Lanthanide-based F-MOFs: Structure, hydrolytic stability, spectral and magnetic properties DOI Creative Commons

D. Princík,

Vladimı́r Zeleňák, Róbert Gyepes

и другие.

Journal of Solid State Chemistry, Год журнала: 2024, Номер 339, С. 124949 - 124949

Опубликована: Авг. 8, 2024

A series of five novel lanthanide-based fluorinated metal-organic frameworks (Ln-F-MOFs) have been synthesized under solvothermal conditions by the reaction 3,3′-bis(trifluoromethyl)-[1,1′-biphenyl]-4,4′-dicarboxylic acid (H2L) and lanthanide Ln(III) ions (Ln(III)La, Ce, Pr, Nd Eu). Powder X-ray diffraction (PXRD) analysis revealed that all prepared complexes are isostructural. single-crystal crystallographic study one representative isostructural group, namely {[La2(L)3(DMF)2(H2O)2]}n showed, compound crystallizes in a triclinic system with space group P-1. The lattice parameter values = 8.563(2) Å, b 13.199(3) c 16.008(4) α 104.588(7) °, β 92.904(7) ° γ 92.717(7) two formula units unit cell. overall structure is formed 2D polymeric layers, which arranged into semi-3D supramolecular through hydrogen bonds other intramolecular interactions. hydrophobic properties showed exhibit surface hydrophobicity "rose petal effect" contact angle approximately 107°. However, structures not hydrolytically stable long term starts to delaminate after days water. This manifestation fact do form 3D polymer network, it made up layers connected only weak non-bonding photoluminescence determined characteristic 5d-4f or 4f-4f electron transitions for individual ions. magnetic Nd(III), Pr(III) Eu(III) variants were studied. {[Pr2(L)3(DMF)2(H2O)2]}n characterized presence low-lying quasi-doublet 15.6 cm−1 energy splitting, whereas variant nonmagnetic at low temperatures, but 7F1 state accessible thermal excitation. For Nd(III) complex, X-band EPR measurements performed. Since 1D channels dimensions 4.90 × 7.23 Å2 present within structure, adsorption N2, CO2 H2 gases was also

Язык: Английский

“Bubble‐Diode” Breathable Electrodes for Fast Gas Transport DOI
Yi He, Peng Tan

Chemistry - A European Journal, Год журнала: 2023, Номер 30(11)

Опубликована: Дек. 13, 2023

Bubbles arising from wild gas evolution commonly exist in electrochemical systems, particularly water electrolysis and rechargeable aqueous batteries (e. g., Zn-air batteries). Substantial energy dissipation occurs due to the obstruction of active sites ion-conducting pathways by evolving bubbles. Efforts are made elucidate effective strategies for fast transport, most which focus on minimizing bubble size facilitating their timely detachment through complex techniques such as constructing super-hydrophilic nano-structure electrodes, flowing electrolytes, ultrasonic oscillation. Recently, an innovative, facile, highly efficient method utilizing a breathable electrode design promote gaseous molecules external environment emerges promising approach since it avoids remarkable accumulation while remaining free additional accessories. This paper highlights origin this design. Starting with introducing basic concept traditional electrodes based hydrophobic polymer networks discussing current progress underlying mechanisms, detailed description advanced inspired "bubble-diode" superior breathability follows. Concept aims contribute deep understanding technology paves way further advancements renewable era.

Язык: Английский

Процитировано

4

Membrane‐Free Water Electrolysis for Hydrogen Generation with Low Cost DOI Open Access

Xintong Gao,

Pengtang Wang, Xiaojie Sun

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Окт. 31, 2024

Abstract Conventional water electrolysis relies on expensive membrane‐electrode assemblies and sluggish oxygen evolution reaction (OER) at the anode, which makes cost of green hydrogen (H 2 ) generation much higher than that grey H . Here, we develop an innovative efficient membrane‐free system to overcome these two obstacles simultaneously. This utilizes thermodynamically more favorable urea oxidation (UOR) generate clean N over a new class Cu‐based catalyst (Cu X O) for replacing OER, fundamentally eliminating explosion risk O mixing while removing need membranes. Notably, this exhibits highest Faradaic efficiency among reported work. In situ spectroscopic studies reveal y intermediate‐mediated UOR mechanism Cu ensures its unique selectivity OER inertness. More importantly, industrial‐type electrolyser (MFE) based successfully reduces electricity consumption only 3.78 kWh Nm −3 , significantly lower 5.17 commercial alkaline electrolyzers (AWE). Comprehensive techno‐economic analysis (TEA) suggests design reduced input MFE plants reduce production US$1.81 kg −1 is those meeting technical target (US$2.00–2.50 set by European Commission United States Department Energy.

