Solution combustion synthesis: the relevant metrics for producing advanced and nanostructured photocatalysts.

The current developments and progress in energy and environment-related areas pay special attention to the fabrication of advanced nanomaterials via green and sustainable paths to accomplish chemical circularity. The design and preparation methods of photocatalysts play a prime role in determining the structural, surface characteristics and optoelectronic properties of the final products. The solution combustion synthesis (SCS) technique is a relatively novel, cost-effective, and efficient method for the bulk production of nanostructured materials. SCS-fabricated metal oxides are of great technological importance in photocatalytic, environmental and energy applications. To date, the SCS route has been employed to produce a large variety of solid materials such as metals, sulfides, carbides, nitrides and single or complex metal oxides. This review intends to provide a holistic perspective of the different steps involved in the chemistry of SCS of advanced photocatalysts, and pursues several SCS metrics that influence their photocatalytic performances to establish a feasible approach to design advanced photocatalysts. The study highlights the fundamentals of SCS and the importance of various combustion parameters in the characteristics of the fabricated photocatalysts. Consequently, this work deals with the design of a concise framework to link the fine adjustment of SCS parameters for the development of efficient metal oxide photocatalysts for energy and environmental applications.

Sustainable chemical processing of flowing wastewater through microwave energy.

Iron oxide nanostructured catalysts have emerged as potential candidates for efficient energy conversion and electrochemical energy storage devices. However, synthesis and design of nanomaterial plays a key role in its performance and efficiency. Herein, we describe a one-pot solution combustion synthesis (SCS) of α-Fe2O3 with glycine as a fuel, and a subsequent reduction step to produce iron-containing catalysts (i.e., Fe3O4, Fe-Fe3O4, and Fe0). The synthesized iron-based nanoparticles were investigated for methyl orange (MO) degradation through Microwave (MW) energy under continuous flow conditions. Fe-Fe3O4 showed higher MO degradation efficiency than α-Fe2O3, Fe3O4 and Fe0 at low absorbed MW power (i.e. 5-80 W). The enhanced degradation efficiency is associated to the combination of higher availability of electron density and higher heating effect under MW energy. Investigation of dielectric properties showed relative dielectric loss of Fe3O4, Fe-Fe3O4, and Fe0 as 3847, 2010, and 1952, respectively. The calculated average local temperature by the comparative analysis of MW treatment with conventional thermal (CT) treatment showed a marked thermal effect of MW-initiated MO degradation. This work highlights the potential of microwave-driven water depollution under continuous-flow processing conditions and demonstrates the positive impact that earth-abundant Fe catalyst synthesized by green SCS method can have over the treatment of wastewater.

Catalytic Activity of Various Carbons during the Microwave-Initiated Deep Dehydrogenation of Hexadecane.

Carbon materials have been widely used as microwave susceptors in many chemical processes because they are highly effective at transforming incoming electromagnetic energy for local (hot spot) heating. This property raises the intriguing possibility of using the all-pervasive carbonaceous deposits in operating heterogeneous catalytic processes to augment the catalytic performance of microwave-initiated reactions. Here, the catalytic activities of a range of carbon materials, together with carbon residues produced from a "test" reaction-the dehydrogenation of hexadecane under microwave-initiated heterogeneous catalytic processes, have been investigated. Despite the excellent microwave absorption properties observed among these various carbons, only activated carbons and graphene nanoplatelets were found to be highly effective for the microwave-initiated dehydrogenation of hexadecane. During the dehydrogenation of hexadecane on a Fe/SiC catalyst, active carbon species were formed at the early stage of the reactions but were subsequently transformed into filamentous but catalytically inert carbons that ultimately deactivated the operating catalyst.

Transforming carbon dioxide into jet fuel using an organic combustion-synthesized Fe-Mn-K catalyst.

