The invention provides methods for completely removing aluminum from existing zeolite frameworks that have been previously considered unalterable due to their small pore sizes and stable crystal structures. Consequently, new combinations of metal atoms and zeolite structures can now be made using the methods disclosed herein. Metal atoms that have useful properties for catalysis and adsorption have been integrated into zeolite structures that provide advantageous size selection or solvation properties to increase rates, conversions, and yields of catalytic processes. The disclosed catalysts and methods reduce the cost of synthesizing useful materials and zeolite structures with compositions of matter that have not been reported.
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