Biomolecular Oxidative Damage Activated by Enzymatic Logic Systems: Biologically Inspired Approach

Abstract

Systems that perform oxidative damage to biomolecules through catalytic cascades in the presence of iron-redox labile species were activated by enzymatic logic gates that process chemical input signals according to built-in logic operations. AND/OR enzymatic logic gates were composed of glucose oxidase (GOx) and GOx/esterase, respectively. The AND/OR logic functions of the enzyme gates were activated by application of glucose-oxygen and glucose-ethyl acetate input signals, respectively. The enzymatic logic gates, upon activation by specific patterns of the chemical input signals, produced acidic solutions and triggered release of redox labile iron species from a complex that is unstable under acidic conditions. This resulted in the activation of a catalytic cascade, which produced reactive oxygen species (ROS) and subsequently yielded oxidative damage in biomolecules. Functional integration of the enzyme-based logic systems with the catalytic redox cascade that performs damage in biomolecules on demand is a first step towards "smart" systems capable of programmed detection, identification, and neutralization of potential biohazards.

Enzyme-based logic systems for information processing

“…133 A variety of biomedical and biotechnological applications could be envisaged for the developed hybrid systems. These applications can range from biochemical processes, e.g., biomolecular oxidative damage, 134 to bioelectronic devices, e.g., biofuel cells, 126,127,133,135 controlled by enzyme logic systems. As mentioned, the biocomputing approach reviewed here, paves the way to novel digital biosensors 18 processing multiplebiochemical signals and producing a combination of outputs dependent on a complex pattern of inputs.…”

A Monolayer-Based Setup for Optical Amplification

“…This concept, introduced in 1993 by de Silva (5), has seen a flurry of activity leading to the design of multitasking compounds (6), bioinspired systems (7)(8)(9)(10), and molecular networks (9,10) capable of mimicking in solution the basic properties of logic gates and circuits (1)(2)(3)(4), electronic locks (11,12), and even calculators (6,13). The prospect of using (bio)molecules as logic gates and circuits may open a unique route to further miniaturization of central processing units (CPUs) (14).…”

“…Molecular Boolean logic is an elegant way to describe and use changes in the physicochemical properties of a system or material as a result of a specific interaction (e.g., chemical, electrochemical, optical) that can transfer it in a different state − . This concept, introduced in 1993 by de Silva , has seen a flurry of activity leading to the design of multitasking compounds , bioinspired systems − , and molecular networks , capable of mimicking in solution the basic properties of logic gates and circuits − , electronic locks , , and even calculators , . The prospect of using (bio)molecules as logic gates and circuits may open a unique route to further miniaturization of central processing units (CPUs).…”