Fig. 2: Concentration screening and proposed mechanism of the organocatalysed aldol-oligomerisation and incorporation of the reaction product aldehydes into the organocatalyst.

a Micrographs of an aqueous solution. Scale bar: 10 µm. b Extracted HRMS data of catalyst-masses with chain lengths of 2 − 20 plotted against dehydration grade extracted for [M + H]⁺. Reaction conditions for a and b: 0.2, 0.5 or 2.0 m acetaldehyde from left to right, with 1, 10 or 20 mol% catalyst loading from top to bottom after 1 d. Sample dilution was referenced to catalyst concentration for every acetaldehyde concentration. c Proposed interlocking catalytic cascade of organocatalysed aldol-oligomerisation reaction and molecular self-modification of the catalyst.