Single-Stranded DNA-Encoded Gold Nanoparticle Clusters as Programmable Enzyme Equivalents

Xiaoliang Chen, Yue Wang, Xinpei Dai, Longjiang Ding, Jielin Chen, Guangbao Yao, Xiaoguo Liu, Shihua Luo, Jiye Shi, Lihua Wang, Rachel Nechushtai, Eli Pikarsky, Itamar Willner, Chunhai Fan, Jiang Li*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

41 Scopus citations

Abstract

Nanozymes have emerged as a class of novel catalytic nanomaterials that show great potential to substitute natural enzymes in various applications. Nevertheless, spatial organization of multiple subunits in a nanozyme to rationally engineer its catalytic properties remains to be a grand challenge. Here, we report a DNA-based approach to encode the organization of gold nanoparticle clusters (GNCs) for the construction of programmable enzyme equivalents (PEEs). We find that single-stranded (ss-) DNA scaffolds can self-fold into nanostructures with prescribed poly-adenine (polyA) loops and double-stranded stems and that the polyA loops serve as specific sites for seed-free nucleation and growth of GNCs with well-defined particle numbers and interparticle spaces. A spectrum of GNCs, ranging from oligomers with discrete particle numbers (2-4) to polymer-like chains, are in situ synthesized in this manner. The polymeric GNCs with multiple spatially organized nanoparticles as subunits show programmable peroxidase-like catalytic activity that can be tuned by the scaffold size and the inter-polyA spacer length. This study thus opens new routes to the rational design of nanozymes for various biological and biomedical applications.

Original languageAmerican English
Pages (from-to)6311-6320
Number of pages10
JournalJournal of the American Chemical Society
Volume144
Issue number14
DOIs
StatePublished - 13 Apr 2022

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