This paper gives a comprehensive review about the most recent progress in synthesis, characterization, fundamental understanding, and the performance of graphene and graphene oxide sponges. Practical applications are considered including use in composite materials, as the electrode materials for electrochemical sensors, as absorbers for both gases and liquids, and as electrode materials for devices involved in electrochemical energy storage and conversion. Several advantages of both graphene and graphene oxide sponges such as three dimensional graphene networks, high surface area, high electro/thermo conductivities, high chemical/electrochemical stability, high flexibility and elasticity, and extremely high surface hydrophobicity are emphasized. To facilitate further research and development, the technical challenges are discussed, and several future research directions are also suggested in this paper.

A review of graphene and graphene oxide sponge: material synthesis and applications to energy and the environment

As swollen polymer networks in water, hydrogels are usually brittle. However, hydrogels with high toughness play critical roles in many plant and animal tissues as well as in diverse engineering applications. Here we review the intrinsic mechanisms of a wide variety of tough hydrogels developed over the past few decades. We show that tough hydrogels generally possess mechanisms to dissipate substantial mechanical energy but still maintain high elasticity under deformation. The integrations and interactions of different mechanisms for dissipating energy and maintaining elasticity are essential to the design of tough hydrogels. A matrix that combines various mechanisms is constructed for the first time to guide the design of next-generation tough hydrogels. We further highlight that a particularly promising strategy for the design is to implement multiple mechanisms across multiple length scales into nano-, micro-, meso-, and macro-structures of hydrogels.

Multi-scale multi-mechanism design of tough hydrogels: building dissipation into stretchy networks

Avoiding wound infection and retaining an appropriate level of moisture around woundz are major challenges in wound care management. Therefore, designing hydrogels with desired antibacterial performance and good water-maintaining ability is of particular significance to promote the development of wound dressing. Thus a series of hydrogels are prepared by crosslinking of Ag/graphene composites with acrylic acid and N,N'-methylene bisacrylamide at different mass ratios. The antibacterial performance and accelerated wound-healing ability of hydrogel are systematically evaluated with the aim of attaining a novel and effective wound dressing. The as-prepared hydrogel with the optimal Ag to graphene mass ratio of 5:1 (Ag5G1) exhibits stronger antibacterial abilities than other hydrogels. Meanwhile, Ag5G1 hydrogel exhibits excellent biocompatibility, high swelling ratio, and good extensibility. More importantly, in vivo experiments indicate that Ag5G1 hydrogel can significantly accelerate the healing rate of artificial wounds in rats, and histological examination reveals that it helps to successfully reconstruct intact and thickened epidermis during 15 day of healing of impaired wounds. In one word, the present approach can shed new light on designing of antibacterial material like Ag/graphene composite hydrogel with promising applications in wound dressing.

A Novel Wound Dressing Based on Ag/Graphene Polymer Hydrogel: Effectively Kill Bacteria and Accelerate Wound Healing

Energy and water are of fundamental importance for our modern society, and advanced technologies on sustainable energy storage and conversion as well as water resource management are in the focus of intensive research worldwide. Beyond their traditional biological applications, hydrogels are emerging as an appealing materials platform for energy- and water-related applications owing to their attractive and tailorable physiochemical properties. In this review, we highlight the highly tunable synthesis of various hydrogels, involving key synthetic elements such as monomer/polymer building blocks, cross-linkers, and functional additives, and discuss how hydrogels can be employed as precursors and templates for architecting three-dimensional frameworks of electrochemically active materials. We then present an in-depth discussion of the structure-property relationships of hydrogel materials based on fundamental gelation chemistry, ultimately targeting properties such as enhanced ionic/electronic conductivities, mechanical strength, flexibility, stimuli-responsiveness, and desirable swelling behavior. The unique interconnected porous structures of hydrogels enable fast charge/mass transport while offering large surface areas, and the polymer-water interactions can be regulated to achieve desirable water retention, absorption, and evaporation within hydrogels. Such structure-derived properties are also intimately coordinated to realize multifunctionality and stability for different target devices. The plethora of stimulating examples is expounded with a focus on batteries, supercapacitors, electrocatalysts, solar water purification, and atmospheric water harvesting, which showcase the unprecedented technological potential enabled by hydrogels and hydrogel-derived materials. Finally, we study the challenges and potential ways of tackling them to reveal the underlying mechanisms and transform the current development of hydrogel materials into sustainable energy and water technologies.

Hydrogels and Hydrogel-Derived Materials for Energy and Water Sustainability.

3D printing alias additive manufacturing can transform 3D virtual models created by computer-aided design (CAD) into physical 3D objects in a layer-by-layer manner dispensing with conventional molding or machining. Since the incipiency, significant advancements have been achieved in understanding the process of 3D printing and the relationship of component, structure, property and application of the created objects. Because hydrogels are one of the most feasible classes of ink materials for 3D printing and this field has been rapidly advancing, this Review focuses on hydrogel designs and development of advanced hydrogel-based biomaterial inks and bioinks for 3D printing. It covers 3D printing techniques including laser printing (stereolithography, two-photon polymerization), extrusion printing (3D plotting, direct ink writing), inkjet printing, 3D bioprinting, 4D printing and 4D bioprinting. It provides a comprehensive overview and discussion of the tailorability of material, mechanical, physical, chemical and biological properties of hydrogels to enable advanced hydrogel designs for 3D printing. The range of hydrogel-forming polymers covered encompasses biopolymers, synthetic polymers, polymer blends, nanocomposites, functional polymers, and cell-laden systems. The representative biomedical applications selected demonstrate how hydrogel-based 3D printing is being exploited in tissue engineering, regenerative medicine, cancer research, in vitro disease modeling, high-throughput drug screening, surgical preparation, soft robotics and flexible wearable electronics. Incomparable by thermoplastics, thermosets, ceramics and metals, hydrogel-based 3D printing is playing a pivotal role in the design and creation of advanced functional (bio)systems in a customizable way. An outlook on future directions of hydrogel-based 3D printing is presented.

3D printing of hydrogels: Rational design strategies and emerging biomedical applications

Polyacrylamide (PAM)/graphene oxide (GO) nanocomposite hydrogels (PGH) with GO nanosheets as cross-linkers were synthesized via in situ free radical polymerization of acrylamide in an aqueous suspension of GO. The tensile properties of the hydrogels were investigated in terms of type and content of cross-linkers. Compared to conventional PAM hydrogels (PBH) cross-linked chemically with N,N′-methylenebisacrylamide, PGH exhibits high tensile strength, high toughness and especially a large elongation at break. The tensile strength of PGH is about 4.5 times higher than that of PBH, and the elongation at break is over 3000%, nearly one order higher than that of PBH even when the content of GO is only 0.0079 wt%. By analyzing the cross-linked structure of PGH and the theoretical calculation on the number of cross-linked polymer chains per unit volume of gels, a structure model was thus proposed.

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Songmiao Liang

Papers

Tough and highly stretchable graphene oxide/polyacrylamide nanocomposite hydrogels