Slowly Removing Surface Ligand by Aging Enhances the Stability of Pd Nanosheets toward Electron Beam Irradiation and Electrocatalysis

Yu Zhang; Shaobo Han; Shangqian Zhu; Ruhui Chen; Tiehuai Li; Zhiheng Lyu; Ming Zhao; Meng Gu; Minhua Shao; Younan Xia

doi:10.1002/anie.202314634

Slowly Removing Surface Ligand by Aging Enhances the Stability of Pd Nanosheets toward Electron Beam Irradiation and Electrocatalysis

Angew Chem Int Ed Engl. 2023 Dec 21;62(52):e202314634. doi: 10.1002/anie.202314634. Epub 2023 Nov 23.

Authors

Yu Zhang^{1

2

3}, Shaobo Han⁴, Shangqian Zhu², Ruhui Chen⁵, Tiehuai Li², Zhiheng Lyu⁵, Ming Zhao⁵, Meng Gu⁴, Minhua Shao², Younan Xia^{1

5}

Affiliations

¹ The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology, Emory University, 30332, Atlanta, GA, USA.
² Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.
³ School of Mechanical and Power Engineering, East China University of Science and Technology, 130 Meilong Road, 200237, Shanghai, China.
⁴ Department of Materials Science and Engineering, Southern University of Science and Technology, 518055, Shenzhen, P. R. China.
⁵ School of Chemistry and Biochemistry, Georgia Institute of Technology, 30332, Atlanta, GA, USA.

PMID: 37955915
DOI: 10.1002/anie.202314634

Abstract

Surface ligands play an important role in shape-controlled growth and stabilization of colloidal nanocrystals. Their quick removal tends to cause structural deformation and/or aggregation to the nanocrystals. Herein, we demonstrate that the surface ligand based on poly(vinylpyrrolidone) (PVP) can be slowly removed from Pd nanosheets (NSs, 0.93±0.17 nm in thickness) by simply aging the colloidal suspension. The aged Pd NSs show well-preserved morphology, together with significantly enhanced stability toward both e-beam irradiation and electrocatalysis (e.g., ethanol oxidation). It is revealed that the slow desorption of PVP during aging forces the re-exposed Pd atoms to reorganize, facilitating the surface to transform from being nearly perfect to defect-rich. The resultant Pd NSs with abundant defects no longer rely on surface ligand to stabilize the atomic arrangement and thus show excellent structural and electrochemical stability. This work provides a facile and effective method to maintain the integrity of colloidal nanocrystals by slowly removing the surface ligand.

Keywords: Catalysis; Pd Nanosheets; Stability; Surface Ligand; Surface Reconstruction.

Abstract

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