Lattice Engineering to Simultaneously Control the Defect/Stacking Structures of Layered Double Hydroxide Nanosheets to Optimize Their Energy Functionalities

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.0c09217.

• Ionic radii and hydration shell radii of various anions (Table S1). EDS–elemental maps (Figure S1). FE-SEM images (Figure S2). Results of fitted Co K-edge EXAFS spectra (Table S2). Chemical compositions and oxygen vacancy contents (Table S3). Co 2p_3/2 XPS data (Figure S3). Relative concentration of Co²⁺/Co³⁺ (Table S4). AFM images (Figure S4). Powder XRD data of restacked Co–Al-LDH NSs synthesized with the pH change, cation change, and temperature change (Figure S5). Stacking structures for restacked Co–Al-LDH NSs synthesized with the pH change, cation change, and temperature change (Table S5). FTs of Co K-edge EXAFS of Co–Al-LDH–NO₃^– synthesized with the pH change, cation change, and temperature change (Figure S6). Results of fitted Co K-edge EXAFS spectra of Co–Al-LDH–NO₃^– synthesized with the pH change, cation change, and temperature change (Table S6). Powder XRD, N₂ adsorption–desorption isotherm, EPR, and FTs of Co K-edge EXAFS data of ion-exchanged Co–Al-LDH materials (Figure S7). Stacking structures, pore structures, and results of fitted Co K-edge EXAFS spectra for ion-exchanged Co–Al-LDH materials (Table S7). EPR and FTs of Co K-edge EXAFS data of bulk Co–Al-LDH, the exfoliated Co–Al-LDH NS, and restacked Co–Al-LDH NSs (Figure S8). Results of fitted Co K-edge EXAFS spectra for bulk Co–Al-LDH and the exfoliated Co–Al-LDH NS (Table S8). Powder XRD, N₂ adsorption–desorption isotherm, EPR, and FTs of Co K-edge EXAFS data of Co–Al-LDH–DS^– and Co–Al-LDH–NO₃^– (Figure S9). Stacking structures, pore structures, and results of fitted Co K-edge EXAFS spectra for Co–Al-LDH–DS^– and Co–Al-LDH–NO₃^– (Table S9). EPR spectra of Co–Al-LDH–CO₃^2– and Co–Al-LDH–NO₃^– (Figure S10). Lattice strains (Figure S11). LSV curves and stability tests of Co–Al-LDH–NO₃^– with/without Cl^– (Figure S12). Powder XRD and EPR of restacked Ni–Fe-LDH NSs (Figure S13). Stacking structures for restacked Ni–Fe-LDH NSs (Table S10). Powder XRD data of Co–Al-LDH–NO₃^– after OER stability test (Figure S14). Specific capacitances of carbon-free LDH-based electrodes (Table S11). Fractions of the capacitive and diffusion-controlled contributions at various scan rates (Figure S15). Electrocatalyst/electrode functionalities of the carbonate-restacked Co–Al-LDH–CO₃^2– (Figure S16). Correlation plots of overpotentials as several functions (Figure S17). Correlation plots of specific capacitances as several functions (Figure S18). DOS analyses (Figure S19). Defect formation energies (Figure S20). DFT-optimized structures (Figure S21). DFT-optimized lattice parameters of model-1 LDH and model-2 LDH (Table S12) (PDF)