Water network-mediated, electron-induced proton transfer in [C5H5N • (H2O)n]– clusters

DeBlase, Andrew F.; Wolke, Conrad T.; Weddle, Gary H.; Archer, Kaye A.; Jordan, Kenneth D.; Kelly, John T.; Tschumper, Gregory S.; Hammer, Nathan I.; Johnson, Mark A.

doi:10.1063/1.4931928

Title: Water network-mediated, electron-induced proton transfer in [C₅H₅N • (H₂O)n]^– clusters

Abstract

The role of proton-assisted charge accommodation in electron capture by a heterocyclic electron scavenger is investigated through theoretical analysis of the vibrational spectra of cold, gas phase [Py·(H₂O)_n=3–5]– clusters. These radical anions are formed when an excess electron is attached to water clusters containing a single pyridine (Py) molecule in a supersonic jet ion source. Under these conditions, the cluster ion distribution starts promptly at n = 3, and the photoelectron spectra, combined with vibrational predissociation spectra of the Ar-tagged anions, establish that for n > 3, these species are best described as hydrated hydroxide ions with the neutral pyridinium radical, PyH⁽⁰⁾, occupying one of the primary solvation sites of the OH^–. The n = 3 cluster appears to be a special case where charge localization on Py and hydroxide is nearly isoenergetic, and the nature of this species is explored with ab initio molecular dynamics calculations of the trajectories that start from metastable arrangements of the anion based on a diffuse, essentially dipole-bound electron. These calculations indicate that the reaction proceeds via a relatively slow rearrangement of the water network to create a favorable hydration configuration around the water molecule that eventually donates a proton to the Py nitrogenmore »« less

Authors:

DeBlase, Andrew F. ^[1]; Wolke, Conrad T. ^[1]; Weddle, Gary H. ^[2]; Archer, Kaye A. ^[3];

^[3];

^[4];

^[4]; Hammer, Nathan I. ^[4];

^[1]

Yale Univ., New Haven, CT (United States)
Yale Univ., New Haven, CT (United States); Fairfield Univ., Fairfield, CT (United States)
Univ. of Pittsburgh, Pittsburgh, PA (United States)
Univ. of Mississippi, University, MS (United States)

Publication Date:: Fri Oct 09 00:00:00 EDT 2015

Research Org.:: Yale Univ., New Haven, CT (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1469362

Alternate Identifier(s):: OSTI ID: 1223330

Grant/Contract Number:: FG02-06ER15800; FG02-00ER15066

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 143; Journal Issue: 14; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    DeBlase, Andrew F., Wolke, Conrad T., Weddle, Gary H., Archer, Kaye A., Jordan, Kenneth D., Kelly, John T., Tschumper, Gregory S., Hammer, Nathan I., and Johnson, Mark A. Water network-mediated, electron-induced proton transfer in [C5H5N • (H2O)n]– clusters.  United States: N. p., 2015. 
Web.  doi:10.1063/1.4931928.

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                    DeBlase, Andrew F., Wolke, Conrad T., Weddle, Gary H., Archer, Kaye A., Jordan, Kenneth D., Kelly, John T., Tschumper, Gregory S., Hammer, Nathan I., & Johnson, Mark A. Water network-mediated, electron-induced proton transfer in [C5H5N • (H2O)n]– clusters.  United States.  https://doi.org/10.1063/1.4931928

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                    DeBlase, Andrew F., Wolke, Conrad T., Weddle, Gary H., Archer, Kaye A., Jordan, Kenneth D., Kelly, John T., Tschumper, Gregory S., Hammer, Nathan I., and Johnson, Mark A. Fri .  
"Water network-mediated, electron-induced proton transfer in [C5H5N • (H2O)n]– clusters".  United States.  https://doi.org/10.1063/1.4931928.  https://www.osti.gov/servlets/purl/1469362.

