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Pathway selection as a tool for crystal defect engineering : a case study with a functional coordination polymer
Abrishamkar, Afshin (ETH Zurich. Institute of Chemical and Bioengineering)
Suárez García, Salvio (Institut Català de Nanociència i Nanotecnologia)
Sevim, Semih (ETH Zurich. Institute of Chemical and Bioengineering)
Sorrenti, Alessandro (ETH Zurich. Institute of Chemical and Bioengineering)
Pons, Ramon (Institut de Química Avançada de Catalunya)
Liu, Shi-Xia (Universitat Bern. Department of Chemistry and Biochemistry)
Decurtins, Silvio (Universitat Bern. Department of Chemistry and Biochemistry)
Aromi, Guillem (Universitat de Barcelona. Departament de Química Inorgànica i Orgànica)
Aguilà, David (Universitat de Barcelona. Departament de Química Inorgànica i Orgànica)
Pane, Salvador (ETH Zurich. Institute of Robotics and Intelligent Systems)
deMello, Andrew J. (ETH Zurich. Institute of Chemical and Bioengineering)
Rotaru, Aurelian (Universitatea Stefan cel Mare din Suceava. Department of Electrical Engineering and Computer Science)
Ruiz-Molina, Daniel (Institut Català de Nanociència i Nanotecnologia)
Puigmartí-Luis, Josep (ETH Zurich. Institute of Chemical and Bioengineering)

Date: 2020
Abstract: New synthetic routes capable of achieving defect engineering of functional crystals through well-controlled pathway selection will spark new breakthroughs and advances towards unprecedented and unique functional materials and devices. In nature, the interplay of chemical reactions with the diffusion of reagents in space and time is already used to favor such pathway selection and trigger the formation of materials with bespoke properties and functions, even when the material composition is preserved. Following this approach, herein we show that a controlled interplay of a coordination reaction with mass transport (i. e. the diffusion of reagents) is essential to favor the generation of charge imbalance defects (i. e. protonation defects) in a final crystal structure (thermodynamic product). We show that this synthetic pathway is achieved with the isolation of a kinetic product (i. e. a metastable state), which can be only accomplished when a controlled interplay of the reaction with mass transport is satisfied. Accounting for the relevance of controlling, tuning and understanding structure-properties correlations, we have studied the spin transition evolution of a well-defined spin-crossover complex as a model system.
Note: Altres ajuts: J.P.L. and S.P. acknowledge networking support by the COST Action CM1407 "e-minds". The ICN2 is funded by the CERCA programme / Generalitat de Catalunya. G.A. thanks support by the Generalitat de Catalunya through the ICREA Academia Prize 2018
Note: Número d'acord de subvenció EC/H2020/734322
Note: Número d'acord de subvenció EC/H2020/677020
Note: Número d'acord de subvenció MINECO/RTI2018-098027-B-C21
Note: Número d'acord de subvenció MINECO/CTQ2017-88948-P
Note: Número d'acord de subvenció MINECO/SEV-2017-0706
Note: Número d'acord de subvenció MINECO/MAT 2015-70615-R
Note: Número d'acord de subvenció MINECO/BES-2015-071492
Rights: Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial i la comunicació pública de l'obra, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original. No es permet la creació d'obres derivades. Creative Commons
Language: Anglès
Document: article ; recerca ; acceptedVersion
Subject: Defect crystal engineering ; Pathway selection ; Out-of-equilibrium crystal state ; Non-covalent synthesis ; Reaction-diffusion condition
Published in: Applied materials today, Vol. 20 (Sep. 2020) , art. 100632, ISSN 2352-9407

DOI: 10.1016/j.apmt.2020.100632


Available from: 2022-09-30
Postprint

The record appears in these collections:
Research literature > UAB research groups literature > Research Centres and Groups (scientific output) > Experimental sciences > Catalan Institute of Nanoscience and Nanotechnology (ICN2)
Articles > Research articles
Articles > Published articles

 Record created 2020-09-14, last modified 2021-01-12



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