Phase-Controlled Synthesis of Pd-Se Nanocrystals for Phase-Dependent Oxygen Reduction Catalysis

Zhiyong Yu; Shulin Xu; Yonggang Feng; Chengyong Yang; Qing Yao; Qi Shao; Ya-Fei Li; Xiaoqing Huang

doi:10.1021/acs.nanolett.1c00147

Phase-Controlled Synthesis of Pd-Se Nanocrystals for Phase-Dependent Oxygen Reduction Catalysis

Nano Lett. 2021 May 12;21(9):3805-3812. doi: 10.1021/acs.nanolett.1c00147. Epub 2021 Apr 20.

Authors

Zhiyong Yu¹, Shulin Xu², Yonggang Feng¹, Chengyong Yang¹, Qing Yao¹, Qi Shao¹, Ya-Fei Li², Xiaoqing Huang³

Affiliations

¹ College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu 215123, China.
² School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China.
³ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.

PMID: 33878871
DOI: 10.1021/acs.nanolett.1c00147

Abstract

Searching for highly efficient oxygen reduction reaction (ORR) electrocatalysts for fuel cell technology, in which the crystal structure plays a powerful role in regulating the electrocatalysis, is urgent yet challenging. Herein, we have explored the active and stable Pd-Se alloy electrocatalysts with controlled phase toward alkaline ORR. The phase-controlled Pd-Se nanoparticles (NPs) show interesting phase-dependent electrocatalytic performance, in which the Pd₁₇Se₁₅ NPs/C exhibits much better ORR performance than its counterpart, Pd₇Se₄ NPs/C, and the commercial Pd/C and Pt/C. Based on the detailed analysis, Pd in Pd₁₇Se₁₅ possesses more Se atom coordination and a higher valence state, thus providing a stronger capacity for the absorption of oxygenated species. DFT further reveals more charge transfer from the Pd₁₇Se₁₅ surface to the *OOH intermediate, which is the reason for the activity enhancement.

Keywords: Chalcogenide; Oxygen Reduction Reaction; Palladium; Phase; Selenium.