Язык: Английский

Процитировано

1

Advancements in membrane-less electrolysis configurations: Innovations and Challenges DOI

Krishna Kumar,

Sara Mateo, A. Osa

и другие.

Current Opinion in Electrochemistry, Год журнала: 2024, Номер 49, С. 101602 - 101602

Опубликована: Ноя. 6, 2024

Язык: Английский

Процитировано

1

Distinct CO2-run-out regime from steric effect of electric double layer in electrochemical CO2 reduction DOI
Longfei Chen, Hao Feng, Ying Zhang

и другие.

Applied Physics Reviews, Год журнала: 2024, Номер 11(3)

Опубликована: Июль 15, 2024

The field of electrochemical CO2 reduction reaction (eCO2RR) is pursuing high operating current densities, eventually controlled by transport. Here, we develop a new multiscale modeling approach that able to more generally describe the effects electric double layer (EDL) on transport over wide potential window extending utmost potentials. By leveraging it, identify distinct CO2-run-out regime where supply runs out due EDL steric effect from dense solvated cations with maximum thickness equal cation size. Consequently, CO2RR density drops at relatively negative transition generating bell-shaped polarization curve, which in contrast CO2-transport-limited reaches plateau. Furthermore, graphical method, verified experimental data, predict regime. This work sheds light for catalyst design and electrolyzer engineering.

Язык: Английский

Процитировано

0

Lanthanide-based F-MOFs: Structure, hydrolytic stability, spectral and magnetic properties DOI Creative Commons

D. Princík,

Vladimı́r Zeleňák, Róbert Gyepes

и другие.

Journal of Solid State Chemistry, Год журнала: 2024, Номер 339, С. 124949 - 124949

Опубликована: Авг. 8, 2024

A series of five novel lanthanide-based fluorinated metal-organic frameworks (Ln-F-MOFs) have been synthesized under solvothermal conditions by the reaction 3,3′-bis(trifluoromethyl)-[1,1′-biphenyl]-4,4′-dicarboxylic acid (H2L) and lanthanide Ln(III) ions (Ln(III)La, Ce, Pr, Nd Eu). Powder X-ray diffraction (PXRD) analysis revealed that all prepared complexes are isostructural. single-crystal crystallographic study one representative isostructural group, namely {[La2(L)3(DMF)2(H2O)2]}n showed, compound crystallizes in a triclinic system with space group P-1. The lattice parameter values = 8.563(2) Å, b 13.199(3) c 16.008(4) α 104.588(7) °, β 92.904(7) ° γ 92.717(7) two formula units unit cell. overall structure is formed 2D polymeric layers, which arranged into semi-3D supramolecular through hydrogen bonds other intramolecular interactions. hydrophobic properties showed exhibit surface hydrophobicity "rose petal effect" contact angle approximately 107°. However, structures not hydrolytically stable long term starts to delaminate after days water. This manifestation fact do form 3D polymer network, it made up layers connected only weak non-bonding photoluminescence determined characteristic 5d-4f or 4f-4f electron transitions for individual ions. magnetic Nd(III), Pr(III) Eu(III) variants were studied. {[Pr2(L)3(DMF)2(H2O)2]}n characterized presence low-lying quasi-doublet 15.6 cm−1 energy splitting, whereas variant nonmagnetic at low temperatures, but 7F1 state accessible thermal excitation. For Nd(III) complex, X-band EPR measurements performed. Since 1D channels dimensions 4.90 × 7.23 Å2 present within structure, adsorption N2, CO2 H2 gases was also

Язык: Английский

Процитировано

0