ALDRIDGE GROUP

FRUSTRATED LEWIS PAIRS IN CATALYSIS AND SENSING

Nitrous oxide detection (MK)

Reversible H2/N2O uptake (ZM)

FLP-catalysed dehydrogenation (ZM)

(Recent work from Mike Kelly and Zhenbo Mo)

Although introduced as a concept as long ago as 1942 by Nobel laureate HC Brown, the exploitation of frustrated Lewis pairs (FLPs) as a new paradigm for small molecule capture and activation stems largely from a landmark report from Stephan in 2006. Such systems typically comprise strong Lewis acid and Lewis base components, that are too sterically bulky to form a conventional donor/acceptor bond. This unquenched reactivity allows for the activation of strong non-polar bonds (e.g. H2) and the capture of otherwise relatively inert molecules such as CO2 and N2O.

Our interests in this area are in the design of FLPs tailored for specific target applications which require the reversible uptake of small molecules. These include (i) the sensing of small oxygen containing analytes of environmental relevance (N2O, CO, CO2 etc) and (ii) catalytic applications of FLPs, particularly in dehydrogenation chemistry. With these goals in mind, a series of single component FLPs has been investigated which show significant promise, for example by (i) heterolytically cleaving dihydrogen to give an equilibrium mixture of FLP and H2 activation product in solution at room temperature, and (ii) reversibly capturing N2O (uptake at room temperature, 1 atm; release at 323 K).

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Copyright S Aldridge

2016

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