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Organic synthesis

Squaramide macrocycles that prefer sulfate in water

Qin L, Hartley A, Turner P, et al. · Chemical science · 2016

Open access · cc by · source: Europe PMC

Meta-linked squaramide macrocycles bind SO42− so tightly in wet DMSO that NMR cannot measure Ka, and they still select sulfate in 50% water.

Study at a glance

Design
Other — Synthesis and aqueous NMR titration of squaramide macrocycles for sulfate recognition
N
Anion-receptor binding study — no sample N
Population
Macrocyclic squaramide receptors in water/DMSO mixtures
Outcome
Sulfate binding affinity and selectivity versus competing anions

Structured fields used in claim comparison tables when every cited study has a complete layer.

Key findings

Meta receptors 1, 2, 5, and 6 are potent, selective sulfate ligands even in 50% water. 1 and 2 have Ka(SO42−) > 10^4 M−1; 2 is more sulfate-selective versus phosphate and acetate. The crystal shows a bowl/cone geometry with four NH···O hydrogen bonds. Receptor 6 discriminates sulfate from chromate better than the sulfate-binding protein.

Methodology

Authors synthesized [2]- and [3]-squaramide macrocycles, titrated anions by 1H NMR in 0.5–50% water/DMSO, crystallized a 1:1 sulfate complex, and compared selectivity with chromate and with the sulfate-binding protein benchmark.

Limitations

Process-scale nuclear-waste extraction and clinical plasma sulfate assays are suggested applications, not demonstrated; some isomers are too insoluble for full Ka tables.

How this study connects

Role on claims

Each row is a claim on a concept or method page where this paper supports, challenges, or qualifies the statement. Roles are hand-checked — not a model guess.

  • SupportsOrganic synthesisconcept

    This library holds 7 empirical chemistry papers on organic synthesis with isolated findings, rates or spectra rather than reviews.

    Evidence for the claim as stated.

  • SupportsOrganic synthesisconcept

    Meta-linked squaramide macrocycles bind SO42− so tightly in wet DMSO that NMR cannot measure Ka, and they still select sulfate in 50% water.

    Evidence for the claim as stated.

  • SupportsOrganic synthesisconcept

    A high yield on one substrate is not a general method, and many 'new reactions' are still one-pot screens rather than mechanism-complete syntheses.

    Evidence for the claim as stated.

  • SupportsNMR Spectroscopymethod

    Titration NMR can rank anion affinities in wet DMSO and still not be a waste-treatment plant. Meta-linked squaramide macrocycles were potent sulfate ligands even in 50% water, with Ka(SO4²⁻) > 10⁴ M⁻¹ for receptors 1 and 2; a crystal showed a bowl/cone with four NH···O hydrogen bonds. Process-scale extraction and plasma assays are suggested, not demonstrated, and some isomers were too insoluble for full Ka tables.

    Evidence for the claim as stated.

  • SupportsNMR Spectroscopymethod

    Solution NMR, in-cell NMR and solid-state/identity NMR are not the same experiment. Titration Kas in wet DMSO, oocyte SOFAST-HMQC of a labelled oligonucleotide, and ³¹P shifts of a diphosphene answer different questions. A student who says 'we ran NMR' without saying which nuclei and which medium cannot compare those papers.

    Evidence for the claim as stated.

Open questions

Tensions this paper is part of

From concept pages' “where studies disagree.” Disagreement means the same question; scope means different assays, populations, or outcomes.

  • Scope difference — different assays, populations, or outcomes

    A high yield on one substrate is not a general method, and many 'new reactions' are still one-pot screens rather than mechanism-complete syntheses.

    Also on this tension

  • Scope difference — different assays, populations, or outcomes

    Solution NMR, in-cell NMR and solid-state/identity NMR are not the same experiment. Titration Kas in wet DMSO, oocyte SOFAST-HMQC of a labelled oligonucleotide, and ³¹P shifts of a diphosphene answer different questions. A student who says 'we ran NMR' without saying which nuclei and which medium cannot compare those papers.

Related papers in this topic

Same topic cluster — not a recommendation engine.