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@article{osti_1469362,

  title        = {Water network-mediated, electron-induced proton transfer in [C5H5N • (H2O)n]– clusters},

  author       = {DeBlase, Andrew F. and Wolke, Conrad T. and Weddle, Gary H. and Archer, Kaye A. and Jordan, Kenneth D. and Kelly, John T. and Tschumper, Gregory S. and Hammer, Nathan I. and Johnson, Mark A.},

  abstractNote = {The role of proton-assisted charge accommodation in electron capture by a heterocyclic electron scavenger is investigated through theoretical analysis of the vibrational spectra of cold, gas phase [Py·(H2O)n=3–5]– clusters. These radical anions are formed when an excess electron is attached to water clusters containing a single pyridine (Py) molecule in a supersonic jet ion source. Under these conditions, the cluster ion distribution starts promptly at n = 3, and the photoelectron spectra, combined with vibrational predissociation spectra of the Ar-tagged anions, establish that for n > 3, these species are best described as hydrated hydroxide ions with the neutral pyridinium radical, PyH(0), occupying one of the primary solvation sites of the OH–. The n = 3 cluster appears to be a special case where charge localization on Py and hydroxide is nearly isoenergetic, and the nature of this species is explored with ab initio molecular dynamics calculations of the trajectories that start from metastable arrangements of the anion based on a diffuse, essentially dipole-bound electron. These calculations indicate that the reaction proceeds via a relatively slow rearrangement of the water network to create a favorable hydration configuration around the water molecule that eventually donates a proton to the Py nitrogen atom to yield the product hydroxide ion. In conclusion, the correlation between the degree of excess charge localization and the evolving shape of the water network revealed by this approach thus provides a microscopic picture of the “solvent coordinate” at the heart of a prototypical proton-coupled electron transfer reaction},

  doi          = {10.1063/1.4931928},

  journal      = {Journal of Chemical Physics},

  number       = 14,

  volume       = 143,

  place        = {United States},

  year         = {Fri Oct 09 00:00:00 EDT 2015},

  month        = {Fri Oct 09 00:00:00 EDT 2015}

}

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We report the water-mediated charge separation of nitric acid upon incorporation into size-selected Cs⁺∙(HNO₃)(H₂O)_n=0-11 clusters at 20 K. Dramatic spectral changes are observed in the range n=7-9 that are traced to the formation of many isomeric structures associated with intermediate transfer of the acidic proton to the water network. This transfer is complete by n=10, which exhibits much simpler vibrational band patterns consistent with those expected for a tri-coordinated hydronium ion (the Eigen motif) along with the NO stretching bands predicted for a hydrated NO₃^– anion that is directly complexed to the Cs⁺ cation. Theoretical analysis of the n=10 spectrummore »« less
https://doi.org/10.1021/acs.jpclett.1c00235

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Probing the Structural Evolution of the Hydrated Electron in Water Cluster Anions (H ₂ O) _n ^–, n ≤ 200, by Electronic Absorption Spectroscopy

Journal Article Herburger, Andreas ; Barwa, Erik ; Ončák, Milan ; ... - Journal of the American Chemical Society

Electronic absorption spectra of water cluster anions (H₂O)_n^-, n ≤ 200, at T = 80 K are obtained by photodissociation spectroscopy and compared with simulations from literature and experimental data for bulk hydrated electrons. Two almost isoenergetic electron binding motifs are seen for cluster sizes 20 ≤ n ≤ 40, which are assigned to surface and partially embedded isomers. With increasing cluster size, the surface isomer becomes less populated, and for n ≥ 50, the partially embedded isomer prevails. The absorption shifts to the blue, reaching a plateau at n ≈ 100. In this size range, the absorption spectrum ismore »« less
Cited by 11
https://doi.org/10.1021/jacs.9b10347

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Water Network Shape-Dependence of Local Interactions with the Microhydrated –NO₂^– and –CO₂^– Anionic Head Groups by Cold Ion Vibrational Spectroscopy

Journal Article Mitra, Sayoni ; Denton, Joanna K. ; Kelleher, Patrick J. ; ... - Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

We report the structural evolutions of water networks and solvatochromic response of the CH₃NO₂^– radical anion in the OH and CH stretching regions by analysis of the vibrational spectra displayed by cryogenically cooled CH₃NO₂^–·(H₂O)_n=1–6 clusters. The OH stretching bands evolve with a surprisingly large discontinuity at n = 6, which features the emergence of an intense, strongly red-shifted band along with a weaker feature that appears in the region assigned to a free OH fundamental. Very similar behavior is displayed by the perdeuterated carboxylate clusters, RCO₂^–·(H₂O)_n=5–7 (R = CD₃CD₂), indicating that this behavior is a general feature in the microhydrationmore »« less
https://doi.org/10.1021/acs.jpca.2c00721

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Title: Water network-mediated, electron-induced proton transfer in [C5H5N • (H2O)n]– clusters

Abstract

Citation Formats

Infrared Characterization of the Icosahedral Shell Closing in Cl - ·H 2 O·Ar n (1 ≤ n ≤ 13) Clusters journal, May 2002

