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Guest-Induced Helical Superstructure from a Gold Nanocluster-Based Supramolecular Organic Framework Enables Efficient
Qiang Li1, Wenxing Gao1, Zijian Wang1
1State Key Laboratory of Solidification Processing, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an 710072, P. R. China.
ACS Nano
|August 7, 2024
Summary
Researchers created novel gold nanocluster frameworks (MSOF-4 and MSOF-5) that selectively capture bromopropane isomers. One framework transforms into a helical structure, enhancing catalytic activity for electron transfer reactions.
Area of Science:
- Supramolecular Chemistry
- Nanomaterials Science
- Catalysis
Background:
- Mimicking natural hierarchical assembly for artificial systems is a significant challenge.
- Atomically precise gold nanoclusters offer potential for complex structures and functions.
- Controlling host-guest interactions in supramolecular frameworks is crucial for functional applications.
Purpose of the Study:
- To design and synthesize novel supramolecular organic frameworks (MSOFs) using custom gold nanoclusters.
- To investigate the host-guest adaptation behaviors of these MSOFs towards 1-bromopropane (1-BPR) and 2-bromopropane (2-BPR) isomers.
- To explore the functional implications of guest adsorption, including structural changes and catalytic activity.
Main Methods:
- Synthesis of atomically precise gold nanoclusters: Au11(4-Mpy)3(PPh3)7.
- Construction of single-crystal supramolecular organic frameworks (MSOF-4 and MSOF-5).
- Single-crystal X-ray diffraction to determine structures and guest-induced transformations.
- Gas adsorption studies to evaluate selective adsorption of BPR isomers.
- Spectroscopic analysis (fluorescence) to monitor structural changes.
- Catalytic activity measurements for electron transfer reactions.
Main Results:
- MSOF-4, with sev topology, selectively adsorbs 1-BPR, leading to a structural transformation of the gold nanocluster to Au11Br3(PPh3)7 and formation of MSOF-6.
- MSOF-6 exhibits a rare helical assembly structure, significantly enhancing electron transfer (ET) catalytic rates (nearly 6-fold increase compared to MSOF-4).
- MSOF-5, with chb topology, shows selective physical adsorption of 1-BPR but no fluorescence change upon guest adsorption.
- Distinct host-guest adaptation behaviors and functional outcomes were observed for MSOF-4 and MSOF-5.
Conclusions:
- Demonstrated a strategy for creating advanced assemblies with high-order complexity using atomically precise gold nanoclusters.
- Engineered the functions of supramolecular frameworks through guest-induced structural transformations and ligand exchange.
- Highlighted the potential of tailored nanocluster-based frameworks for selective guest binding and catalysis.
