Advanced electrocatalytic redox processes for environmental remediation of halogenated organic water pollutants.

Halogenated organic compounds are widespread, and decades of heavy use have resulted in global bioaccumulation and contamination of the environment, including water sources. Here, we introduce the most common halogenated organic water pollutants, their classification by type of halogen (fluorine, chlorine, or bromine), important policies and regulations, main applications, and environmental and human health risks. Remediation techniques are outlined with particular emphasis on carbon-halogen bond strengths. Aqueous advanced redox processes are discussed, highlighting mechanistic details, including electrochemical oxidations and reductions of the water-oxygen system, and thermodynamic potentials, protonation states, and lifetimes of radicals and reactive oxygen species in aqueous electrolytes at different pH conditions. The state of the art of aqueous advanced redox processes for brominated, chlorinated, and fluorinated organic compounds is presented, along with reported mechanisms for aqueous destruction of select PFAS (per- and polyfluoroalkyl substances). Future research directions for aqueous electrocatalytic destruction of organohalogens are identified, emphasizing the crucial need for developing a quantitative mechanistic understanding of degradation pathways, the improvement of analytical detection methods for organohalogens and transient species during advanced redox processes, and the development of new catalysts and processes that are globally scalable.

Melt-Processed Halide Perovskite Thin Films from a Two-Dimensional Ruddlesden-Popper Phase Precursor.

While halide perovskite thin films have enormous potential for photovoltaics and other optoelectronics, the use of environmentally hazardous solvents during their deposition and processing poses a barrier to their commercialization. In this work, we demonstrated the deposition of melt-processable precursors and subsequent transformation into halide perovskite thin films without using environmentally hazardous solvents. We melted the wide-bandgap layered perovskites [(C6H5CH(CH3)CH2NH3)2PbI4:ß-Me-PEA2PbI4] at ∼210 °C and blade coated them into films. The ß-Me-PEA2PbI4 films were subsequently transformed to perovskite-phase methylammonium or formamidinium lead iodide films using a cation-exchange process in an alcohol-based solvent. Lastly, we demonstrate the potential and limitations of a completely solvent-free approach that uses solid-state transformation of a ß-Me-PEA2PbI4 film. This work represents a substantial step toward eliminating environmentally hazardous solvents and enables inexpensive industrial-scale liquid-phase deposition processes that do not require expensive systems for handling and disposing of environmentally hazardous solvents.

Analysis of the Scale of Global Human Needs and Opportunities for Sustainable Catalytic Technologies.

We analyzed the enormous scale of global human needs, their carbon footprint, and how they are connected to energy availability. We established that most challenges related to resource security and sustainability can be solved by providing distributed, affordable, and clean energy. Catalyzed chemical transformations powered by renewable electricity are emerging successor technologies that have the potential to replace fossil fuels without sacrificing the wellbeing of humans. We highlighted the technical, economic, and societal advantages and drawbacks of short- to medium-term decarbonization solutions to gauge their practicability, economic feasibility, and likelihood for widespread acceptance on a global scale. We detailed catalysis solutions that enhance sustainability, along with strategies for catalyst and process development, frontiers, challenges, and limitations, and emphasized the need for planetary stewardship. Electrocatalytic processes enable the production of solar fuels and commodity chemicals that address universal issues of the water, energy and food security nexus, clothing, the building sector, heating and cooling, transportation, information and communication technology, chemicals, consumer goods and services, and healthcare, toward providing global resource security and sustainability and enhancing environmental and social justice. Supplementary Information: The online version contains supplementary material available at 10.1007/s11244-023-01799-3.

Pulsed Laser in Liquids Made Nanomaterials for Catalysis.

Catalysis is essential to modern life and has a huge economic impact. The development of new catalysts critically depends on synthetic methods that enable the preparation of tailored nanomaterials. Pulsed laser in liquids synthesis can produce uniform, multicomponent, nonequilibrium nanomaterials with independently and precisely controlled properties, such as size, composition, morphology, defect density, and atomistic structure within the nanoparticle and at its surface. We cover the fundamentals, unique advantages, challenges, and experimental solutions of this powerful technique and review the state-of-the-art of laser-made electrocatalysts for water oxidation, oxygen reduction, hydrogen evolution, nitrogen reduction, carbon dioxide reduction, and organic oxidations, followed by laser-made nanomaterials for light-driven catalytic processes and heterogeneous catalysis of thermochemical processes. We also highlight laser-synthesized nanomaterials for which proposed catalytic applications exist. This review provides a practical guide to how the catalysis community can capitalize on pulsed laser in liquids synthesis to advance catalyst development, by leveraging the synergies of two fields of intensive research.