Catalytically active Janus particles suspended in solution create gradients in the chemical composition of the solution along their surfaces, as well as along any nearby container walls. The former leads to self-phoresis, while the latter gives rise to chemiosmosis, providing an additional contribution to self-motility. Chemiosmosis strongly depends on the molecular interactions between the diffusing chemical species and the wall. We show analytically, using an approximate "point-particle" approach, that by chemically patterning a planar substrate one can direct the motion of Janus particles: the induced chemiosmotic flows can cause particles to either "dock" at the chemical step between the two materials or follow a chemical stripe. These theoretical predictions are confirmed by full numerical calculations. Generically, docking occurs for particles which tend to move away from their catalytic caps, while stripe following occurs in the opposite case. Our analysis reveals the physical mechanisms governing this behavior.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1103/PhysRevLett.117.048002 | DOI Listing |
J Am Chem Soc
January 2025
Laboratory of Synthesis and Natural Products (LSPN), Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne, EPFL-SB-ISIC-LSPN, BCH 5304, CH-1015 Lausanne, Switzerland.
In the dyotropic rearrangement of molecules with semiflexible structures, characterized by a freely rotating static C-C bond, the formation of a mixture of products is common due to the coexistence of several energetically comparable conformers. Herein, we report that it is possible to modulate the shifting groups by adjusting the metal's coordination sphere in Pd-based dyotropic rearrangement. In the presence of a catalytic amount of Pd(II) salt, the reaction of γ-hydroxyalkenes or γ,δ-dihydroxyalkenes with Selectfluor affords fluorinated tetrahydropyranols or 6,8-dioxabicyclo[3.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, The Scripps Research Institute, 10550 N. Torrey Pines Road, La Jolla, California 92037, United States.
The development of catalytic methods for the synthesis of enantiopure saturated heterocycles has been a long-standing challenge in asymmetric catalysis. We describe the first highly enantioselective palladium-catalyzed βC(sp)-H arylation and olefination of lactams for the preparation of various chiral N-heterocycles bearing quaternary carbon centers. The presence of strongly electron-withdrawing groups on the chiral bifunctional MPAThio ligand is crucial to the reactivity of weakly coordinating lactams.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Although microenvironments surrounding single-atom catalysts (SACs) have been widely demonstrated to have a remarkable effect on their catalytic performances, it remains unclear whether the local structure beyond the secondary coordination shells works as well or not. Herein, we employed a series of metal-organic frameworks (MOFs) with well-defined and tunable second-beyond coordination spheres as model SAC electrocatalysts to discuss the influence of long-distance structure on the ammonia synthesis from nitrate, which were synthesized and denoted as Cu-NDI-X (X = NMe, H, F). It is first experimentally confirmed that the remote substitution of function groups beyond the secondary coordination sphere can remarkably affect the activity of ammonia synthesis.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Research Center for Solar Energy Chemistry and Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, Toyonaka 560-8531, Japan.
Photocatalytic transformation of nitrate (NO) in wastewater into ammonia (NH) is a challenge in the detoxification and recycling of limited nitrogen resources. In particular, previously reported photocatalysts cannot promote the reaction using water as an electron donor. Herein, we report that copper-doped titanium dioxide (Cu-TiO) powders, prepared via the sol-gel method and subsequent calcination, promote NO-to-NH reduction in water.
View Article and Find Full Text PDFSmall
January 2025
School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai, 200093, P. R. China.
Chlorophenols are difficult to degrade and mineralize by traditional advanced oxidation processes due to the strong electronegativity of chlorine. Here, a dual-site atomically dispersed catalyst (FeMoNC) is reported, which Fe/Mo supported on mesoporous nitrogen-doped carbon is prepared through high-temperature migration. The FeMoNC exhibits a high dechlorination rate of 93.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!