Abstract

Engineered living hydrogels that can protect cells from harsh environments have achieved preliminary successes in biomedicine and environmental remediation. However, their biocatalytic applications in pure organic solvents have not been explored. Here, living hydrogels were engineered by integrating genetically modified Escherichia coli cells into alginate hydrogels for robust biocatalysis in pure organic solvents. The biocompatible hydrogels could not only support cell growth and diminish cell escape but could also act as protective matrices to improve organic solvent tolerance, thereby prolonging catalytic activity of whole-cell biocatalysts. Moreover, the influence of hydrogel microenvironments on biocatalytic efficiency was thoroughly investigated. Importantly, the versatility of engineered living hydrogels paves the way to achieve robust biocatalytic efficiency in a variety of pure organic co-solvents. Overall, we are able to engineer living hydrogels for regio-selective synthesis in pure organic solvents, which may be particularly useful for the innovation of living hydrogels in biocatalysis. • Living hydrogels are engineered by integrating microbial cells and alginate hydrogels • Hydrogel microenvironments modulate catalytic efficiency of engineered living hydrogels • Engineered living hydrogels enable improved solvent tolerance in pure organic solvents • The versatility of engineered living hydrogels for robust biocatalysis is verified A versatile strategy to improve the organic solvent tolerance of whole-cell biocatalysts is highly demanded. Gao et al. design engineered living hydrogels using genetically modified microbial cells for improved organic solvent tolerance and robust biocatalysis in pure organic solvents.

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