| 1. |
- Chen, Tianyang, et al.
(författare)
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Dimensionality Modulates Electrical Conductivity in Compositionally Constant One-, Two-, and Three-Dimensional Frameworks
- 2022
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 144:12, s. 5583-5593
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Tidskriftsartikel (refereegranskat)abstract
- We reveal here the construction of Ni-based metal-organic frameworks (MOFs) and conjugated coordination polymers (CCPs) with different structural dimensionalities, including closely pi-stacked 1D chains (Ni-1D), aggregated 2D layers (Ni-2D), and a 3D framework (Ni-3D), based on 2,3,5,6-tetraamino-1,4-hydroquinone (TAHQ) and its various oxidized forms. These materials have the same metal-ligand composition but exhibit distinct electronic properties caused by different dimensionalities and supramolecular interactions between SBUs, ligands, and structural motifs. The electrical conductivity of these materials spans nearly 8 orders of magnitude, approaching 0.3 S/cm.
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| 2. |
- Chen, Tianyang, et al.
(författare)
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High-rate, high-capacity electrochemical energy storage in hydrogen-bonded fused aromatics
- 2023
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Ingår i: Joule. - : Elsevier BV. - 2542-4351. ; 7:5, s. 986-1002
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Tidskriftsartikel (refereegranskat)abstract
- Designing materials for electrochemical energy storage with short charging times and high charge capacities is a longstanding challenge. The fundamental difficulty lies in incorporating a high density of redox couples into a stable material that can efficiently conduct both ions and electrons. We report all-organic, fused aromatic materials that store up to 310 mAh g−1 and charge in as little as 33 s. This performance stems from abundant quinone/imine functionalities that decorate an extended aromatic backbone, act as redox-active sites, engage in hydrogen bonding, and enable a delocalized high-rate energy storage with stability upon cycling. The extended conjugation and hydrogen-bonding-assisted bulk charge storage contrast with the surface-confined or hydration-dependent behavior of traditional inorganic electrodes.
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| 3. |
- Dou, Jin-Hu, et al.
(författare)
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Atomically precise single-crystal structures of electrically conducting 2D metal-organic frameworks
- 2021
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Ingår i: Nature Materials. - : Springer Science and Business Media LLC. - 1476-1122 .- 1476-4660. ; 20, s. 222-228
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Tidskriftsartikel (refereegranskat)abstract
- Electrically conducting 2D metal-organic frameworks (MOFs) have attracted considerable interest, as their hexagonal 2D lattices mimic graphite and other 2D van der Waals stacked materials. However, understanding their intrinsic properties remains a challenge because their crystals are too small or of too poor quality for crystal structure determination. Here, we report atomically precise structures of a family of 2D pi-conjugated MOFs derived from large single crystals of sizes up to 200 mu m, allowing atomic-resolution analysis by a battery of high-resolution diffraction techniques. A designed ligand core rebalances the in-plane and out-of-plane interactions that define anisotropic crystal growth. We report two crystal structure types exhibiting analogous 2D honeycomb-like sheets but distinct packing modes and pore contents. Single-crystal electrical transport measurements distinctively demonstrate anisotropic transport normal and parallel to the pi-conjugated sheets, revealing a clear correlation between absolute conductivity and the nature of the metal cation and 2D sheet packing motif. Two-dimensional MOFs can possess porosity and electrical conductivity but are difficult to grow as single crystals. Here, by balancing in-plane and out-of-plane interactions, single crystals of sizes up to 200 mu m are grown, allowing in-plane transport measurements and atomic-resolution analysis.
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| 4. |
- Wan, Ruomeng, et al.
(författare)
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Dipole-mediated exciton management strategy enabled by reticular chemistry
- 2022
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Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 13:36, s. 10792-10797
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Tidskriftsartikel (refereegranskat)abstract
- Selectively blocking undesirable exciton transfer pathways is crucial for utilizing exciton conversion processes that involve participation of multiple chromophores. This is particularly challenging for solid-state systems, where the chromophores are fixed in close proximity. For instance, the low efficiency of solid-state triplet–triplet upconversion calls for inhibiting the parasitic singlet back-transfer without blocking the flow of triplet excitons. Here, we present a reticular chemistry strategy that inhibits the resonance energy transfer of singlet excitons. Within a pillared layer metal–organic framework (MOF), pyrene-based singlet donors are situated perpendicular to porphyrin-based acceptors. High resolution transmission electron microscopy and electron diffraction enable direct visualization of the structural relationship between donor and acceptor (D–A) chromophores within the MOF. Time-resolved photoluminescence measurements reveal that the structural and symmetry features of the MOF reduce the donor-to-acceptor singlet transfer efficiency to less than 36% compared to around 96% in the control sample, where the relative orientation of the donor and acceptor chromophores cannot be controlled.
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