1. In Situ Precise Tuning of Bimetallic Electronic Effect for Boosting Oxygen Reduction Catalysis
- Author
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Sung Fu Hung, Weichang Xu, Hua Bing Tao, Junming Zhang, Yuan Liu, Wei Liu, Hai Xiao, Bin Liu, Zhenhui Lam, Hongbin Yang, Hongyu Chen, Weizheng Cai, School of Chemical and Biomedical Engineering, School of Physical and Mathematical Sciences, Interdisciplinary Graduate School (IGS), and Nanyang Environment and Water Research Institute
- Subjects
Materials science ,Mechanical Engineering ,Fermi level ,Analytical chemistry ,Bioengineering ,General Chemistry ,Condensed Matter Physics ,Electronic Effect ,Catalysis ,Overlayer ,symbols.namesake ,Chemistry [Science] ,Monolayer ,Electronic effect ,symbols ,Reversible hydrogen electrode ,General Materials Science ,Reactivity (chemistry) ,Bimetallic Surface ,Bimetallic strip - Abstract
Tuning intermediate adsorption energy by shifting the d-band center offers a powerful strategy to tailor the reactivity of metal catalysts. Here we report a potential sweep method to grow Pd layer-by-layer on Au with the capability to in situ measure the surface structure through an ethanol oxidation reaction. Spectroscopic characterizations reveal charge-transfer induced valence band restructuring in the Pd overlayer, which shifts the d-band center away from the Fermi level compared to bulk Pd. Precise overlayer control gives the optimal bimetallic surface of two monolayers (ML) Pd on Au, which exhibits more than 370-fold mass activity enhancement in oxygen reduction reaction (at 0.9 V vs. reversible hydrogen electrode) and 40 mV increase in half-wave potential compared to the Pt/C. Tested in a homemade Zn-air battery, the 2-ML-Pd/Au/C exhibits a maximum power density of 296 mW/cm2 and specific activity of 804 mAh/gZn, much higher than Pt/C with the same catalyst loading amount. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) This work was supported by the fund from the Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1: RG4/20 and Tier 2: MOET2EP10120-0002, and Agency for Science, Technology, and Research (A*Star IRG: A20E5c0080).
- Published
- 2021