Abstract
We report H2 adsorption capacities reaching 0.05 wt % at 303 K and at 1 atm H2 pressure on solid-state CuCl-exchanged [Al]-SSZ-13 and [B]-SSZ-13 zeolites. Differential heat of H2 adsorption is found in the range between 16 and 48 kJ mol H2–1 on Cu(I)-SSZ-13 at 323 K and isosteric heat of adsorption is found between 20 and 55 kJ mol H2–1 on Cu(I)-[B]-SSZ-13 at temperatures between 293 and 323 K. Strong interactions between H2 and the copper cations in Cu(I)-SSZ-13 are evidenced using Rietveld refinements of neutron powder diffraction patterns revealing Cu–deuterium (D2) distances of 2.3(2) and 2.41(1) A. A temperature-dependent Cu(I) migration—away from the six-membered ring (6MR) and eight-membered ring (8MR)—is related to the high adsorption capacities of the samples at 303 K. At 10 K, access to Cu(I) at 6MR is sterically hindered by framework oxygen atoms (Cu–Oframework distance of 2.196(5) A), rationalizing the low H2 adsorption capacities of Cu(I)-SSZ-13 samples as compared to Na-SSZ-13 at 77 K.
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