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Electrochemistry

Frustrated Lewis pairs oxidize H2 without metals

Lawrence EJ, Clark ER, Curless LD, et al. · Chemical science · 2016

Open access · cc by · source: Europe PMC

A carbon Lewis acid, BArF18, and lutidine cleave H2 and oxidize it at carbon electrodes about 1 V milder, without CO poisoning.

Key findings

Pre-formed 1-H lowers the H2 oxidation potential by ~1 V (~197 kJ mol−1) and another 110 mV versus prior FLP electrochemistry. After 25 min at 20 °C, 30% of 1+ is hydrided; conversion is quantitative in 17 h. The system tolerates CO and avoids H2-evolution side reactions.

Methodology

Authors combined a carbon-based Lewis acid (1+), a boron hydride-shuttle (BArF18), and 2,6-lutidine, tracked H2 activation by NMR and CV, and cycled bulk electrolysis at carbon paper.

Limitations

An operating H2/O2 fuel cell and a fully air-stable boron FLP are future goals; a fourth H2 charge failed until more lutidine was added.

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