Carbon-based structures are the most versatile materials used in the modern field of renewable energy (i.e., in both generation and storage) and environmental science (e.g., purification/remediation). However, there is a need and indeed a desire to develop increasingly more sustainable variants of classical carbon materials (e.g., activated carbons, carbon nanotubes, carbon aerogels, etc.), particularly when the whole life cycle is considered (i.e., from precursor "cradle" to "green" manufacturing and the product end-of-life "grave"). In this regard, and perhaps mimicking in some respects the natural carbon cycles/production, utilization of natural, abundant and more renewable precursors, coupled with simpler, lower energy synthetic processes which can contribute in part to the reduction in greenhouse gas emissions or the use of toxic elements, can be considered as crucial parameters in the development of sustainable materials manufacturing. Therefore, the synthesis and application of sustainable carbon materials are receiving increasing levels of interest, particularly as application benefits in the context of future energy/chemical industry are becoming recognized. This review will introduce to the reader the most recent and important progress regarding the production of sustainable carbon materials, whilst also highlighting their application in important environmental and energy related fields.

Highly internal phase emulsion (polyHIPE) materials are promising macrocellular foams bearing versatile applications ranging from catalysis, optics, filtration, insulator and so forth. In this critical review water-in-oil HIPE, oil-in-water HIPE and Pickering-based HIPE are discussed. Also in each above-mentioned HIPE family, declination between the organic, inorganic or hybrid-organic foams chemical nature is proposed. The polyHIPE audience is thereby strongly interdisciplinary in nature crossing boundaries of physical chemistry, colloids, polymer science, sol-gel chemistry, hybrid materials, biology and beyond (114 references).

Acid pretreatment of lignocellulosic biomass, required for bioethanol production, generates large amounts of by-products, such as lignin and hydrolyzed hemicellulose fractions, which have found so far very limited applications. In this work, we demonstrate how the recovered hemicellulose hydrolysis products can be effectively utilized as a precursor for the synthesis of functional carbon materials through hydrothermal carbonization (HTC). The morphology and chemical structure of the synthesized HTC carbons are thoroughly characterized to highlight their similarities with glucose-derived HTC carbons. Furthermore, two routes for introducing porosity within the HTC carbon structure are presented: i) silica nanoparticle hard-templating, which is shown to be a viable method for the synthesis of carbonaceous hollow spheres; and ii) KOH chemical activation. The synthesized activated carbons (ACs) show an extremely high porosity (pore volume≈1.0 cm(3) g(-1)) mostly composed of micropores (90 % of total pore volume). Because of their favorable textural properties, the ACs are further tested as electrodes for supercapacitors, yielding very promising results (300 F g(-1) at 250 mA g(-1)) and confirming the high suitability of KOH-activated HTC carbons derived from spruce and corncob hydrolysis products as materials for electric double layer supercapacitors.

The production of carbon aerogels based on the conversion of inexpensive and abundant precursors using environmentally friendly processes is a highly attractive subject in materials chemistry today. This article reviews the latest developments regarding the rapidly developing field of carbonaceous aerogels prepared from biomass and biomass-derived precursors, highlighting exciting and innovative approaches to green, sustainable nanomaterial synthesis. A review of the state-of-the-art technologies will be provided with a specific focus on two complimentary synthetic approaches developed upon the principles of green chemistry. These carbonaceous aerogel synthesis strategies, namely the Starbon and carbogel approaches, can be regarded as "top-down" and "bottom-up" strategies, respectively. The structural properties can be easily tailored by controlling synthetic parameters such as the precursor selection and concentration, the drying technique employed and post-synthesis temperature annealing. In addition to these parameters, the behavior of these sustainable carbon aerogel platforms in a variety of environmental and energy-related applications will also be discussed, including water remediation and fuel cell chemistry (i.e., the oxygen reduction reaction). This Review reveals the fascinating variety of highly porous, versatile, nanostructured, and functional carbon-based aerogels accessible through the highlighted sustainable synthetic platforms.

A new sustainable approach based on the hydrothermal carbonization of biomass-derivatives is reported for the synthesis of nitrogen-doped carbon-based aerogels. The catalyst-free hydrothermal treatment of both carbohydrate-based derivatives, i.e. glucose, D-glucosamine and/or N-acetyl-D-glucosamine, and phenolic compounds, i.e. phloroglucinol and/or cyanuric acid, led to highly porous monolithic gels. After pyrolysis under an inert atmosphere, conductive N-doped carbon aerogels were obtained, displaying nitrogen-doping levels of 3-5 wt% and BET surface areas of up to 450 m 2 g −1 . These original materials showed the first promising results as electrocatalysts for the oxygen reduction reaction and are expected to be used in a wide variety of fields, including for advanced energy conversion and storage devices. † Electronic supplementary information (ESI) available. See

Carbon hollow spheres were produced using a sustainable approach, i.e. hydrothermal carbonization, using monosaccharides as carbon precursors and silica nanoparticles as hard-templates. Hydrothermal carbonization is an eco-efficient and cost-effective route to synthesize nanostructured carbonaceous materials from abundant biomass-derived molecules. After further thermal treatment under an inert atmosphere and removal of the silica-based core by chemical etching, porous hollow spheres depicting 5-8 nm thin shells were obtained. Subsequently, carbon-sulfur composites were synthesized via a melt diffusion method and used as nanostructured composites for cathodes in lithium-sulfur (Li-S) cells. The morphology of the hollow spheres was controlled and optimized to achieve improved electrochemical properties. Both high specific energies and high specific powers were obtained, due to the unique nanostructure of the hollow spheres. These results revealed that using optimized carbonaceous materials, it is possible to design sustainable Li-S cells showing promising electrochemical properties.

We show that we can select magnetically steerable nanopropellers from a set of carbon coated aggregates of magnetic nanoparticles using weak homogeneous rotating magnetic fields. The carbon coating can be functionalized, enabling a wide range of applications. Despite their arbitrary shape, all nanostructures propel parallel to the vector of rotation of the magnetic field. We use a simple theoretical model to find experimental conditions to select nanopropellers which are predominantly smaller than previously published ones.

The derivatization and covalent modification of biomass derived platform chemicals expand the biomass derived chemical spaces allowing for the preparation of new bioactive molecules and materials.