Fig 1

(a) Procedures for the synthesis of Pd/Cu-MFI catalysts, (b) XRD patterns of Pd/Cu-MFI catalysts at different Pd loadings, (c) Nitrogen sorption isotherms and their pore size distributions (insert) of Cu-MFI and (1)Pd/Cu-MFI catalysts, (d) SEM, (e) EDS elemental mapping, (f) HAADF-STEM (insert: particle size distribution of Cu), and (g) AC-HAADF-STEM images of the (1)Pd/Cu-MFI catalyst (Pd single atoms are highlighted by red circles)."

Fig 2

(a) Pd K-edge XANES spectra (insert: enlarged signal) and (b) Fourier transform EXAFS spectra of Pd/Cu-MFI catalysts at different Pd loadings and Pd foil, (c) DRIFTS spectra of CO adsorption on the (1)Pd/Cu-MFI catalyst, and (d) The electronic structure of metals over the (1)Pd/Cu-MFI catalyst (the arrows indicate the electron transfer direction)."

Fig 3

XPS spectra of (a) Cu 2p, (b) Cu-LMM and (c) Pd 3d for Cu-MFI and Pd/Cu-MFI catalysts."

Fig 4

(a) Productivities and (b) Turnover frequencies (TOFs) of different catalysts (a: normalized by the weight of catalyst and mole of metals, with the contribution of Cu omitted when calculating the productivity of single Pd atoms; b: the method for calculating TOF is described in Section 1.4 of the Supporting Information), (c) Arrhenius plots of ethanol dehydrogenation over Cu-MFI and (1)Pd/Cu-MFI catalysts, and (d) Stability of the (1)Pd/Cu-MFI catalyst (reaction conditions: 2.26 kPa ethanol, 453 K, WHSV(weight hourly space velocity) = 0.55 h−1, N2: 40 mL∙min−1)."

Fig 5

(a) H2-TPR profiles, (b) H2-TPD profiles, (c) H2 static chemisorption isotherms at 323 K, and (d) H2 uptakes on Cu/MFI and (1)Pd/Cu-MFI catalysts."

Fig 6

DRIFT spectra of ethanol adsorption and desorption over (a) Cu-MFI and (b) (1)Pd/Cu-MFI catalysts at different temperatures, (c) Energy profiles for ethanol dehydrogenation on Cu (111) (blue) and single-atom Pd/Cu (100) (red) slabs, and (d) The proposed reaction process for ethanol dehydrogenation over Pd/Cu-MFI catalysts."