Abstract. A novel class of readily accessible tartramide ligands has been demonstrated to promote copper-catalysed N-arylation under mild conditions. In addition, the coupling protocol employs cheap and readily available pre-catalyst, ligand, and base (NaOH), and overcomes many current limitations often associated with Ullmann coupling: it can be r...
The mechanism and dynamics of the CO2 reduction reaction (CO2RR) remain poorly understood, which is largely caused by mass transport limitations and lack of time-correlated product analysis tools. In this work, a custom-built gas accessible membrane electrode (GAME) system is used to comparatively assess the CO2RR behavior of Au and Au−Cu catalysts...
Under mild conditions of room temperature and pressure, and using either pure oxygen or air, aldehydes are converted using a heterogeneous Fe–N/C catalyst to produce the corresponding organic peroxy acid and acylperoxy radicals, which forms the epoxide from cyclohexene with high yield (91% for isobutyraldehyde in O2). Real-time monitoring of the ra...
A novel radiolabelling method exploiting 11C-dithiocarbamate ligands has been used to generate 11C-labelled Au(I), Au(III), Pd(II) and Pt(II) complexes in high radiochemical yields (71–99%). Labelled complexes were prepared in a rapid one-pot procedure via the substitution reaction of 11C-dithiocarbamate ligands with appropriate transition metal ch...
Published in Journal of Artificial General Intelligence
In 2011, Hibbard suggested an intelligence measure for agents who compete in an adversarial sequence prediction game. We argue that Hibbard’s idea should actually be considered as two separate ideas: first, that the intelligence of such agents can be measured based on the growth rates of the runtimes of the competitors that they defeat; and second,...
A selective Pd-catalyzed C(3)–H cis-functionalization of piperidine and tetrahydropyran carboxylic acids is achieved using a C(4) aminoquinoline amide auxiliary. High mono- and cis-selectivity is attained by using mesityl carboxylic acid as an additive. Conditions are developed with significantly lower reaction temperatures (≤50 °C) than other repo...
Hydrous iridium oxides (IrOx) are the best oxygen evolution electrocatalysts available for operation in acidic environments. In this study, we employ time-resolved operando spectroelectrochemistry to investigate the redox-state kinetics of IrOx electrocatalyst films for both water and hydrogen peroxide oxidation. Three different redox species invol...
There is currently a disconnect between the high electrocatalyst oxygen reduction reaction (ORR) performance measured ex situ, using the rotating disc electrode (RDE), and the in situ membrane electrode assembly (MEA) performance. The disconnect in the electrocatalyst performance raises questions both about the pitfalls of the RDE technique at extr...
‘Frustrated Lewis pairs’ (FLPs) continue to exhibit unique reactivity for the reduction of organic substrates, yet to date the catalytic hydrogenation of an ester functionality has not been demonstrated. Here we report that iPr3SnNTf2 (1-NTf2; Tf = SO2CF3) is a more potent Lewis acid than the previously studied iPr3SnOTf; in an FLP with 2,4,6-colli...
Molecular materials are challenging to design as their packing arrangement and hence properties are subject to subtle variations in the interplay of soft intermolecular interactions that are difficult to predict. The rational design of new molecular materials with tailored properties is currently hampered by the lack of knowledge of how a candidate...
