Gas Adsorption Snapshots in Metal–Organic Frameworks Unveil the Impact of Pore Geometry on Hydrogen Storage

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-08-06 DOI:10.1021/acsmaterialslett.4c0124610.1021/acsmaterialslett.4c01246

Nan Chieh Chiu, Andrzej Gładysiak, Ankit K. Yadav, Coset Abreu-Jaureguí, Alicia Manjón-Sanz, Cheng Li, Hongliang Huang, Joaquin Silvestre-Albero and Kyriakos C. Stylianou*,

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Abstract

Metal–organic frameworks (MOFs) are promising candidates for hydrogen (H₂) storage. However, effective H₂ storage in MOFs is challenging, because of weak adsorbent–adsorbate interactions. Optimizing the pore volume, size, and functionality in porous MOFs is crucial, but it is still unclear how to maximize H₂ storage capacity while minimizing loading pressure. Herein, we investigate Al-TBAPy (H₄TBAPy: 1,3,6,8-tetrakis(p-benzoic acid)pyrene), a low-density MOF, for H₂ storage. Al-TBAPy features three interconnected pores (A–C), possesses a pore volume of 0.51 cm³/g, and demonstrates a H₂ uptake of 22.5 mmol/g at 77 K and 100 bar. In situ deuterium (D₂) gas loading neutron diffraction experiments reveal molecular-level insights into pore filling. Pores B and C exhibit high H₂ affinity, while pore A, with a larger volume, takes up more H₂ molecules. The collective properties of all pores and their interconnection result in a high deliverable gravimetric H₂ capacity of 4.3 wt % under combined temperature and pressure swing conditions.

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金属有机框架中的气体吸附快照揭示了孔隙几何形状对储氢的影响

金属有机框架（MOFs）是氢气（H2）存储的理想候选材料。然而，由于吸附剂与吸附剂之间的相互作用较弱，在 MOFs 中有效储存氢气具有挑战性。优化多孔 MOF 的孔隙体积、大小和功能性至关重要，但如何在最大限度地提高 H2 储存能力的同时最小化负载压力仍不清楚。在此，我们研究了 Al-TBAPy（H4TBAPy：1,3,6,8-四（对苯甲酸）芘）这种低密度 MOF 的 H2 储存。Al-TBAPy 具有三个相互连接的孔隙（A-C），孔隙体积为 0.51 cm3/g，在 77 K 和 100 bar 条件下的 H2 吸收率为 22.5 mmol/g。原位氘（D2）气体装载中子衍射实验揭示了孔隙填充的分子水平。孔隙 B 和 C 表现出较高的 H2 亲和性，而孔隙 A 的体积较大，吸收的 H2 分子较多。所有孔隙的共同特性及其相互连接使其在组合温度和压力摆动条件下的可输送重量计量 H2 容量高达 4.3 wt %。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.