Three-dimensional electrodes offer great advantages, such as enhanced ion and electron transport, increased material loading per unit substrate area, and improved mechanical stability upon repeated charge-discharge. The origin of these advantages is discussed and the criteria for ideal 3D electrode structure are outlined. One of the common features of ideal 3D electrodes is the use of a 3D carbon- or metal-based porous framework as the structural backbone and current collector. The synthesis methods of these 3D frameworks and their composites with redox-active materials are summarized, including transition metal oxides and conducting polymers. The structural characteristics and electrochemical performances are also reviewed. Synthesis of composite 3D electrodes is divided into two types - template-assisted and template-free methods - depending on whether a pre-made template is required. The advantages and drawbacks of both strategies are discussed.

Membrane-based architectures enable optimization of charge transport and electrochemical potential gradients in artificial photosynthesis.

This study describes the use of a benzimidazolium-based anion exchange membrane for creating bipolar membranes and the assessment of their suitability for solar-driven water splitting. Bipolar membranes were prepared by laminating anion exchange membrane with Nafion NR-211 membrane without modification of the interface. Under acidic and basic conditions, proton and hydroxide ion conductivities of 103 and 102 mS cm were obtained for Nafion and benzimidazolium-based membranes, respectively. The fabricated bipolar membranes have an average thickness of 90 μm and show high transmittance, up to 75% of the visible light. The findings suggest that the two membranes create a sharp hydrophilic interface with a space charge region of only a few nanometers, thereby generating a large electric field at the interface that enhances water dissociation.

Ultralight and strong three-dimensional (3D) silicon carbide (SiC) structures have been generated by the carbothermal reduction of SiO with a graphene foam (GF). The resulting SiC foams have an average height of 2 mm and density ranging between 9 and 17 mg cm(-3). They are the lightest reported SiC structures. They consist of hollow struts made from ultrathin SiC flakes and long 1D SiC nanowires growing from the trusses, edges, and defect sites between layers. AFM results revealed an average flake thickness of 2-3 nm and lateral size of 2 μm. In-situ compression tests in the scanning electron microscope (SEM) show that, compared with most of the existing lightweight foams, the present 3D SiC exhibited superior compression strengths and significant recovery after compression strains of about 70%.

Three dimensional (3D) graphene-based architectures such as 3D graphene-based hydrogels, aerogels, foams, and sponges have attracted huge attention owing to the combination of the structural interconnectivities and the outstanding properties of graphene which offer these interesting structures with low density, high porosity, large surface area, stable mechanical properties, fast mass and electron transport. They have been extensively studied for a wide range of applications including capacitors, batteries, sensors, catalyst, etc. There are several reviews focusing on the 3D graphene-based architectures and their applications. In this work, we only summarise the latest development on the preparation of 3D graphene-based architectures and their applications in supercapacitors, with emphasis on the preparation strategies. Crown