Structural Landscape and Proton Conduction of Lanthanide 5-(Dihydroxyphosphoryl)isophthalates Article Swipe

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Inés R. Salcedo , Montse Bazaga-García , Rosario M. P. Colodrero , Álvaro Vílchez-Cózar , Fernando Cañamero-Cebrián , Pascual Olivera‐Pastor , Jan K. Zaręba , Aurelio Cabeza ·

YOU? · · 2024 · Open Access · · DOI: https://doi.org/10.1021/acs.cgd.4c00786

Metal phosphonate-carboxylate compounds represent a promising class of materials for proton conduction applications. This study investigates the structural, thermal, and proton conduction properties of three groups of lanthanide-based compounds derived from 5-(dihydroxyphosphoryl)isophthalic acid (PiPhtA). The crystal structures, solved ab initio from X-ray powder diffraction data, reveal that groups Ln-I, Ln[O₃P-C₆H₃(COO)(COOH)(H₂O)₂] (Ln = La, Pr), and Ln-II, Ln₂{[O₃P-C₆H₃(COO)(COOH)]₂(H₂O)₄}·2H₂O (Ln = La, Pr, Eu), exhibit three-dimensional frameworks, while group Ln-III, Ln[O₃P-C₆H₃(COO)(COOH)(H₂O)] (Ln = Yb), adopts a layered structure with unbonded carboxylic groups oriented toward the interlayer region. All compounds feature carboxylic groups and coordinating water molecules. Impedance measurements demonstrate that these materials exhibit water-mediated proton conductivity, initially following a vehicle-type proton-transfer mechanism. Upon exposure to ammonia vapors from a 14 or 28% aqueous solution, compounds from groups II and III adsorb ammonia and water, leading to an enhancement in proton conductivity consistent with a Grotthuss-type proton-transfer mechanism. Notably, group II of the studied compounds undergoes the formation of a new expanded phase through the internal reaction of carboxylic groups with ammonia, coexisting with the as-synthesized phase. This postsynthetic modification results in a significant increase in proton conductivity, from approximately ∼5 × 10^-6 to ∼10^-4 S·cm^-1 at 80 °C and 95% relative humidity (RH), attributed to a mixed intrinsic/extrinsic contribution. Remarkably, the NH₃(28%)-exposed Yb-III compound achieves an enhancement in proton conductivity, reaching ∼ 5 × 10^-3 S·cm^-1 at 80 °C and 95% RH, primarily through an extrinsic contribution.

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Lanthanide Proton Thermal conduction Chemistry Crystallography Materials science Physics Nuclear physics Organic chemistry Ion Composite material

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Type: article
Language: en
Landing Page: https://doi.org/10.1021/acs.cgd.4c00786
OA Status: hybrid
Cited By: 2
References: 54
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OpenAlex ID: https://openalex.org/W4402477791

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DOI: https://doi.org/10.1021/acs.cgd.4c00786

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Title: Structural Landscape and Proton Conduction of Lanthanide 5-(Dihydroxyphosphoryl)isophthalates

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Language: en

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Publication year: 2024

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Publication date: 2024-09-12

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Authors: Inés R. Salcedo, Montse Bazaga-García, Rosario M. P. Colodrero, Álvaro Vílchez-Cózar, Fernando Cañamero-Cebrián, Pascual Olivera‐Pastor, Jan K. Zaręba, Aurelio Cabeza

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Landing page: https://doi.org/10.1021/acs.cgd.4c00786

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Concepts: Lanthanide, Proton, Thermal conduction, Chemistry, Crystallography, Materials science, Physics, Nuclear physics, Organic chemistry, Ion, Composite material

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Cited by: 2

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