Prying Apart a Water Molecule with Anionic H-Bonding: A Comparative Spectroscopic Study of the X - ·H 2 O (X = OH, O, F, Cl, and Br) Binary Complexes in the 600−3800 cm -1 Region journal, April 2006

Photoelectron spectroscopy of pyridine cluster anions, (Py)n−(n=4–13) journal, September 1999

Correction to “Vibrational Autodetachment–Intramolecular Vibrational Relaxation Translated Into Electronic Motion” journal, August 2011

Photoelectron spectroscopy of hydrated electron cluster anions, (H 2 O) − n =2–69 journal, March 1990

Angular Distribution of Photoelectrons journal, January 1968

Density-functional exchange-energy approximation with correct asymptotic behavior journal, September 1988

How the Shape of an H-Bonded Network Controls Proton-Coupled Water Activation in HONO Formation journal, January 2010

Observation of Large Water-Cluster Anions with Surface-Bound Excess Electrons journal, January 2005

Electron Attachment Energies of the DNA Bases journal, July 1998

Dissociative electron attachment in chloroalkanes and the correlation with vertical attachment energies journal, January 1998

The angular distribution of photoelectrons ejected from the hydrated electron cluster (H 2 O) − 18 journal, March 1990

Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal, January 1989

Reconstruction of Abel-transformable images: The Gaussian basis-set expansion Abel transform method journal, July 2002

Photochemistry of hydrated electron clusters (H 2 O) − n (15≤ n ≤40) at 1064 nm: Size dependent competition between photofragmentation and photodetachment journal, October 1988

Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions journal, May 1992

Spectroscopic Determination of the OH- Solvation Shell in the OH-middle dot(H2O)n Clusters journal, January 2003

Negative ion formation, vibrational excitation, and transmission spectroscopy in hydrogen halides journal, September 1975

The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals journal, July 2007

Electronic Relaxation Dynamics of Water Cluster Anions journal, November 2005

Model Potential Approaches for Describing the Interaction of Excess Electrons with Water Clusters: Incorporation of Long-Range Correlation Effects † journal, November 2008

A reciprocal space based method for treating long range interactions in ab initio and force-field-based calculations in clusters journal, February 1999

Survey of Ar-Tagged Predissociation and Vibrationally Mediated Photodetachment Spectroscopies of the Vinylidene Anion, C 2 H 2 − † journal, January 2010

Microhydration of Contact Ion Pairs in M 2+ OH – (H 2 O) n =1–5 (M = Mg, Ca) Clusters: Spectral Manifestations of a Mobile Proton Defect in the First Hydration Shell journal, June 2014

Spectroscopic Study of the Ion−Radical H-Bond in H 4 O 2 + † journal, April 2009

Photoelectron imaging of negative ions journal, January 2008

Photoelectron spectra of hydrated electron clusters: Fitting line shapes and grouping isomers journal, July 2006

Electron Binding Motifs of (H 2 O) n - Clusters journal, May 2006

Photoelectron imaging study of vibrationally mediated electron autodetachment in the type I isomer of the water hexamer anion journal, December 2008

Cluster size effects upon anion solvation of N-heterocyclic molecules and nucleic acid bases journal, February 2000

The influence of polarization functions on molecular orbital hydrogenation energies journal, January 1973

Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density journal, January 1988

Theoretical Study on the Excess Electron Binding Mechanism in the [CH 3 NO 2 ·(H 2 O) n ] − ( n = 1−6) Anion Clusters journal, September 2010

Temporary anion states of phosphabenzene, arsabenzene, and stibabenzene. Trends in the .pi. and .pi.* orbital energies journal, January 1982

The onset of electron-induced proton-transfer in hydrated azabenzene cluster anions journal, January 2016

MP2 energy evaluation by direct methods journal, December 1988

Infrared Spectra of the 1-Pyridinium (C 5 H 5 NH + ) Cation and Pyridinyl (C 5 H 5 NH and 4-C 5 H 6 N) Radicals Isolated in Solid para- Hydrogen journal, October 2013

Photoelectron spectroscopy of the `missing' hydrated electron clusters (H2O)−n, n=3, 5, 8 and 9: Isomers and continuity with the dominant clusters n=6, 7 and ⩾11 journal, November 1998

Relativistic separable dual-space Gaussian pseudopotentials from H to Rn journal, August 1998

Separable dual-space Gaussian pseudopotentials journal, July 1996

Size-dependent collisional incorporation of D2O into (H2O)−n around n = 15: implications on the origin of magic numbers in the hydrated electron cluster distribution journal, June 1991

