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A ReaxFF investigation of hydride formation in palladium nanoclusters (ACS author proof PDF)

Evidence and attribution

Authority of statements

Prose sections below (Summary, Methods, Findings, etc.) are curated summaries of the publication identified by doi, title, and pdf_path in the front matter above. They are not new primary claims by this wiki.

For definitive numerical values, reaction schemes, and interpretations, use the peer-reviewed article (and optional records under normalized/papers/ when present)—not this page alone.

Summary

This manifest row registers an ACS author-proof PDF variant of Senftle, Janik & van Duin, J. Phys. Chem. C, on Pd/H ReaxFF modeling (DOI 10.1021/jp411015a; canonical narrative: paper:2014senftle-venue-jp411015a). Palladium dissociates and absorbs hydrogen, motivating membranes, storage, and catalyst designs. The abstract describes deriving a ReaxFF Pd/H potential from extensive quantum data for bulk and surface properties, then applying a hybrid grand-canonical Monte Carlo / molecular dynamics (GC-MC/MD) method to compute hydrogen absorption isotherms for Pd bulk and nanoclusters over H₂ pressures ~10⁻¹–10⁻¹⁴ atm and temperatures 300–500 K. Equilibrated cluster structures illustrate roles of surface, subsurface, and bulk regions in size-dependent transitions between low-H solid-solution (α-like) and high-H hydride (β-like) regimes and miscibility-gap behavior. Additional MD studies address dissociative adsorption kinetics and extract H diffusion coefficients, barriers, and pre-exponential factors from bulk Pd trajectories. The abstract states thermodynamic (GC-MC/MD) and kinetic (MD) results agree with experimental literature, validating the Pd/H parameterization.

Methods

This slug’s ACS author-proof PDF is the same article as [[2014senftle-venue-jp411015a]] (DOI 10.1021/jp411015a). Methods mirror that page; only PDF provenance differs.

ReaxFF training / sampling (see VOR page for authoritative pagination)

  • Pd/H ReaxFF derived from extensive QM data for bulk and surface properties (abstract).
  • GC-MC/MD hydrogen absorption isotherms for Pd bulk and ~1.0–2.0 nm clusters over p(H₂) = 10⁻¹–10⁻¹⁴ atm and T = 300–500 K (abstract).
  • MD for dissociative adsorption kinetics in clusters and H diffusion in bulk Pd (coefficients, barriers, pre-exponentials reported in the article).
  • Timestep / thermostat / cutoffs: use the version-of-record Methods/SI—not inferred here.

Grand-canonical / MD protocol: identical to [[2014senftle-venue-jp411015a]]: molecular dynamics segments support GC-MC/MD hydrogen absorption isotherms for Pd bulk and nanoclusters with H\(_2\) pressures spanning \(10^{-1}\)–\(10^{-14}\) atm and temperatures 300–500 K (abstract). Ensemble: NVT molecular dynamics is used for the relaxation/kinetics portions as described in the JPCC article (see version-of-record [[2014senftle-venue-jp411015a]]). Engine, timestep (fs), thermostat, PBC, barostat, and full ps/ns tables: N/A — not retyped on this proof wiki page—use papers/Senftle_PdH_JPCCproof_2014.pdf or the typeset sibling PDF.

Findings

  • Proof extract aligns with the published narrative summarized on [[2014senftle-venue-jp411015a]]: thermodynamic GC-MC/MD results and kinetic MD observables reported as consistent with experiment; miscibility-gap / α–β framing for clusters with surface/subsurface/bulk decomposition of H content.
  • Pd/H parameters are described as transferable with prior Pd/O work for future Pd/O/H catalysis extensions (abstract).
  • Use [[2014senftle-venue-jp411015a]] for figure/table citations; this proof slug exists for byte-accurate manifest hashing of the alternate PDF.

Limitations

Proof PDFs may show placeholder metadata or typography drift—cite paper:2014senftle-venue-jp411015a for pagination. Maintain separate manifest rows for hash provenance only. GC-MC/MD sampling details (chemical potential grids, cluster sizes, equilibration lengths) materially affect isotherm shapes—reuse numerical plateau positions only after confirming the Methods section in the version-of-record article.

Relevance to group

Duplicate PDF lineage for the same scientific artifact; useful when only the proof bytes are archived locally. The Pd/H GC-MC/MD workflow is a canonical example of open ensemble ReaxFF practice in the van Duin corpus and pairs with hydrogen-storage and catalysis notes on Pd surfaces.

Citations and evidence anchors

  • DOI: https://doi.org/10.1021/jp411015a — papers/Senftle_PdH_JPCCproof_2014.pdf; extract normalized/extracts/2014senftle-venue-research_p1-2.txt; canonical article page: paper:2014senftle-venue-jp411015a.