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Record W2008401399 · doi:10.1016/j.crci.2012.04.010

New structures of hydronium cation clusters

2012· article· en· W2008401399 on OpenAlex
Sonjae Wallace, Lulu Huang, Chérif F. Matta, Lou Massa, Ivan Bernal

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueComptes Rendus Chimie · 2012
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsMount Saint Vincent UniversityDalhousie University
FundersNational Institute of General Medical Sciences
KeywordsHydroniumChemistryIonCrystallographyDensity functional theoryComputational chemistryInorganic chemistryPhysical chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Four new hydronium ion structures are investigated by means of quantum mechanical calculations at the DFT/B3LYP6-311+G(2d,2p) level of theory. There exist experimental crystallographic hydronium cations (H 11 O 5 + ) of two different geometrical structures, one BEXFEQ (acyclic) and one IYEPEH (cyclic). Molecular calculations reveal their relative stability. Another hydronium cation NEBDII (H 15 O 7 + ) when optimized reveals a totally new and unexpected structure. All three optimized structures are shown to be quite stable as judged by their binding energies, and therefore may possibly be found in solution. A main result of this article is the discovery of three new optimized structures of hydronium ions, all of which are preferentially ring structures. The optimized structure of H 15 O 7 + is a cube lacking a vertex. Putting a water molecule at the “empty” vertex leads by energy optimization to a structure of H 17 O 8 + which has the approximate symmetry of a cube. This cubic structure, as judged by its fragments, is one of the most interesting of the hydronium ions studied in this paper. The addition of H 3 O + to a group of seven neutral molecules in the hypothetical reaction H 3 O + + 7 H 2 O → H 17 O 8 + induces two water molecules to each capture a proton at the expense of two other water molecules (converting them into hydroxyl anions) leading to a cluster with the formula <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" overflow="scroll"> <mml:mrow> <mml:msub> <mml:mrow> <mml:mo stretchy="false">[</mml:mo> <mml:msub> <mml:mtext>H</mml:mtext> <mml:mn>3</mml:mn> </mml:msub> <mml:msup> <mml:mtext>O</mml:mtext> <mml:mrow> <mml:mo>+</mml:mo> <mml:mn>0.7</mml:mn> </mml:mrow> </mml:msup> <mml:mo stretchy="false">]</mml:mo> </mml:mrow> <mml:mn>3</mml:mn> </mml:msub> <mml:msubsup> <mml:mrow> <mml:mo stretchy="false">[</mml:mo> <mml:msub> <mml:mtext>H</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> <mml:mtext>O</mml:mtext> <mml:mo stretchy="false">]</mml:mo> </mml:mrow> <mml:mn>3</mml:mn> <mml:mrow> <mml:mo>+</mml:mo> <mml:mn>0.1</mml:mn> </mml:mrow> </mml:msubsup> <mml:msub> <mml:mrow> <mml:mo stretchy="false">[</mml:mo> <mml:msup> <mml:mtext>OH</mml:mtext> <mml:mrow> <mml:mo>−</mml:mo> <mml:mn>0.6</mml:mn> </mml:mrow> </mml:msup> <mml:mo stretchy="false">]</mml:mo> </mml:mrow> <mml:mn>2</mml:mn> </mml:msub> </mml:mrow> </mml:math> , where the superscripts are the integrated QTAIM atomic charges (in atomic units) on the respective species (inside the bracket) or on groups of a given species (outside the bracket). The cubic arrangement of 3H 3 O + .3H 2 O.2OH − is accompanied with a significant redistribution of charge: Each hydronium cation carries ca. +0.7 au, the hydroxyl anions only around –0.6 au each, while the water molecules remain quasi-neutral with a slight positive charge.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.484
Threshold uncertainty score0.443

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.014
GPT teacher head0.258
Teacher spread0.244 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it