issue 23
  • DOI: 10.1021/jacs.5b03836

The impact of the resolution of the identity approximate integral method on modern ab initio algorithm development
journal, October 1997

  • Kendall, Rick A.; Früchtl, Herbert A.
  • Theoretical Chemistry Accounts: Theory, Computation, and Modeling (Theoretica Chimica Acta), Vol. 97, Issue 1-4
  • DOI: 10.1007/s002140050249

Structural Defects in Graphene
journal, November 2010

  • Banhart, Florian; Kotakoski, Jani; Krasheninnikov, Arkady V.
  • ACS Nano, Vol. 5, Issue 1
  • DOI: 10.1021/nn102598m

New Relativistic ANO Basis Sets for Transition Metal Atoms
journal, July 2005

  • Roos, Björn O.; Lindh, Roland; Malmqvist, Per-Åke
  • The Journal of Physical Chemistry A, Vol. 109, Issue 29
  • DOI: 10.1021/jp0581126

Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy
journal, January 2005

  • Weigend, Florian; Ahlrichs, Reinhart
  • Physical Chemistry Chemical Physics, Vol. 7, Issue 18, p. 3297-3305
  • DOI: 10.1039/b508541a

Biomass Derived N-Doped Porous Carbon Supported Single Fe Atoms as Superior Electrocatalysts for Oxygen Reduction
journal, April 2017

Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials
journal, August 2015

  • Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa
  • Nature Materials, Vol. 14, Issue 9
  • DOI: 10.1038/nmat4367

Open Babel: An open chemical toolbox
journal, October 2011

  • O'Boyle, Noel M.; Banck, Michael; James, Craig A.
  • Journal of Cheminformatics, Vol. 3, Issue 1
  • DOI: 10.1186/1758-2946-3-33

Orbital-dependent density functionals: Theory and applications
journal, January 2008

Water splitting: Taking cobalt in isolation
journal, January 2016

Structural and mechanistic basis for the high activity of Fe–N–C catalysts toward oxygen reduction
journal, January 2016

  • Li, Jingkun; Ghoshal, Shraboni; Liang, Wentao
  • Energy & Environmental Science, Vol. 9, Issue 7
  • DOI: 10.1039/C6EE01160H

Multiplet splittings and other properties from density functional theory: an assessment in iron–porphyrin systems
journal, January 2005

What zeroth-order Hamiltonian for CASPT2 adiabatic energetics of Fe(II)N6 architectures?
journal, September 2009

  • Kepenekian, Mikaël; Robert, Vincent; Le Guennic, Boris
  • The Journal of Chemical Physics, Vol. 131, Issue 11
  • DOI: 10.1063/1.3211020

Strain control of magnetism in graphene decorated by transition-metal atoms
journal, August 2011

Toward reliable density functional methods without adjustable parameters: The PBE0 model
journal, April 1999

  • Adamo, Carlo; Barone, Vincenzo
  • The Journal of Chemical Physics, Vol. 110, Issue 13
  • DOI: 10.1063/1.478522

Delocalization Error and “Functional Tuning” in Kohn–Sham Calculations of Molecular Properties
journal, June 2014

  • Autschbach, Jochen; Srebro, Monika
  • Accounts of Chemical Research, Vol. 47, Issue 8
  • DOI: 10.1021/ar500171t

Singlet versus Triplet Reactivity in an Mn(V)–Oxo Species: Testing Theoretical Predictions Against Experimental Evidence
journal, September 2016

  • Yang, Tzuhsiung; Quesne, Matthew G.; Neu, Heather M.
  • Journal of the American Chemical Society, Vol. 138, Issue 38
  • DOI: 10.1021/jacs.6b05027

Hydrogen-Bonding Interactions Trigger a Spin-Flip in Iron(III) Porphyrin Complexes
journal, February 2015

  • Sahoo, Dipankar; Quesne, Matthew G.; de Visser, Sam P.
  • Angewandte Chemie International Edition, Vol. 54, Issue 16
  • DOI: 10.1002/anie.201411399

Density functional theory for modelling large molecular adsorbate–surface interactions: a mini-review and worked example
journal, November 2016

Theoretical investigation on reaction pathways for ethylene epoxidation on Ti-decorated graphene
journal, August 2017

Two-State Reactivity Mechanism of Benzene C–C Activation by Trinuclear Titanium Hydride
journal, August 2016

  • Zhu, Bo; Guan, Wei; Yan, Li-Kai
  • Journal of the American Chemical Society, Vol. 138, Issue 35
  • DOI: 10.1021/jacs.6b02433

Electronic structure and reactivity of high-valent oxo iron porphyrins
journal, March 2002

A DFT Study of Nucleobase Dealkylation by the DNA Repair Enzyme AlkB
journal, April 2009

  • Liu, Haining; Llano, Jorge; Gauld, James W.
  • The Journal of Physical Chemistry B, Vol. 113, Issue 14
  • DOI: 10.1021/jp810715t

Two-State Reactivity in Organometallic Gas-Phase Ion Chemistry
journal, September 1995

  • Shaik, Sason; Danovich, David; Fiedler, Andreas
  • Helvetica Chimica Acta, Vol. 78, Issue 6
  • DOI: 10.1002/hlca.19950780602

Single Cobalt Atom and N Codoped Carbon Nanofibers as Highly Durable Electrocatalyst for Oxygen Reduction Reaction
journal, September 2017

Spin State Energetics in First-Row Transition Metal Complexes: Contribution of (3s3p) Correlation and Its Description by Second-Order Perturbation Theory
journal, January 2017

  • Pierloot, Kristine; Phung, Quan Manh; Domingo, Alex
  • Journal of Chemical Theory and Computation, Vol. 13, Issue 2
  • DOI: 10.1021/acs.jctc.6b01005

Nanoporous Graphene with Single-Atom Nickel Dopants: An Efficient and Stable Catalyst for Electrochemical Hydrogen Production
journal, October 2015

  • Qiu, H. -J.; Ito, Yoshikazu; Cong, Weitao
  • Angewandte Chemie International Edition, Vol. 54, Issue 47
  • DOI: 10.1002/anie.201507381

Discriminating Catalytically Active FeN x Species of Atomically Dispersed Fe–N–C Catalyst for Selective Oxidation of the C–H Bond
journal, July 2017

  • Liu, Wengang; Zhang, Leilei; Liu, Xin
  • Journal of the American Chemical Society, Vol. 139, Issue 31
  • DOI: 10.1021/jacs.7b05130

Accurate Spin-State Energetics of Transition Metal Complexes. 1. CCSD(T), CASPT2, and DFT Study of [M(NCH) 6 ] 2+ (M = Fe, Co)
journal, October 2012

  • Lawson Daku, Latévi Max; Aquilante, Francesco; Robinson, Timothy W.
  • Journal of Chemical Theory and Computation, Vol. 8, Issue 11
  • DOI: 10.1021/ct300592w

Isolated Ni single atoms in graphene nanosheets for high-performance CO 2 reduction
journal, January 2018

  • Jiang, Kun; Siahrostami, Samira; Zheng, Tingting
  • Energy & Environmental Science, Vol. 11, Issue 4
  • DOI: 10.1039/C7EE03245E
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