Pore size effects on high-efficiency proton conduction in three stable 3D Al-based MOFs modified with imidazole

Zhang, Lu; Ma, Xiaoxue; Li, Xin; Liu, Ronghua; Zhao, Xin; Hao, Hongguo; Yan, Hui; Zhu, Hongjie; Zhou, Huawei; Zhong, Dichang

doi:10.1039/d3qi01941a

Cited by 6 publications

(2 citation statements)

References 52 publications

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“…The AC impedance of the MOFs was measured by varying the temperature from 30 to 100 °C at an AC amplitude with a frequency of 1–10 6 Hz and a voltage of 100 mV. To obtain optimal data, the disk must be equilibrated for 1 day before measurement at every RH, − where the RHs were: 68, 75, 85, 93, and 98%. These RHs are tuned by employing variably saturated salt solutions: KI (68% RH), NaCl (75% RH), KCl (85% RH), KNO 3 (93% RH), and K 2 SO 4 (98% RH).…”

Section: Methodsmentioning

confidence: 99%

Ligand-Functionalized MIL-68-type Indium(III) Metal–Organic Frameworks with Prominent Intrinsic Proton Conductivity

Song,

Sang,

et al. 2024

Inorg. Chem.

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Indium-based metal−organic frameworks (In-MOFs) have now become an attractive class of porous solids in materials science and electrochemistry due to their diverse structures and promising applications. In the field of proton conduction, to find more crystalline MOFs with splendid proton-conductive properties, herein, five three-dimensional isostructural In-MOFs, MIL-68-In or MIL-68-In-X (X = NH 2 , OH, Br, or NO 2 ) using terephthalic acid (H 2 BDC) or functionalized terephthalic acids (H 2 BDC-X) as multifunctional linkages were efficiently fabricated. First, the outstanding structural stability of the five MOFs, including thermal and water stability, was verified by thermal analysis and powder X-ray diffraction. Subsequently, the H 2 O-mediated proton conductivities (σ) were fully assessed and compared. Notably, their σ evinced a significant positive correlation between the temperature or relative humidity (RH) and varied with the functional groups on the organic ligands. Impressively, their highest σ values are up to 10 −3 −10 −4 S/cm (100 °C/98% RH) and change in this order: MIL-68-In-OH (1.72 × 10 −3 S/cm) > MIL-68-In-NH 2 (1.70 × 10 −3 S/cm) > MIL-68-In-NO 2 (4.47 × 10 −4 S/cm) > MIL-68-In-Br (4.11 × 10 −4 S/cm) > MIL-68-In (2.37 × 10 −4 S/cm). Finally, the computed activation energy values under 98 or 68% RHs are assessed, and the related proton conduction mechanisms are speculated. Moreover, after electrochemical testing, these MOFs illustrate remarkable structural rigidity, laying a meritorious material foundation for future applications.

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Section: Methodsmentioning

confidence: 99%

Ligand-Functionalized MIL-68-type Indium(III) Metal–Organic Frameworks with Prominent Intrinsic Proton Conductivity

Song,

Sang,

et al. 2024

Inorg. Chem.

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“…We have obtained some exciting findings, such as the optimal proton conductivity of up to 10 −3 S/cm [ 35 , 36 , 37 , 38 , 39 ]. At the same time, free N -heterolytic small molecules can be employed as a proton source or carrier in a MOF’s framework, resulting in high-efficiency proton transmission [ 40 , 41 , 42 , 43 ]. However, these post-modified molecules are not anchored firmly enough in the MOF framework, resulting in leakage defects during use.…”

Section: Introductionmentioning

confidence: 99%

High H2O-Assisted Proton Conduction in One Highly Stable Sr(II)-Organic Framework Constructed by Tetrazole-Based Imidazole Dicarboxylic Acid

Feng,

Li,

Xie

et al. 2024

Molecules

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Solid electrolyte materials with high structural stability and excellent proton conductivity (σ) have long been a popular and challenging research topic in the fuel cell field. This problem can be addressed because of the crystalline metal–organic frameworks’ (MOFs’) high structural stability, adjustable framework composition, and dense H-bonded networks. Herein, one highly stable Sr(II) MOF, {[Sr(H2tmidc)2(H2O)3]·4H2O}n (1) (H3tmidc = 2-(1H-tetrazolium-1-methylene)-1H-imidazole-4,5-dicarboxylic acid) was successfully fabricated, which was structurally characterized by single-crystal X-ray diffraction and electrochemically examined by the AC impedance determination. The results demonstrated that the σ of the compound manifested a positive dependence on temperature and humidity, and the optimal proton conductivity is as high as 1.22 × 10−2 S/cm under 100 °C and 98% relative humidity, which is at the forefront of reported MOFs with ultrahigh σ. The analysis of the proton conduction mechanism reveals that numerous tetrazolium groups, carboxyl groups, coordination, and crystallization water molecules in the framework are responsible for the high efficiency of proton transport. This work offers a fresh perspective on how to create novel crystalline proton conductive materials.

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Superprotonic conductivity of ketoenamine covalent-organic frameworks grafted by imidazole-based units

Zhang,

Xia,

Xie

et al. 2024

Journal of Colloid and Interface Science

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Pore size effects on high-efficiency proton conduction in three stable 3D Al-based MOFs modified with imidazole

Abstract: Three stable porous aluminum-based MOFs 1–3 with different pore sizes were selected as an imidazole (Im) supporter and three proton conductive composites Im@1–3 were prepared. Due to the pore size effect, the σ value of Im@3 can be up to 2.55 × 10−1 S cm−1 at 80 °C and 100% RH.

Cited by 6 publications

References 52 publications

Ligand-Functionalized MIL-68-type Indium(III) Metal–Organic Frameworks with Prominent Intrinsic Proton Conductivity

Ligand-Functionalized MIL-68-type Indium(III) Metal–Organic Frameworks with Prominent Intrinsic Proton Conductivity

High H2O-Assisted Proton Conduction in One Highly Stable Sr(II)-Organic Framework Constructed by Tetrazole-Based Imidazole Dicarboxylic Acid

Superprotonic conductivity of ketoenamine covalent-organic frameworks grafted by imidazole-based units

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