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.
Electrocatalytic conversion of the greenhouse gas carbon dioxide to liquid fuels or upgraded chemicals is a critical strategy to mitigate anthropogenic climate change. Selectivity for one product at high activity...
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.
We report the selective hydroxylation of carbon surfaces that rendered initially hydrophobic carbon fiber paper hydrophilic for more than five months. This long time of sustained hydrophilicity is unprecedented. Carbon fiber paper is an inexpensive, electrically conductive, high surface area material that is additionally nontoxic, biocompatible, robust, and scalable. But its hydrophobicity prevents widespread use in aqueous applications. Inhibition of overoxidation of carbon beyond hydroxylation is especially challenging because the first oxidation step is thermodynamically most difficult and subsequent oxidations are much easier. We achieved selectivity for less oxidized hydroxyls over carboxyls by an environmentally friendly, solution-processable, acid-free carbon surface functionalization treatment that is rapid, amenable to large scale applications, and did not damage carbon fibers and their network architectures. The development of this mild, green chemistry carbon surface treatment that provides selectivity for surface hydroxyls transforms the utility of carbon materials.
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