AI Article Synopsis

  • Metallo-supramolecular self-assembly offers a promising method for creating economically valuable materials but faces challenges in characterizing complex mixtures efficiently.
  • A large library of transition metals and ligands was robotically prepared and analyzed using advanced techniques, bypassing the need for individual structural assignments.
  • This automated approach simplifies the assessment of self-assembly activities, enabling quicker and more efficient screening of supramolecular processes.

Article Abstract

Embracing complexity in design, metallo-supramolecular self-assembly presents an opportunity for fabricating materials of economic significance. The array of accessible supramolecules is alluring, along with favourable energy requirements. Implementation is hampered by an inability to efficiently characterise complex mixtures. The stoichiometry, size, shape, guest binding properties and reactivity of individual components and combinations thereof are inherently challenging to resolve. A large combinatorial library of four transition metals (Fe, Cu, Ni and Zn), and six β-diketonate ligands at different molar ratios and pH was robotically prepared and directly analysed over multiple timepoints with electrospray ionisation travelling wave ion mobility-mass spectrometry. The dataset was parsed for self-assembling activity without first attempting to structurally assign individual species. Self-assembling systems were readily categorised without manual data-handling, allowing efficient screening of self-assembly activity. This workflow clarifies solution phase supramolecular assembly processes without manual, bottom-up processing. The complex behaviour of the self-assembling systems was reduced to simpler qualities, which could be automatically processed.

Download full-text PDF

Source
http://dx.doi.org/10.1002/anie.202313892DOI Listing

Publication Analysis

Top Keywords

ion mobility-mass
8
mobility-mass spectrometry
8
self-assembling systems
8
automated structural
4
structural activity
4
activity screening
4
screening β-diketonate
4
β-diketonate assemblies
4
assemblies high-throughput
4
high-throughput ion
4

Similar Publications

We report the first implementation of ion mobility mass spectrometry combined with an ultra-high throughput sample introduction technology for high throughput screening (HTS). The system integrates differential ion mobility (DMS) with acoustic ejection mass spectrometry (AEMS), termed DAEMS, enabling the simultaneous quantitation of structural isomers that are the sub-strates and products of isomerase mediated reactions in intermediary metabolism. We demonstrate this potential by comparing DAEMS to a luminescence assay for the isoform of phosphoglycerate mutase (iPGM) distinctively present in pathogens offering an opportunity as a drug target for a variety of microbial and parasite borne diseases.

View Article and Find Full Text PDF

"Liquid gold" has been traditionally used for over a century to decorate ceramicware, but its chemical composition has not been thoroughly investigated. One of the keys to successfully characterizing liquid gold, which is a complex mixture, is to distinguish Au-containing products from other chemicals. In this paper, we propose a separation based on the difference in collision cross section, of which chemicals with heavy atoms are relatively smaller than those without in ion mobility-mass spectrometry (IM-MS).

View Article and Find Full Text PDF

Most conventional methods used to measure protein melting temperatures reflect changes in structure between different conformational states and are typically fit to a two-state model. Population abundances of distinct conformations were measured using variable-temperature electrospray ionization ion mobility mass spectrometry to investigate the thermally induced unfolding of the model protein cytochrome . Nineteen conformers formed at high temperature have elongated structures, consistent with unfolded forms of this protein.

View Article and Find Full Text PDF

Targeted metabolomics and lipidomics are increasingly utilized in clinical research, providing quantitative and comprehensive assessments of metabolic profiles that underlie physiological and pathological mechanisms. These approaches enable the identification of critical metabolites and metabolic alterations essential for accurate diagnosis and precision treatment. Mass spectrometry, in combination with various separation techniques, offers a highly sensitive and specific platform for implementing targeted metabolomics and lipidomics in clinical settings.

View Article and Find Full Text PDF

Selective Reduction of Esters to Access Aldehydes Using Fiddler Crab-Type Boranes.

J Am Chem Soc

January 2025

Organocatalysis Research Group, Institute of Organic Chemistry, HUN-REN Research Centre for Natural Sciences, Magyar tudósok körútja 2, Budapest H-1117, Hungary.

The partial reduction of esters to aldehydes is a fundamentally important transformation for the synthesis of numerous fine chemicals and consumer goods. However, despite the many efforts, limitations have persisted, such as competing overreduction, low reproducibility, use of exigent reaction conditions and hazardous chemicals. Here, we report a novel catalyst family with a unique steric design which promotes the catalytic partial reduction of esters with unprecedented, near-perfect selectivity and efficiency.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!