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.

Pulsed Laser in Liquids Made Nanomaterials for Catalysis.

Ru/TiO2 catalyst for selective hydrogenation of benzene: Effect of surface hydroxyl groups and spillover hydrogen

Bimetallic Ru–M/TiO2 (M = Fe, Ni, Cu, Co) nanocomposite catalysts facribated by galvanic replacement: Structural elucidation and catalytic behavior in benzene selective hydrogenation

Ru-containing catalysts supported on halloysite aluminosilicate nanotubes (HNTs) were prepared by incipient wetness impregnation, vacuum impregnation, and impregnation under the microwave irradiation methods. Composition and structure of the catalysts were determined by X-ray fluorescence (XRF), thermo-programmed reduction (TPR-H2), and transmission electron microscopy (TEM). Textural characteristics were detected by low-temperature nitrogen adsorption—desorption. The activity of the catalysts was investigated in benzene hydrogenation at 80°?, a hydrogen pressure of 3.0 MPa, and a molar ratio of benzene to Ru of 2000. It was found that Ru nanoparticles prepared by vacuum impregnation are deposited mainly into the internal cavity of aluminosilicate nanotubes, while in samples obtained by wetness impregnation the active phase is formed predominantly on the external surface of halloysite. The catalyst prepared by impregnation under microwave irradiation is characterized by a high Ru content, its uniformly distributed metal particles are located mainly on the external surface of HNT, and it demonstrated the superior activity in hydrogenation of benzene to cyclohexane.

Effect of the ruthenium deposition method on the nanostructured catalyst activity in the deep hydrogenation of benzene

Bimetallic catalysts (BMC) for hydroconversion of aromatic hydrocarbons (ArH) have been designed by modification of Ni/Al2O3 with chromium(0) compounds and phosphoromolybdic heteropolyacid (HPA). Catalysts were tested in hydrogenation of benzene and toluene, in hydrodemethylation of pure toluene and they were shown to possess a high activity, selectivity and sulfur tolerance under conditions of the processes above. The activity of BMC in these processes was much higher as compared with that of two-component (Ni-Cr, Ni-HPA) or conventional Ni/Al2O3 catalysts. Using BMC, hydrogenation of benzene and toluene proceeds with activity increased (up to 34–38 mol/kg·h) and toluene hydrodemethylation may be performed with improved selectivity (90.3%) and benzene yield (81%). The high sulfur tolerance of BMC was demonstrated by performing hydrodemethylation of toluene containing up to 500 ppm S.

Hydroconversion of Aromatic Hydrocarbons over Bimetallic Catalysts

In recent years, the defect engineering of titania via reduction treatments has shown a high potential for enabling efficient and co-catalyst-free photocatalytic H2 generation from methanol/water solutions. However, defect engineering simultaneously alters several properties of TiO2. Here, we use pristine (white) and hydrogenated (gray) anatase nanosheets with dominant (001) facets. By comparing electrical conductivity, photocurrent spectra, transient photocurrent response, and photocatalytic H2 evolution, we show that the increased conductivity or broad visible light absorption of gray titania is not responsible for its increased activity. Instead, the true bottleneck is the hole transfer rate that is significantly accelerated while using gray instead of white modification. Moreover, the hole transfer reaction causes the accumulation of the reaction products in pure water, hindering the photocatalytic H2 evolution over time. These combined factors explain the superior performance of gray titania over white titania in photoelectrochemical or photocatalytic water splitting.

Critical factors for photoelectrochemical and photocatalytic H2 evolution from gray anatase (001) nanosheets

Construction of bismuth-deposited Bi4O5Br2 complex and exploration of its photocatalytic properties

Effect of support composition on the structural and catalytic properties of Ru/AlOOH–SiO2 catalysts for benzene selective hydrogenation

In the present work, the spontaneous dewetting of thin Au layers on single crystalline anatase nanosheets into narrow-disperse Au nanoparticles is investigated. Patterns of the Au particles can be formed on the main facets of anatase that provide a high co-catalytic activity for photocatalytic generation of H2 . Dewetting is distinctly influenced by the respective facets (001) and (101), the deposit thickness, and secondary thermal dewetting, but most strongly by the surface termination of the nanosheets. Fluoride termination not only leads to an enhanced Au-phobic behavior but strongly affects the co-catalytic activity for photocatalytic generation of H2 . While fluoride termination with or without Au decoration is detrimental for hole transfer, the interplay of the Au co-catalyst and surface fluoride yields highly beneficial effect for electron transfer. This results in a three-times higher photocatalytic H2 production for the F-terminated surface. The findings suggest that dewetting of Au on surface fluorinated TiO2 is an effective way to modulate surface dewetting and achieve a strongly enhanced photocatalytic activity.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/smll.202303306

Spontaneous Dewetting of Au-Thin Layers on Oxide- and Fluorine-Terminated Single Crystalline Anatase and Efficient Use in Photocatalytic H2 Production.

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Critical factors for photoelectrochemical and photocatalytic H2 evolution from gray anatase (001) nanosheets

Construction of bismuth-deposited Bi4O5Br2 complex and exploration of its photocatalytic properties

Effect of support composition on the structural and catalytic properties of Ru/AlOOH–SiO2 catalysts for benzene selective hydrogenation

Spontaneous Dewetting of Au-Thin Layers on Oxide- and Fluorine-Terminated Single Crystalline Anatase and Efficient Use in Photocatalytic H2 Production.