With mounting concerns over climate change, the utilisation or conversion of carbon dioxide into sustainable, synthetic hydrocarbons fuels, most notably for transportation purposes, continues to attract worldwide interest. This is particularly true in the search for sustainable or renewable aviation fuels. These offer considerable potential since, instead of consuming fossil crude oil, the fuels are produced from carbon dioxide using sustainable renewable hydrogen and energy. We report here a synthetic protocol to the fixation of carbon dioxide by converting it directly into aviation jet fuel using novel, inexpensive iron-based catalysts. We prepare the Fe-Mn-K catalyst by the so-called Organic Combustion Method, and the catalyst shows a carbon dioxide conversion through hydrogenation to hydrocarbons in the aviation jet fuel range of 38.2%, with a yield of 17.2%, and a selectivity of 47.8%, and with an attendant low carbon monoxide (5.6%) and methane selectivity (10.4%). The conversion reaction also produces light olefins ethylene, propylene, and butenes, totalling a yield of 8.7%, which are important raw materials for the petrochemical industry and are presently also only obtained from fossil crude oil. As this carbon dioxide is extracted from air, and re-emitted from jet fuels when combusted in flight, the overall effect is a carbon-neutral fuel. This contrasts with jet fuels produced from hydrocarbon fossil sources where the combustion process unlocks the fossil carbon and places it into the atmosphere, in longevity, as aerial carbon - carbon dioxide.

Facile in situ reductive synthesis of both nitrogen deficient and protonated g-C3N4 nanosheets for the synergistic enhancement of visible-light H2 evolution.

A new strategy is reported here to synthesize both nitrogen deficient and protonated graphitic carbon nitride (g-C3N4) nanosheets by the conjoint use of NH4Cl as a dynamic gas template together with hypophosphorous acid (H3PO2) as a doping agent. The NH4Cl treatment allows for the scalable production of protonated g-C3N4 nanosheets. With the corresponding co-addition of H3PO2, nitrogen vacancies, accompanied by both additional protons and interstitially-doped phosphorus, are introduced into the g-C3N4 framework, and the electronic bandgap of g-C3N4 nanosheets as well as their optical properties and hydrogen-production performance can be precisely tuned by careful adjustment of the H3PO2 treatment. This conjoint approach thereby results in improved visible-light absorption, enhanced charge-carrier separation and a high H2 evolution rate of 881.7 µmol h-1 achieved over the H3PO2 doped g-C3N4 nanosheets with a corresponding apparent quantum yield (AQY) of 40.4% (at 420 nm). We illustrate that the synergistic H3PO2 doping modifies the layered g-C3N4 materials by introducing nitrogen vacancies as well as protonating them, leading to significant photocatalytic H2 evolution enhancements, while the g-C3N4 materials doped with phosphoric acid (H3PO4) are simply protonated further, revealing the varied doping effects of phosphorus having different (but accessible) valence states.

Rapid, non-invasive characterization of the dispersity of emulsions via microwaves.

A rapid and non-invasive method to determine the dispersity of emulsions is developed based on the interrelationship between the droplet size distribution and the dielectric properties of emulsions. A range of water-in-oil emulsions with different water contents and droplet size distributions were analysed using a microwave cavity perturbation technique together with dynamic light scattering. The results demonstrate that the dielectric properties, as measured by non-invasive microwave cavity analysis, can be used to characterise the dispersity of emulsions, and is also capable of characterizing heavy oil emulsions. This technique has great potential for industrial applications to examine the sedimentation, creaming and hence the stability of emulsions.

Rapid Production of High-Purity Hydrogen Fuel through Microwave-Promoted Deep Catalytic Dehydrogenation of Liquid Alkanes with Abundant Metals.

Hydrogen as an energy carrier promises a sustainable energy revolution. However, one of the greatest challenges for any future hydrogen economy is the necessity for large scale hydrogen production not involving concurrent CO2 production. The high intrinsic hydrogen content of liquid-range alkane hydrocarbons (including diesel) offers a potential route to CO2 -free hydrogen production through their catalytic deep dehydrogenation. We report here a means of rapidly liberating high-purity hydrogen by microwave-promoted catalytic dehydrogenation of liquid alkanes using Fe and Ni particles supported on silicon carbide. A H2 production selectivity from all evolved gases of some 98 %, is achieved with less than a fraction of a percent of adventitious CO and CO2 . The major co-product is solid, elemental carbon.