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Pt TPE cages harvest light for cyclization

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Self-assembled platinum–tetraphenylethene cages transfer energy to rhodamine B (up to 77% ΦET) and photocatalyze maleimide–aniline cyclization in water-rich solvent.

Source

Self-assembled metallasupramolecular cages towards light harvesting systems for oxidative cyclization

Kumar A, Saha R, Mukherjee PS · Chemical science · 2021

doi.org/10.1039/d1sc00097gRead the full paper ↗50 citationscc by

Study at a glance

Design
Other — Pt–TPE metallacages as AIE donors for FRET to RhB and photo-oxidative cyclization
N
Supramolecular photocatalysis — no sample N
Population
Pt4L2/Pt8L2 TPE cages with rhodamine B acceptors
Outcome
Energy-transfer efficiency and visible-light oxidative cyclization yields

Structured fields used in claim comparison tables when every cited study has a complete layer.

What they did

They made tetraimidazole TPE donor L (67%) and assembled it with 180°/120° trans-Pt acceptors into Pt4L2 and Pt8L2 cages, exchanged to PF6 salts, and studied AIE in 90% water/MeCN. Cages 2b/3b donated FRET to RhB; the pair catalyzed visible-light oxidative cyclization of N,N-dimethylaniline with maleimides.

What they found

AIE: 5-, 25-, and 16-fold emission boosts for 1b–3b; aggregate ΦF up to 25.67% (2b). ΦET is 77% (2b+RhB) and 58% (3b+RhB) at 5:1 donor/acceptor; antenna effects 21 and 16. Photocatalysis: 97% of 6a with 2a+RhB (12 h), 92% with 3b+RhB, 74% even with bulky N-pyrenemaleimide. TPE–TPE separations 9.1, 20.4, and 17.8 Å.

The limits

What it doesn't show

Energy-transfer efficiencies are for one solvent ratio and one dye. Cage 1b is a weaker AIE/FRET platform. Yields are for a specific cyclization, not a general photoredox scope. DFT geometries are gas-phase models, not crystal structures of the assemblies.

Key terms

AIE
Aggregation-induced emission: TPE fluoresces when propeller rotation is blocked in aggregates.
FRET
Through-space dipole energy transfer from cage emission to RhB absorption.
Metallacage
3D coordination assembly; here Pt4L2 or Pt8L2 prisms from a tetratopic donor.
Antenna effect
How much acceptor emission is amplified by the donor relative to direct acceptor excitation.
TPE
Tetraphenylethene, the AIE-active core of ligand L.

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Maximum FRET efficiency (2b + RhB, 5:1) is about

Common questions

Why 90% water/MeCN?

Maximum AIE, stable nano-aggregates, and no self-quenching precipitation on the FRET timescale.

Who is the FRET acceptor?

Rhodamine B, whose absorption overlaps cage emission.

Does the harvested energy do chemistry?

Yes—photo-oxidative cyclization of dimethylaniline with maleimides in up to 97% yield.

Cage 2 vs 3?

2b has higher ΦET (77% vs 58%) and antenna effect (21 vs 16).

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