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Popping and Locking: Balanced Rigidity and Porosity of Zeolitic Imidazolate Frameworks for High-Productivity Methane Purification. | LitMetric

Popping and Locking: Balanced Rigidity and Porosity of Zeolitic Imidazolate Frameworks for High-Productivity Methane Purification.

J Am Chem Soc

School of Physical Science and Technology, Shanghai Key Laboratory of High-Resolution Electron Microscopy, State Key Laboratory of Advanced Medical Materials and Devices, ShanghaiTech University, Shanghai 201210, China.

Published: April 2024

AI Article Synopsis

Article Abstract

Zeolitic imidazolate frameworks (ZIFs) hold great promise in carbon capture, owing to their structural designability and functional porosity. However, intrinsic linker dynamics limit their pressure-swing adsorption application to biogas upgrading and methane purification. Recently, a functionality-locking strategy has shown feasibility in suppressing such dynamics. Still, a trade-off between structural rigidity and uptake capacity remains a key challenge for optimizing their high-pressure CO/CH separation performance. Here, we report a sequential structural locking (SSL) strategy for enhancing the CO capture capacity and CH purification productivity in dynamic ZIFs (dynaZIFs). Specifically, we isolated multiple functionality-locked phases, ZIF-78-lt, -ht1, and -ht2, by activation at 50, 160, and 210 °C, respectively. We observed multiple-level locking through gas adsorption and powder X-ray diffraction. We uncovered an SSL mechanism dominated by linker-linker π-π interactions that transit to C-H···O hydrogen bonds with binding energies increasing from -0.64 to -2.77 and -5.72 kcal mol, respectively, as evidenced by single-crystal X-ray diffraction and density functional theory calculations. Among them, ZIF-78-ht1 exhibits the highest CO capture capacity (up to 18.6 mmol g) and CH purification productivity (up to 7.6 mmol g) at 298 K and 30 bar. These findings provide molecular and energetic insights into leveraging framework flexibility through the SSL mechanism to optimize porous materials' separation performance.

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Source
http://dx.doi.org/10.1021/jacs.4c00045DOI Listing

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