| Resumo: | 28 pages. -- PDF file includes: Experimental Procedures; Simulation of hard polyhedral particles in spherical confinement. -- Figure S1. (a) Scheme and FESEM image of an as-synthesized C-ZIF-8 particle, highlighting the edge length (f). Scale bar: 500 nm. (b) Left: Representative FE-SEM image of C-ZIF-8 particles. Scale bar: 1 μm. Middle: Size-distribution histogram of as-synthesized C-ZIF-8 particles with a mean f of 191 ± 9 nm. Right: PXRD patterns of simulated (black) and as-synthesized C-ZIF-8 particles (red). -- Figure S2. (a) Scheme and FESEM image of an as-synthesized TRD-ZIF-8 particle, highlighting the particle size (f) and edge length (x). Scale bar: 500 nm. (b-e) TRD ZIF-8 particles (t= 0.68) with a mean f of 181 ± 9 nm (b), 198 ± 10 nm (c), 229 ± 9 nm (d) and 247 ± 10 nm (e). Left: Representative FE-SEM images; Middle: Size-distribution histograms; and Right: PXRD patterns of simulated (black) and assynthesized TRD-ZIF-8 particles (red). -- Figure S3. (a) Scheme and FESEM image of an as-synthesized RD-ZIF-8 particle, highlighting the particle size (f). Scale bar: 500 nm. (b-e) RD ZIF-8 particles with a mean f of 246 ± 12 nm (b), 267 ±12 nm (c), and 293 ± 13 nm (d). Left: Representative FE-SEM images; Middle: Size-distribution histograms; and Right: PXRD patterns of simulated (black) and as-synthesized RD-ZIF-8 particles (red). -- Figure S4. (a) Scheme and FESEM image of an as-synthesized O-UiO-66 particle, highlighting the edge length of particles (f). Scale bar: 500 nm. O-UiO-66 particles a mean f of 194 ± 12 nm (b), 238 ± 13 nm (c), and 247 ± 13 nm (d). Left: Representative FE-SEM images; Middle: Size-distribution histograms; and Right: PXRD patterns of simulated (black) and as-synthesized RD-ZIF-8 particles (red). -- Figure S5. Representative FESEM images of polydisperse C-ZIF-8 (a) and O-UiO-66 (b) supraparticles prepared by shaking emulsifying, with a size of 21 ± 5.6 μm (26% polydispersity) and 9.9 ± 3.4 μm (34% polydispersity, approximately 500 counts), respectively. -- Figure S6. Representative FESEM images of monodispersed RD-ZIF-8 (a) and TRD-ZIF-8 (b) supraparticles prepared using a droplet-based microfluidic device, with a size of 20.1 ± 0.6 μm (3% polydispersity) and 10.4 ± 0.5 μm (5% polydispersity, approximately 200 counts), respectively. -- Figure S7. Transmissive X-ray image of MOF supraparticles of a) RD-ZIF-8, showing few onion-like layers near the surface; b) TRD-ZIF-8, showing thick onion-like layers, as well as some lattice fringes; c) C-ZIF-8, showing thick onion-like layers, as well as some lattice fringes; and d) O-UiO-66 particles, showing only little onion-like layer structures. -- Figure S8. Cross-section of RD-ZIF-8 supraparticles revealed by focused-ion beam milling. -- Figure S9. Cross-section of TRD-ZIF-8 supraparticles revealed by focused-ion beam milling. -- Figure S10. Cross-section of C-ZIF-8 supraparticles revealed by focused-ion beam milling. -- Figure S11. Cross-section of O-UiO-66 supraparticles revealed by focused-ion beam milling. -- Figure S12. A TRD-ZIF-8 supraparticle exhibiting local five-fold symmetric surface pattern, marked with blue colour. -- Figure S13. Cross-sectional images of simulated supraparticles of hard polyhedra in spherical confinement. -- Figure S14. Photograph of the self-assembled superstructures resulting from the centrifugation of different aqueous colloidal MOF particles (from left to right: RD-ZIF-8, TRD-ZIF-8, C-ZIF-8 and OUiO-66). -- Figure S15. Relationship between MOF particle size of different shapes and layer distance. -- Figure S16. Optical setup to measure reflectance spectra directly from MOF supraparticles suspended in liquid in a glass vial. -- Figure S17. Angle-dependent reflection spectra of four types of MOF supraparticles measured directly from liquid suspension. -- Figure S18. Shift of the reflectance peak with increasing viewing angle for four types of MOF supraparticles. -- Figure S19. Buckled RD-ZIF-8 supraparticles. 1.0 mL 1 wt% Lutensol TO8 surfactant is added to 0.5 mL 2 wt% RD-ZIF-8 particle dispersion. -- Figure S20. Angle-dependent reflection spectra of buckled MOF supraparticles measured directly from suspension. -- Figure S21. Hypothesized surface grating effects of MOF supraparticles. -- Figure S22. Buckled RD-ZIF-8 supraparticles exhibit ordered surface features, visualized in scanning electron microscopy. -- Figure S23. The surface packing of RD ZIF-8 supraparticles shows a sawtooth groove profile, as seen in scanning electron microscopy.
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