Hierarchy of Hydrogen Bonding versus Anion Binding in Self-Assembled Network Structures of Silver(I)
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Bibliographic record
Abstract
Reaction of the ligands 1,2-C 6 H 4 {NHC( O)-4-C 5 H 4 N} 2 ( 1 ) and 1,2-C 6 H 4 {NHC( O)-3-C 5 H 4 N} 2 ( 2 ) with silver(I) salts AgX, X = CF 3 CO 2, NO 3, CF 3 SO 3, and PF 6, gave the corresponding complexes [(AgX)(μ-LL)] n, 3a − 4d ( 3a − 3d: LL = 1; 4a − 4d: LL = 2; a, X = CF 3 CO 2; b, X = NO 3; c, X = CF 3 SO 3; d, X = PF 6 ). The complexes probably exist in solution primarily as the disilver(I) macrocyclic complexes [{AgX(μ-LL)} 2 ] or [Ag 2 (μ-LL) 2 ]X 2, but in the solid state they may exist as either macrocycles or polymers [{AgX(μ-LL)} n ] or [Ag n (μ-LL) n ]X n . The silver(I) centers have distorted tetrahedral stereochemistry when X = CF 3 CO 2 or NO 3 but roughly linear stereochemistry when X = CF 3 SO 3 or PF 6, and it is argued that the hierarchy of control in the self-assembly process is by the bonds Ag−N > Ag−O > NH···O C when X = CF 3 CO 2 or NO 3, but Ag−N > NH···O C > Ag···O or Ag···F when X = CF 3 SO 3 or PF 6 . In complexes 3a and 3b, macrocyclic complexes are connected to form polymers or sheets, respectively, through bridging anions, whereas polymers of 4a are connected through bridging anions to form a double-stranded polymer. In all these cases, network structures are formed through formation of intermolecular hydrogen bonds NH···O C, and these porous networks contain large solvent-filled channels. In the molecular materials assembled using the more weakly bonding anions (X = CF 3 SO 3 or PF 6 ), the network structures are more compact, and they do not contain solvent molecules. Complexes 3c and 4d exist as polymers, whereas 4c exists as a macrocycle. These complexes are further connected through hydrogen bonding and through weak Ag···O or Ag···F interactions to form network structures. Complexes 3a − 3c and 4a adopt the polar anti conformation of the two amidopyridyl units of the bidentate ligands, and 4d adopts a similar conformation with an intramolecular NH···O C bond, but complex 4c adopts the nonpolar syn conformation. Complex 4d is unusual because it undergoes spontaneous resolution to give crystals in which chiral polymers are self-assembled to give a chiral network.
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Full frame distilled prediction
Teacher imitationNot 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.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.001 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it