Why does the IR spectrum of hydroxide stretching vibration weaken with increase in hydration? journal, January 2014

Mechanism of Homogeneous Reduction of CO 2 by Pyridine: Proton Relay in Aqueous Solvent and Aromatic Stabilization journal, December 2012

Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal, September 1997

Semiempirical GGA-type density functional constructed with a long-range dispersion correction journal, January 2006

How Do Small Water Clusters Bind an Excess Electron? journal, October 2004

Temporary negative-ion states in pyridine and diazine molecules journal, September 1976

Formation and photodestruction of dual dipole-bound anion (H2O)6{e−}CH3NO2 journal, June 2009

Electrocatalytic Carbon Dioxide Activation: The Rate-Determining Step of Pyridinium-Catalyzed CO2 Reduction journal, February 2011

Photoelectron spectroscopy of 1-nitropropane and 1-nitrobutane anions journal, February 2012

Vibrational predissociation spectroscopy of the (H2O)6−⋅Arn, n⩾6, clusters journal, January 1998

Note on an Approximation Treatment for Many-Electron Systems journal, October 1934

Ground-State Dipole-Bound Anions journal, May 1996

Efficient diffuse function-augmented basis sets for anion calculations. III. The 3-21+G basis set for first-row elements, Li-F journal, October 1983

Bottom-Up View of Water Network-Mediated CO 2 Reduction Using Cryogenic Cluster Ion Spectroscopy and Direct Dynamics Simulations journal, December 2011

The FT-IR spectra of pyridine and pyridine-d5 journal, March 1984

Temporary anion states of polyatomic hydrocarbons journal, June 1987

Infrared Spectrum and Structural Assignment of the Water Trimer Anion † journal, December 2005

Self—Consistent Molecular Orbital Methods. XII. Further Extensions of Gaussian—Type Basis Sets for Use in Molecular Orbital Studies of Organic Molecules journal, March 1972

Title: Water network-mediated, electron-induced proton transfer in [C₅H₅N • (H₂O)n]^– clusters

Infrared Characterization of the Icosahedral Shell Closing in Cl ^- ·H ₂ O·Ar _n (1 ≤ n ≤ 13) Clusters
journal, May 2002

Prying Apart a Water Molecule with Anionic H-Bonding: A Comparative Spectroscopic Study of the X ^- ·H ₂ O (X = OH, O, F, Cl, and Br) Binary Complexes in the 600−3800 cm ^-1 Region
journal, April 2006

Photoelectron spectroscopy of pyridine cluster anions, (Py)n−(n=4–13)
journal, September 1999

Correction to “Vibrational Autodetachment–Intramolecular Vibrational Relaxation Translated Into Electronic Motion”
journal, August 2011

Photoelectron spectroscopy of hydrated electron cluster anions, (H ₂ O) ⁻ _{n =2–69}
journal, March 1990

Angular Distribution of Photoelectrons
journal, January 1968

Density-functional exchange-energy approximation with correct asymptotic behavior
journal, September 1988

How the Shape of an H-Bonded Network Controls Proton-Coupled Water Activation in HONO Formation
journal, January 2010

Observation of Large Water-Cluster Anions with Surface-Bound Excess Electrons
journal, January 2005

Electron Attachment Energies of the DNA Bases
journal, July 1998

Dissociative electron attachment in chloroalkanes and the correlation with vertical attachment energies
journal, January 1998

The angular distribution of photoelectrons ejected from the hydrated electron cluster (H ₂ O) ⁻ ₁₈
journal, March 1990

Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen
journal, January 1989

Reconstruction of Abel-transformable images: The Gaussian basis-set expansion Abel transform method
journal, July 2002

Photochemistry of hydrated electron clusters (H ₂ O) ⁻ _n (15≤ n ≤40) at 1064 nm: Size dependent competition between photofragmentation and photodetachment
journal, October 1988

Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions
journal, May 1992

Spectroscopic Determination of the OH- Solvation Shell in the OH-middle dot(H2O)n Clusters
journal, January 2003

Negative ion formation, vibrational excitation, and transmission spectroscopy in hydrogen halides
journal, September 1975

The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals
journal, July 2007

Electronic Relaxation Dynamics of Water Cluster Anions
journal, November 2005

Model Potential Approaches for Describing the Interaction of Excess Electrons with Water Clusters: Incorporation of Long-Range Correlation Effects ^†
journal, November 2008

