Interactive Materials for Bidirectional Redox-Based Communication.

Emerging research indicates that biology routinely uses diffusible redox-active molecules to mediate communication that can span biological systems (e.g., nervous and immune) and even kingdoms (e.g., a microbiome and its plant/animal host). This redox modality also provides new opportunities to create interactive materials that can communicate with living systems. Here, it is reported that the fabrication of a redox-active hydrogel film can autonomously synthesize a H2 O2 signaling molecule for communication with a bacterial population. Specifically, a catechol-conjugated/crosslinked 4-armed thiolated poly(ethylene glycol) hydrogel film is electrochemically fabricated in which the added catechol moieties confer redox activity: the film can accept electrons from biological reductants (e.g., ascorbate) and donate electrons to O2 to generate H2 O2 . Electron-transfer from an Escherichia coli culture poises this film to generate the H2 O2 signaling molecule that can induce bacterial gene expression from a redox-responsive operon. Overall, this work demonstrates that catecholic materials can participate in redox-based interactions that elicit specific biological responses, and also suggests the possibility that natural phenolics may be a ubiquitous biological example of interactive materials.

Synthetic biology as driver for the biologization of materials sciences.

Materials in nature have fascinating properties that serve as a continuous source of inspiration for materials scientists. Accordingly, bio-mimetic and bio-inspired approaches have yielded remarkable structural and functional materials for a plethora of applications. Despite these advances, many properties of natural materials remain challenging or yet impossible to incorporate into synthetic materials. Natural materials are produced by living cells, which sense and process environmental cues and conditions by means of signaling and genetic programs, thereby controlling the biosynthesis, remodeling, functionalization, or degradation of the natural material. In this context, synthetic biology offers unique opportunities in materials sciences by providing direct access to the rational engineering of how a cell senses and processes environmental information and translates them into the properties and functions of materials. Here, we identify and review two main directions by which synthetic biology can be harnessed to provide new impulses for the biologization of the materials sciences: first, the engineering of cells to produce precursors for the subsequent synthesis of materials. This includes materials that are otherwise produced from petrochemical resources, but also materials where the bio-produced substances contribute unique properties and functions not existing in traditional materials. Second, engineered living materials that are formed or assembled by cells or in which cells contribute specific functions while remaining an integral part of the living composite material. We finally provide a perspective of future scientific directions of this promising area of research and discuss science policy that would be required to support research and development in this field.

Vision Statement: Interactive Materials-Drivers of Future Robotic Systems.

A robot senses its environment, processes the sensory information, acts in response to these inputs, and possibly communicates with the outside world. Robots generally achieve these tasks with electronics-based hardware or by receiving inputs from some external hardware. In contrast, simple microorganisms can autonomously perceive, act, and communicate via purely physicochemical processes in soft material systems. A key property of biological systems is that they are built from energy-consuming "active" units. Exciting developments in material science show that even very simple artificial active building blocks can show surprisingly rich emergent behaviors. Active nonequilibrium systems are therefore predicted to play an essential role in realizing interactive materials. A major challenge is to find robust ways to couple and integrate the energy-consuming building blocks to the mechanical structure of the material. However, success in this endeavor will lead to a new generation of sophisticated micro and soft-robotic systems that can operate autonomously.

Design Principles for Aqueous Interactive Materials: Lessons from Small Molecules and Stimuli-Responsive Systems.

Interactive materials are at the forefront of current materials research with few examples in the literature. Researchers are inspired by nature to develop materials that can modulate and adapt their behavior in accordance with their surroundings. Stimuli-responsive systems have been developed over the past decades which, although often described as "smart," lack the ability to act autonomously. Nevertheless, these systems attract attention on account of the resultant materials' ability to change their properties in a predicable manner. These materials find application in a plethora of areas including drug delivery, artificial muscles, etc. Stimuli-responsive materials are serving as the precursors for next-generation interactive materials. Interest in these systems has resulted in a library of well-developed chemical motifs; however, there is a fundamental gap between stimuli-responsive and interactive materials. In this perspective, current state-of-the-art stimuli-responsive materials are outlined with a specific emphasis on aqueous macroscopic interactive materials. Compartmentalization, critical for achieving interactivity, relies on hydrophobic, hydrophilic, supramolecular, and ionic interactions, which are commonly present in aqueous systems and enable complex self-assembly processes. Relevant examples of aqueous interactive materials that do exist are given, and design principles to realize the next generation of materials with embedded autonomous function are suggested.

Vision Statement: Materials in Motion.

At the dawn of a new era of interactive and responsive materials and dynamic molecular systems there is ample opportunity to raise the level of complexity enabling mechanical motion, autonomous behavior, or interactive self-regulatory functions. Some of the major challenges and opportunities are discussed with a brief perspective toward future developments on responsive materials.

Viewpoint: From Responsive to Adaptive and Interactive Materials and Materials Systems: A Roadmap.

Soft matter systems and materials are moving toward adaptive and interactive behavior, which holds outstanding promise to make the next generation of intelligent soft materials systems inspired from the dynamics and behavior of living systems. But what is an adaptive material? What is an interactive material? How should classical responsiveness or smart materials be delineated? At present, the literature lacks a comprehensive discussion on these topics, which is however of profound importance in order to identify landmark advances, keep a correct and noninflating terminology, and most importantly educate young scientists going into this direction. By comparing different levels of complex behavior in biological systems, this Viewpoint strives to give some definition of the various different materials systems characteristics. In particular, the importance of thinking in the direction of training and learning materials, and metabolic or behavioral materials is highlighted, as well as communication and information-processing systems. This Viewpoint aims to also serve as a switchboard to further connect the important fields of systems chemistry, synthetic biology, supramolecular chemistry and nano- and microfabrication/3D printing with advanced soft materials research. A convergence of these disciplines will be at the heart of empowering future adaptive and interactive materials systems with increasingly complex and emergent life-like behavior.