Issue 38, 2024

CO2-actuated spin transition tuning in an interdigitated Hofmann-type coordination polymer

Abstract

The increased anthropogenic emission level of CO2 urges the development of CO2-responsive materials, but is it possible to regulate the inherent electronic properties through weak physisorption of a ubiquitous gas such as CO2? Herein, we intended to answer this imperative question by the first case of CO2-actuated variable spin-state stabilisation in an interdigitated Hofmann-type coordination polymer [FeIIPd(CN)4L2] (1, L = methyl isonicotinate), showing a wide shift in transition temperature (Teq) from 178 K at PCO2 = 0 kPa to 229 K at PCO2 = 100 kPa. Interestingly, the emergence of a stepped behaviour in the heating process below PCO2 = 10 kPa and overlapping magnetic susceptibility values above PCO2 = 10 kPa elucidate the selective LS state stabilisation solely correlated with the extent of CO2 accommodation. Based on the magnetic response and phase transition diagrams obtained under respective PCO2, a plausible scenario of the spin-state switching can be interpreted as (1ls + Image ID:d4sc04266b-t1.gif) → (1hs + Image ID:d4sc04266b-t2.gif) → 1hs at PCO2 ≤ 10 kPa, Image ID:d4sc04266b-t3.gif1hs at 100 kPa < PCO2 ≥ 32 kPa and Image ID:d4sc04266b-t4.gifImage ID:d4sc04266b-t5.gif1hs at 100 kPa, where 1 and 1′ represent CO2-free and CO2-encapsulated states, respectively. The cooperative CO2 sorption with SCO based on the varied CO2 pressure corroborates a novel case for developing CO2-responsive magnetic materials henceforth.

Graphical abstract: CO2-actuated spin transition tuning in an interdigitated Hofmann-type coordination polymer

Supplementary files

Article information

Article type
Edge Article
Submitted
28 Jun 2024
Accepted
28 Aug 2024
First published
30 Aug 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 15610-15616

CO2-actuated spin transition tuning in an interdigitated Hofmann-type coordination polymer

A. Paul, W. Kosaka, B. Kumar, D. J. Mondal, H. Miyasaka and S. Konar, Chem. Sci., 2024, 15, 15610 DOI: 10.1039/D4SC04266B

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