10.1021/acs.chemmater.8b00109.s001 Maria Castro Maria Castro Pit Losch Pit Losch Woojin Park Woojin Park Mohamed Haouas Mohamed Haouas Francis Taulelle Francis Taulelle Claudia Loerbroks Claudia Loerbroks Gert Brabants Gert Brabants Eric Breynaert Eric Breynaert Christine E. A. Kirschhock Christine E. A. Kirschhock Ryong Ryoo Ryong Ryoo Wolfgang Schmidt Wolfgang Schmidt Unraveling Direct Formation of Hierarchical Zeolite Beta by Dynamic Light Scattering, Small Angle X‑ray Scattering, and Liquid and Solid-State NMR: Insights at the Supramolecular Level American Chemical Society 2018 N 6 solution 1 H-DOSY NMR probe nano-Beta zeolite crystals Hierarchical Zeolite Beta formation mesopore diphe Dynamic Light Scattering spinodal decomposition-type segregation nm 2018-03-12 00:00:00 Journal contribution https://acs.figshare.com/articles/journal_contribution/Unraveling_Direct_Formation_of_Hierarchical_Zeolite_Beta_by_Dynamic_Light_Scattering_Small_Angle_X_ray_Scattering_and_Liquid_and_Solid-State_NMR_Insights_at_the_Supramolecular_Level/6116099 A case study on the understanding of the formation of hierarchical Beta zeolites using gemini-type piperidine based multiammonium surfactant (N<sub>6</sub>-diphe) is reported. Complementary techniques were used to investigate N<sub>6</sub>-diphe’s structure-directing effect at the molecular level. Combining characterization of the resulting zeolite materials with the toolboxes herein developed for studying clear solutions and dense gels discloses self-assembly processes that govern the growth (and growth inhibition) of nano-Beta zeolite crystals. In clear solution, small-angle X-ray scattering and liquid-state NMR provide insights about the formation of nanoparticles and their degree of order. <sup>14</sup>N and <sup>1</sup>H-DOSY NMR probe the dynamics and mobility of soluble species. In a dense gel, on the other side, <sup>27</sup>Al- and <sup>29</sup>Si-(MAS) NMR elucidate the varying local connectivity between initial nano-objects and the final solid products. It has been found that cylindrical micelles control the transformation of solubilized silica and alumina during the formation of zeolite nuclei and guide their crystal growth to nano-Beta rods with bimodal mesoporosity. The predominant smaller mesopores (6 to 8 nm) originate from the template’s hydrophobic alkyl chains, while larger mesopores (10 to 30 nm) are supposed to result from a spinodal decomposition-type segregation of phases consisting of as-formed hydrophobic zeolite rods and an aqueous solution.