ALDRIDGE GROUP

MAIN GROUP MEDIATED BOND ACTIVATION AND CATALYSIS

Silylene H2 cleavage (AP)

Reversible M-C scission (AP)

Catalytic CO2 reduction (JA)

(recent work from Andrey Protchenko and Joe Abdalla)

Oxidative addition and reductive elimination represent fundamental chemical steps which are key to numerous societally important catalytic processes. The associated n+/(n-2)+ redox shuttle, while facile for noble metals, is not well established for Main Group systems. This reflects the fact that although oxidative bond activation by sub-valent Main Group systems is precedented, subsequent regeneration of the reduced state via reductive elimination is typically not thermodynamically viable. We are currently looking at two approaches to circumvent this problem.

Group 14 metal systems incorporating strongly sigma donating ancillary substituents, particularly germanium and tin systems. The use of boryl or silyl ancillary ligands not only allows for unprecedented oxidative addition chemistry at M(II) centres, but also brings about favourable reaction kinetics. Recently we have exploited these and related Group 13 systems to achieve reversible redox-based bond modification at Main Group element centres.

Cooperative bond activation. In very recent work we have synthesized Main Group metal systems featuring non-innocent ancillary ligands which can be exploited in the activation of a range of protic and hydridic E-H bonds, and even in the catalytic reduction of carbon dioxide.

Projects looking at FLP approaches to bond activation/catalysis are also under investigation

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Copyright S Aldridge

2016

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