JultikaUniversity of Oulu repository

Spacetime defines existence and evolution of materials. A key path to human’s sustainability through materials innovation can hardly circumvent materials dimensionalities. Despite numerous studies in electrically distinct 2D semiconductors, the route to engage them in high-performance photocatalysts remains elusive. Herein, CATCH proposes a cross-dimensional activation strategy of 2D semiconductors to implement practical photocatalysis. It operates electronic structures of dimensionally paradoxical 2D semiconductors and spatially limited nD (n=0-2) guests, directs charge migration processes, mass-produces advanced catalysts and elucidates time-evolved catalysis. Synergic impacts crossing 2D-nD will lead to > 95%/hour rates for pollutant removal and >20% quantum efficiencies for H2 evolution under visible light. CATCH enumerates chemical coordination and writes reaction equations with sub-nanosecond precision. CATCH employs density functional theory optimization and data mining prediction to select most probable heterojunctional peers from hetero/homo- dimensions. Through facile but efficient wet and dry synthesis, nanostructures will be bonded to basal planes or brinks of 2D slabs. CATCH benefits in-house techniques for product characterizations and refinements and emphasizes on cutting-edge in situ studies to unveil photocatalysis at advanced photon sources. Assisted with theoretical modelling, ambient and time-evolved experiments will illustrate photocatalytic dynamics and kinetics in mixed spacetime. CATCH unites low-dimensional materials designs by counting physical and electronic merits from spacetime confinements. It metrologically elaborates photocatalysis in an elevated 2D+nD+t, alters passages of materials combinations crossing dimensions, and directs future photocatalyst designs. Standing on cross-dimensional materials innovation and photocatalysis study, CATCH breaks the deadlock of practical photocatalysis that eventually leads to sustainability.