Abstract
Metal-catalyzed chemical transformations performed at the cellular level bear great potential for the manipulation of biological processes. The complexity of the cell renders the use of transition metal chemistry difficult in cellular systems. The delivery of the reactive catalyst and the control of its spatial localization remain challenging. Here we report the surface functionalization of the unicellular eukaryote Chlamydomonas reinhardtii with a tailor-made artificial metalloenzyme for on-cell catalysis. The functionalized cells remain viable and are able to uncage a fluorogenic substrate on their surface. This work leverages cell surface engineering to provide live cells with new-to-nature reactivity. In addition, this operationally simple approach is not genetically encoded and thereby transient, which offers advantages with regard to temporal control, cell viability, and safety. Therefore, and as a feature, the movement of the functionalized cells can be directed by light (via phototaxis), allowing for the three-dimensional localization of catalysts by outside stimuli.
Highlights
Metal-catalyzed chemical transformations performed at the cellular level bear great potential for the manipulation of biological processes
We report the surface functionalization of live Chlamydomonas reinhardtii cells with a tailor-made artificial allylic deallylase for on-cell catalysis
The approach developed here does not rely on the biological machinery of the target cell but takes advantage of chemical surface functionalization to introduce the artificial metalloenzyme
Summary
Metal-catalyzed chemical transformations performed at the cellular level bear great potential for the manipulation of biological processes. Surface functionalization of live cells with an artificial metalloenzyme could allow both reactivity and spatial control over the desired transformation. In this context, bacterial surface display has emerged as a promising technology for the development and the study of new reactions at a cellular level[34,41]. We reasoned that the functionalization of the cell surface of an eukaryote without relying on genetic means would represent an attractive alternative Such approach might offer flexibility by allowing time control of the functionalization, being non-hereditary and operationally simple to perform
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