A reciprocal space based method for treating long range interactions in ab initio and force-field-based calculations in clusters
journal, February 1999

Survey of Ar-Tagged Predissociation and Vibrationally Mediated Photodetachment Spectroscopies of the Vinylidene Anion, C ₂ H ₂ ⁻ ^†
journal, January 2010

Microhydration of Contact Ion Pairs in M ²⁺ OH ^– (H ₂ O) _{n =1–5} (M = Mg, Ca) Clusters: Spectral Manifestations of a Mobile Proton Defect in the First Hydration Shell
journal, June 2014

Spectroscopic Study of the Ion−Radical H-Bond in H ₄ O ₂ ⁺ ^†
journal, April 2009

Photoelectron imaging of negative ions
journal, January 2008

Photoelectron spectra of hydrated electron clusters: Fitting line shapes and grouping isomers
journal, July 2006

Electron Binding Motifs of (H ₂ O) _n ^- Clusters
journal, May 2006

Photoelectron imaging study of vibrationally mediated electron autodetachment in the type I isomer of the water hexamer anion
journal, December 2008

Cluster size effects upon anion solvation of N-heterocyclic molecules and nucleic acid bases
journal, February 2000

The influence of polarization functions on molecular orbital hydrogenation energies
journal, January 1973

Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
journal, January 1988

Theoretical Study on the Excess Electron Binding Mechanism in the [CH ₃ NO ₂ ·(H ₂ O) _n ] ⁻ ( n = 1−6) Anion Clusters
journal, September 2010

Temporary anion states of phosphabenzene, arsabenzene, and stibabenzene. Trends in the .pi. and .pi.* orbital energies
journal, January 1982

The onset of electron-induced proton-transfer in hydrated azabenzene cluster anions
journal, January 2016

MP2 energy evaluation by direct methods
journal, December 1988

Infrared Spectra of the 1-Pyridinium (C ₅ H ₅ NH ⁺ ) Cation and Pyridinyl (C ₅ H ₅ NH and 4-C ₅ H ₆ N) Radicals Isolated in Solid para- Hydrogen
journal, October 2013

Photoelectron spectroscopy of the `missing' hydrated electron clusters (H2O)−n, n=3, 5, 8 and 9: Isomers and continuity with the dominant clusters n=6, 7 and ⩾11
journal, November 1998

Relativistic separable dual-space Gaussian pseudopotentials from H to Rn
journal, August 1998

Separable dual-space Gaussian pseudopotentials
journal, July 1996

Size-dependent collisional incorporation of D2O into (H2O)−n around n = 15: implications on the origin of magic numbers in the hydrated electron cluster distribution
journal, June 1991

Why does the IR spectrum of hydroxide stretching vibration weaken with increase in hydration?
journal, January 2014

Mechanism of Homogeneous Reduction of CO ₂ by Pyridine: Proton Relay in Aqueous Solvent and Aromatic Stabilization
journal, December 2012

Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen
journal, September 1997

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

How Do Small Water Clusters Bind an Excess Electron?
journal, October 2004

Temporary negative-ion states in pyridine and diazine molecules
journal, September 1976

Formation and photodestruction of dual dipole-bound anion (H2O)6{e−}CH3NO2
journal, June 2009

Electrocatalytic Carbon Dioxide Activation: The Rate-Determining Step of Pyridinium-Catalyzed CO₂ Reduction
journal, February 2011

Photoelectron spectroscopy of 1-nitropropane and 1-nitrobutane anions
journal, February 2012

Vibrational predissociation spectroscopy of the (H2O)6−⋅Arn, n⩾6, clusters
journal, January 1998

Note on an Approximation Treatment for Many-Electron Systems
journal, October 1934

Ground-State Dipole-Bound Anions
journal, May 1996

Efficient diffuse function-augmented basis sets for anion calculations. III. The 3-21+G basis set for first-row elements, Li-F
journal, October 1983

Bottom-Up View of Water Network-Mediated CO ₂ Reduction Using Cryogenic Cluster Ion Spectroscopy and Direct Dynamics Simulations
journal, December 2011

The FT-IR spectra of pyridine and pyridine-d5
journal, March 1984

Temporary anion states of polyatomic hydrocarbons
journal, June 1987

Infrared Spectrum and Structural Assignment of the Water Trimer Anion ^†
journal, December 2005

Self—Consistent Molecular Orbital Methods. XII. Further Extensions of Gaussian—Type Basis Sets for Use in Molecular Orbital Studies of Organic Molecules
journal, March 1972