Cascade nanozymatic network mimicking cells with selective and linear perception of H2O2

Abstract

A single stimulus leading to multiple responses is an essential function of many biological networks, which enable complex life activities. However, it is challenging to duplicate a similar chemical reaction network (CRN) using non-living chemicals, aiming at the disclosure of the origin of life. Herein, we report a nanozyme-based CRN with feedback and feedforward functions for the first time. It demonstrates multiple responses at different modes and intensities upon a single H₂O₂ stimulus. In the two-electron cascade oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB), the endogenous product H₂O₂ competitively inhibited substrates in the first one-electron oxidation reaction on a single-atom nanozyme (Co-N-CNTs) and strikingly accelerated the second one-electron oxidation reaction under a micellar nanozyme. As a proof-of-concept, we further confined the nanozymatic network to a microfluidic chip as a simplified artificial cell. It exhibited remarkable selectivity and linearity in the perception of H₂O₂ stimulus against more than 20 interferences in a wide range of concentrations (0.01–100 mM) and offered an instructive platform for studying primordial life-like processes.