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Volume 4, Issue 2, Pages 359-371 (February 2018)
Coupled s-p-d Exchange in Facet-Controlled Pd3Pb Tripods Enhances Oxygen Reduction Catalysis Lingzheng Bu, Qi Shao, Yecan Pi, Jianlin Yao, Mingchuan Luo, Jianping Lang, Sooyeon Hwang, Huolin Xin, Bolong Huang, Jun Guo, Dong Su, Shaojun Guo, Xiaoqing Huang Chem Volume 4, Issue 2, Pages (February 2018) DOI: /j.chempr Copyright © 2018 Elsevier Inc. Terms and Conditions
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Chem 2018 4, DOI: ( /j.chempr ) Copyright © 2018 Elsevier Inc. Terms and Conditions
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Figure 1 Morphological and Structural Characterizations of Pd-Pb TPs
TEM image (A), PXRD pattern (B), STEM-EELS elemental mappings (C), reconstructed 3D tomograms along the [110] zone axis (D), atomic model along the [110] zone axis (E), 3D illustration along the 〈100〉 zone axis (F), and cross-sectional reconstructed planes and corresponding atomic models of the 〈100〉 fork (G and I) and the 〈111〉 fork (H and J) of Pd3Pb TPs. See also Figures S1–S9 and Movies S1 and S2. Chem 2018 4, DOI: ( /j.chempr ) Copyright © 2018 Elsevier Inc. Terms and Conditions
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Figure 2 Atomic Structure of Pd-Pb TPs
(A–C, E–G, and I–K) Low-magnification HAADF-STEM and TEM images (A, E, and I), the corresponding atomic models (B, F, and J), and high-resolution HAADF-STEM images (C, G, and K) of Pd3Pb TP along the 〈100〉, 〈110〉, and 〈112〉 zone axes. (D, H, and L) The enlarged HAADF-STEM images of selected areas in (C), (G), and (K), respectively. Predominant facets of {100} and {110} planes are marked. See also Figures S10–S13. Chem 2018 4, DOI: ( /j.chempr ) Copyright © 2018 Elsevier Inc. Terms and Conditions
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Figure 3 ORR Performance of Ordered Pd-Pb TPs/C, Pd-Pb NPs/C, Pt/C, and Pd/C (A–C) CO stripping curves (A), ORR polarization curves (B), and histogram of mass and specific activities (C) of different electrocatalysts. Error bars in (C) represent the activity standard deviations calculated on the basis of five parallel measurements after Ohmic drop correction. (D) ORR polarization curves of Pd3Pb TPs/C before and after various potential cycles. (E) The normalized mass activity changes of Pd3Pb TPs/C, Pd3Pb NPs/C, Pt/C, and Pd/C before and after various potential cycles. The current densities in (B) and (D) were normalized to the geometric area of the rotating disk electrode (0.196 cm2). See also Figures S14–S23 and S28 and Tables S1–S3. Chem 2018 4, DOI: ( /j.chempr ) Copyright © 2018 Elsevier Inc. Terms and Conditions
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Figure 4 DFT Calculation the s-p-d Exchange Effect
(A) The Gibbs energy profiles ΔG of ORR on Pd3Pb (110); TS represents transition states. Asterisks denote a molecule absorbed on the specific site of the surface. (B) Combined projected DOS of Pd-metal, Pd3Pb bulk, and Pd3Pb (110) surface. (C) Top and side views of both HOMO and LUMO orbital configurations on the Pd3Pb (100) surface, where the lattice is shown at different angles (Pd, dark green; Pb, gray). (D) Schematic diagram and equivalent atom (E.A.) model approached by the s-p-d exchange effect. See also Figures S24–S27. Chem 2018 4, DOI: ( /j.chempr ) Copyright © 2018 Elsevier Inc. Terms and Conditions
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