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Eu(II) cryptate photocatalyzes bibenzyl coupling

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A visible-absorbing Eu(II) azacryptate, assembled in situ from EuCl3, ligand and Zn0, reductively couples benzyl chloride to 1,2-diphenylethane with an excited-state potential near −3 V.

Source

First use of a divalent lanthanide for visible-light-promoted photoredox catalysis

Jenks TC, Bailey MD, Hovey JL, et al. · Chemical science · 2018

doi.org/10.1039/c7sc02479gRead the full paper ↗52 citationscc by

What they did

Authors encapsulated Eu(II) in octaazacryptand 1, measured absorption/emission, lifetime, quantum yield and electrochemistry, then ran blue-light couplings of benzyl chloride with sacrificial Zn0, including wet EuCl3·6H2O conditions.

What they found

Stoichiometric irradiation gave 85±2% bibenzyl in 30 min. Catalytic loadings of 5/1/0.5 mol% gave 71/70/60% bibenzyl (~14–120 turnovers). Excited-state E* ≈ −3.0 V vs Ag/AgCl; τ = 0.98 μs; Φ = 37% in MeOH. The system tolerates some water.

The limits

What it doesn't show

Scope on unactivated aryl bromides is proposed, not demonstrated; E1/2 was measured in DMF not methanol.

Key terms

Eu(II) photoredox
Visible 5d–4f excitation of divalent europium used to transfer electrons.
Azacryptand 1
Octaazacryptand that shifts Eu(II) absorption into the visible.
Sacrificial Zn0
Reductant that returns Eu(III) to Eu(II) for catalysis.
Excited-state potential
Estimated −3.0 V vs Ag/AgCl from E1/2 and emission energy.
Bibenzyl
1,2-Diphenylethane, the C–C coupled product from PhCH2Cl.

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The C–C product from PhCH2Cl is:

Common questions

What C–C product is formed?

1,2-Diphenylethane from benzyl chloride.

What regenerates Eu(II)?

Zn0.

Approximate E*?

−3.0 V vs Ag/AgCl.

Can it start from Eu(III)?

Yes—in situ from EuCl3, 1 and Zn0.

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