As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The constructi...

Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

A fundamental change has been achieved in understanding surface electrochemistry due to the profound knowledge of the nature of electrocatalytic processes accumulated over the past several decades and to the recent technological advances in spectroscopy and high resolution imaging. Nowadays one can preferably design electrocatalysts based on the deep theoretical knowledge of electronic structures, via computer-guided engineering of the surface and (electro)chemical properties of materials, followed by the synthesis of practical materials with high performance for specific reactions. This review provides insights into both theoretical and experimental electrochemistry toward a better understanding of a series of key clean energy conversion reactions including oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The emphasis of this review is on the origin of the electrocatalytic activity of nanostructured catalysts toward the aforementioned reactions by correlating the apparent electrode performance with their intrinsic electrochemical properties. Also, a rational design of electrocatalysts is proposed starting from the most fundamental aspects of the electronic structure engineering to a more practical level of nanotechnological fabrication.

Design of electrocatalysts for oxygen- and hydrogen-involving energy conversion reactions

Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances. First, we introduce the unique advances on ultrathin 2D nanomaterials, followed by the description of their composition and crystal structures. The assortments of their synthetic methods are then summarized, including insights on their advantages and limitations, alongside some recommendations on suitable characterization techniques. We also discuss in detail the utilization of these ultrathin 2D nanomaterials for wide ranges of potential applications among the electronics/optoelectronics, electrocat...

Recent Advances in Ultrathin Two-Dimensional Nanomaterials

Graphene has attracted tremendous research interest in recent years, owing to its exceptional properties. The scaled-up and reliable production of graphene derivatives, such as graphene oxide (GO) and reduced graphene oxide (rGO), offers a wide range of possibilities to synthesize graphene-based functional materials for various applications. This critical review presents and discusses the current development of graphene-based composites. After introduction of the synthesis methods for graphene and its derivatives as well as their properties, we focus on the description of various methods to synthesize graphene-based composites, especially those with functional polymers and inorganic nanostructures. Particular emphasis is placed on strategies for the optimization of composite properties. Lastly, the advantages of graphene-based composites in applications such as the Li-ion batteries, supercapacitors, fuel cells, photovoltaic devices, photocatalysis, as well as Raman enhancement are described (279 references).

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Graphene-based composites

Graphene oxide: preparation, functionalization, and electrochemical applications.

Solar vapour generation is an efficient way of harvesting solar energy for the purification of polluted or saline water. However, water evaporation suffers from either inefficient utilization of solar energy or relies on complex and expensive light-concentration accessories. Here, we demonstrate a hierarchically nanostructured gel (HNG) based on polyvinyl alcohol (PVA) and polypyrrole (PPy) that serves as an independent solar vapour generator. The converted energy can be utilized in situ to power the vaporization of water contained in the molecular meshes of the PVA network, where water evaporation is facilitated by the skeleton of the hydrogel. A floating HNG sample evaporated water with a record high rate of 3.2 kg m−2 h−1 via 94% solar energy from 1 sun irradiation, and 18–23 litres of water per square metre of HNG was delivered daily when purifying brine water. These values were achievable due to the reduced latent heat of water evaporation in the molecular mesh under natural sunlight. Effective energy confinement via tailored water transport in hierarchical nanostructured gels enables highly efficient solar vapour generation.

Highly efficient solar vapour generation via hierarchically nanostructured gels

Solar-powered water evaporation — the extraction of vapour from liquid water using solar energy — provides the basis for the development of eco-friendly and cost-effective freshwater production. Liquid water consumes and carries energy, and, thus, plays an essential role in this process. As such, extensive experimental and theoretical studies have been focused on water management to achieve efficient solar vapour generation. Many innovative materials have been proposed to enable highly controllable and efficient solar-to-thermal energy conversion to address the challenges in the energy–water nexus from the microscale to the molecular level. In this Review, we summarize the fundamental principles of materials design for efficient solar-to-thermal energy conversion and vapour generation. We discuss how to integrate photothermal materials, nanostructures/microstructures and water–material interactions to improve the performance of the evaporation system via in situ utilization of solar energy. Focusing on materials science and engineering, we overview the key challenges and opportunities for nanostructured and microstructured materials in both fundamental research and practical water-purification applications. Materials engineering enables the control of water–material interactions in solar vapour generators, which aim to efficiently utilize solar energy for the cost-effective production of clean water. This Review discusses material-design principles for solar evaporators, spanning from macrostructures to molecular configurations.

Materials for solar-powered water evaporation

Solar desalination is a promising method for large-scale water purification by utilizing sustainable energy. However, current high-rate solar evaporation often relies on optical concentration due to the diffusion of natural sunlight, which leads to inadequate energy supply. Here we demonstrate a hydrogel-based solar evaporator that is capable of generating vapor at a high rate of ∼2.5 kg m−2 h−1 under one sun irradiation (1 kW m−2), among the best values reported in the literature. Such highly efficient solar evaporation is achieved by a hybrid hydrogel composed of a hydrophilic polymer framework (polyvinyl alcohol, PVA) and solar absorber (reduced graphene oxide, rGO), which has internal capillary channels. The PVA can greatly facilitate the water evaporation owing to the reduced water evaporation enthalpy in the hydrogel network. The rGO penetrating into the polymeric network enables efficient energy utilization. The capillary channels sustain an adequate water supply for continuous solar vapor generation at a high rate. This hydrogel-based solar evaporator also exhibits promising antifouling properties, enabling long-term water desalination without recycling. The high-efficiency hydrogel-based solar vapor generators open significant opportunities to enhance solar water evaporation performance and reduce the cost of solar desalination systems.

A hydrogel-based antifouling solar evaporator for highly efficient water desalination

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.

Water purification by solar distillation is a promising technology to produce fresh water. However, solar vapor generation, is energy intensive, leading to a low water yield under natural sunlight. Therefore, developing new materials that can reduce the energy requirement of water vaporization and speed up solar water purification is highly desirable. Here, we introduce a highly hydratable light-absorbing hydrogel (h-LAH) consisting of polyvinyl alcohol and chitosan as the hydratable skeleton and polypyrrole as the light absorber, which can use less energy ( −2  hour −1 under 1 sun. The h-LAH-based solar still also exhibits long-term durability and antifouling functionality toward complex ionic contaminants.

Fei Zhao

Papers

Highly efficient solar vapour generation via hierarchically nanostructured gels

Materials for solar-powered water evaporation

A hydrogel-based antifouling solar evaporator for highly efficient water desalination

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

Architecting highly hydratable polymer networks to tune the water state for solar water purification