The ambient metastability of the rock-salt phase in well-defined model systems comprising nanospheres or nanorods of cadmium selenide, cadmium sulfide, or both was investigated as a function of composition, initial crystal phase, particle structure, shape, surface functionalization, and ordering level of their assemblies. Our experiments show that these nanocrystal systems exhibit ligand-tailorable reversibility in the rock salt–to–zinc blende solid-phase transformation. Interparticle sintering was used to engineer kinetic barriers in the phase transformation to produce ambient-pressure metastable rock-salt structures in a controllable manner. Interconnected nanocrystal networks were identified as an essential structure that hosted metastable high-energy phases at ambient conditions. These findings suggest general rules for transformation-barrier engineering that are useful in the rational design of next-generation materials.
This study describes a world of new carbon “fullerene” allotropes that may be synthesized by molten carbonate electrolysis using greenhouse CO2 as the reactant. Beyond the world of conventional diamond, graphite and buckyballs, a vast array of unique nanocarbon structures exist. Until recently, CO2 was thought to be unreactive. Here, we show that CO2 can be transformed into distinct nano-bamboo, nano-pearl, nano-dragon, solid and hollow nano-onion, nano-tree, nano-rod, nano-belt and nano-flower morphologies of carbon. The capability to produce these allotropes at high purity by a straightforward electrolysis, analogous to aluminum production splitting of aluminum oxide, but instead nanocarbon production by splitting CO2, opens an array of inexpensive unique materials with exciting new high strength, electrical and thermal conductivity, flexibility, charge storage, lubricant and robustness properties. Commercial production technology of nanocarbons had been chemical vapor deposition, which is ten-fold more expensive, generally requires metallo-organics reactants and has a highly carbon-positive rather than carbon-negative footprint. Different nanocarbon structures were prepared electrochemically by variation of anode and cathode composition and architecture, electrolyte composition, pre-electrolysis processing and current ramping and current density. Individual allotrope structures and initial growth mechanisms are explored by SEM, TEM, HAADF EDX, XRD and Raman spectroscopy.
Solar-boosted oxidation plus hydrogen production for pollutant removal in wastewater, driven by a high thermal and low-potential electrochemical combination, is facilitated and demonstrated from theory to experiments. One sun fully offers both thermal and electrical energy powered thermo- and electrochemistry for pollutant oxidation. Solar thermal action provides high temperatures for the activation of the pollutant molecules to gear up for solar-driven electrochemical oxidation. Taking wastewater containing phenol as an example, the cyclic voltammetry (CV) curves display two redox processes at less than 100 °C, while only one redox process of single oxidation of phenol appears at more than 100 °C. The oxidation of phenol is accompanied by an efficient evolution of hydrogen, in which the yield of 0.627 mL at 30 °C is increased to 2.294 mL at 210 °C. The phenol removal is enhanced to 80.50% at 210 °C. Tracking the reaction progress shows that small molecular organic acids are detected as the only intermediate at the high temperatures, which suggests the easy realization of full mineralization. The kinetic reaction of the phenol oxidation is fitted to the first order with an increase of the rate constant of 10 times compared with that at low temperatures. Solar engineering of oxidation of organic pollutants not only solves the issue of energy demand for the tough wastewater treatment but also realizes fast and efficient oxidation of organic pollutants. This study opens up new avenues to achieve solar wastewater treatment and simultaneous hydrogen production.
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