Dataset of the manuscript: Open the Pores: Particles with Fully Accessible Hierarchical Pore Networks by Controlling Phase Separation in Confinement

This data publication is based on the metadata and datasets underlying the manuscript: Open the Pores: Particles with Fully Accessible Hierarchical Pore Networks by Controlling Phase Separation in Confinement Abstract: Hierarchical porous materials combine large surface area with efficient mass transport, in particular when macropores directly connect mesopores. Polymerization-induced spinodal decomposition of polyethylene glycol and tetraethyl orthosilicate can produce such macro-mesoporous material in bulk. However, the confinement of the spinodal decomposition to emulsion droplets typically produces porous particles with a dense silica shell that blocks pore accessibility. Here, we address this issue by controlling the interfacial energies of the two phases undergoing spinodal decomposition within the emulsion droplet. We use surfactant mixtures to induce neutral wetting to prevent shell formation and generate particles with fully open, accessible and interconnected pore systems. Lattice Boltzmann simulations corroborate the experimental findings and underline that neutral wetting conditions with a contact angle to the continuous phase of ~90° for both phases are essential to provide open surface pores. Our work provides a simple strategy for producing hierarchical porous particles with controlled surface and bulk porosity between ~200 and ~6000 nm, expanding their potential for applications in catalysis, separation technologies, and adsorption. Author Contributions: U.S. designed and realized all the experiments, synthesized all the materials, performed characterization, analysis, interpretation, wrote the original draft, reviewed, and edited the final manuscript. A.G. and A.K. performed tomographic characterization, reviewed, and edited the final manuscript. N.S. performed synthesis, reviewed, and edited the final manuscript. L.S. and C.S. performed textural characterization, reviewed and edited the final manuscript. J.B. and P.M. performed the lattice Boltzmann simulations, reviewed, and edited the final manuscript. B.A.Z, M.T., J.H., E.S., and N.V. acquired the funding, reviewed, and edited the final manuscript. U.S. and N.V. conceptualized and supervised all the research work. All authors contributed to the discussion and analysis of the results presented. The data is organized according to the figures presented in the manuscript. Folder '"Figure 1" contains: Photograph of porous silica monolith. SEM images of porous silica monolith and porous particle with dense silica shell. Vector file with chemical structure of TEOS and PEG. Folder "Figure 2" contains: High and Low magnification SEM images of porous particles formed using surfactant ratios S2/S1 of 0, 0.5, 1, and 1.9. Vector file with chemical structure of surfactants S1 and S2. Folder '"Figure 3" contains: Cross-sections of the simulated spinodal decomposition in spherical confinement for an interfacial contact angle of blue phase of 70°, 90°, 110°, and 180°. Surface renderings of the simulated particle with a removed red phase for an interfacial contact angle of blue phase of 70°, 90°, 110°, and 180°. Interfacial fraction of blue and red phase as a function of their interfacial contact angle. Folder '"Figure 4" contains: 3D X-ray nano-computed tomography reconstruction video of porous particles formed using surfactant ratios S2/S1 of 0 and 1. Pore size distribution via mercury intrusion porosimetry and Ar physisorption of porous particles formed using surfactant ratios S2/S1 of 0 and 1. Folder "Figure 5" contains: SEM images of porous particles formed using TEOS/PEG ratios of 0.62, 0.66, and 0.70. 3D electron tomography reconstruction video of macropore wall of a porous particle. Mesopore size distributions via N2 physisorption of particles with varying no basic treatment and with basic treatment temperatures of 30, 50, 70, and 90 °C. Pore size distribution via mercury intrusion porosimetry and Ar physisorption of porous particles formed using TEOS/PEG ratios of 0.62, 0.66, and 0.70. Folder '"Figure S1" contains: SEM images of porous particles formed using surfactant ratios S2/S1 of 0, 0.2, 0.5, 0.9, 1, 1.5, 1.9 and 3.7. Folder '"Figure S2" contains: SEM images of porous particles formed with surfactant ratios S2/S1 of 0 and 1, using recycled perfluorinated oil. Folder "Figure S3" contains: Cross-sections of the simulated spinodal decomposition in spherical confinement for an interfacial contact angle of blue phase of 0°, 30°, 50°, 70°, 90°, 100°, 110°, 130°, 150°, and 180°. Surface renderings of the simulated particle with a removed red phase for an interfacial contact angle of blue phase of 0°, 30°, 50°, 70°, 90°, 100°, 110°, 130°, 150°, and 180°. Additional data and info on the reproduction of lattice Boltzmann simulations. Folder '"Figure S4" contains: Cumulative pore volume curves via mercury intrusion porosimetry and Ar physisorption of porous particles formed using only surfactant S1 (S2/S1=0) and mixture of S1 and S2 (S2/S1=1). Hg intrusion-extrusion curves of porous particles formed using only surfactant S1 (S2/S1=0) and mixture of S1 and S2 (S2/S1=1). Ar physisorption isotherms of porous particles formed using only surfactant S1 (S2/S1=0) and mixture of S1 and S2 (S2/S1=1). Folder '"Figure S5" contains: Pore size distribution and porosity via nano-computed tomography analysis of porous particles formed using only surfactant S1 (S2/S1=0) and mixture of S1 and S2 (S2/S1=1). Folder '"Figure S6" contains: SEM images of porous particles formed using TEOS/PEG ratios of 0.62, 0.66, and 0.70. Cumulative pore volume curves via mercury intrusion porosimetry and Ar physisorption of porous particles formed using TEOS/PEG ratios of 0.62, 0.66, and 0.70. Hg intrusion-extrusion curves of porous particles formed using TEOS/PEG ratios of 0.62, 0.66, and 0.70. Ar physisorption isotherms of porous particles formed using TEOS/PEG ratios of 0.62, 0.66, and 0.70. Folder '"Figure S7" contains: SEM image of a porous particles formed using surfactant ratio S2/S1 of 1. 3D electron tomography reconstruction video of macropore wall of a porous particle. Folder '"Figure S8" contains: SEM images of porous particles produced using membrane emulsification with membranes of pore diameter 5, 10 and 20 µm. Size distributions of porous particles produced using membrane emulsification with membranes of pore diameter 5, 10 and 20 µm, and vortex emulsification. Folder '"Figure S9" contains: SEM images of a porous particle being prepared for electron tomography analysis by first glueing on the tip of a needle, then stepwise removal of material using FIB, and finally a thin pillar of macropore wall is prepared. Cross-section from nano-computed tomography segmentation analysis of a porous particle.