In Situ Precise Tuning of Bimetallic Electronic Effect for Boosting Oxygen Reduction Catalysis

Junming Zhang; Weichang Xu; Yuan Liu; Sung-Fu Hung; Wei Liu; Zhenhui Lam; Hua Bing Tao; Hongbin Yang; Weizheng Cai; Hai Xiao; Hongyu Chen; Bin Liu

doi:10.1021/acs.nanolett.1c02705

In Situ Precise Tuning of Bimetallic Electronic Effect for Boosting Oxygen Reduction Catalysis

Junming Zhang, Weichang Xu, Yuan Liu, Sung-Fu Hung, Wei Liu, Zhenhui Lam, Hua Bing Tao, Hongbin Yang, Weizheng Cai, Hai Xiao, Hongyu Chen^*, Bin Liu^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

38 Citations (Scopus)

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/g_Zn, much higher than Pt/C with the same catalyst loading amount. © 2021 American Chemical Society.

Original language	English
Pages (from-to)	7753-7760
Journal	Nano Letters
Volume	21
Issue number	18
Online published	13 Sept 2021
DOIs	https://doi.org/10.1021/acs.nanolett.1c02705
Publication status	Published - 22 Sept 2021
Externally published	Yes

Research Keywords

bimetallic surface
electronic effect
in situ
layer-by-layer growth
oxygen reduction reaction

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title = "In Situ Precise Tuning of Bimetallic Electronic Effect for Boosting Oxygen Reduction Catalysis",

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. {\textcopyright} 2021 American Chemical Society.",

keywords = "bimetallic surface, electronic effect, in situ, layer-by-layer growth, oxygen reduction reaction",

author = "Junming Zhang and Weichang Xu and Yuan Liu and Sung-Fu Hung and Wei Liu and Zhenhui Lam and Tao, {Hua Bing} and Hongbin Yang and Weizheng Cai and Hai Xiao and Hongyu Chen and Bin Liu",

year = "2021",

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doi = "10.1021/acs.nanolett.1c02705",

language = "English",

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TY - JOUR

T1 - In Situ Precise Tuning of Bimetallic Electronic Effect for Boosting Oxygen Reduction Catalysis

AU - Zhang, Junming

AU - Xu, Weichang

AU - Liu, Yuan

AU - Hung, Sung-Fu

AU - Liu, Wei

AU - Lam, Zhenhui

AU - Tao, Hua Bing

AU - Yang, Hongbin

AU - Cai, Weizheng

AU - Xiao, Hai

AU - Chen, Hongyu

AU - Liu, Bin

PY - 2021/9/22

Y1 - 2021/9/22

N2 - 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. © 2021 American Chemical Society.

AB - 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. © 2021 American Chemical Society.

KW - bimetallic surface

KW - electronic effect

KW - in situ

KW - layer-by-layer growth

KW - oxygen reduction reaction

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U2 - 10.1021/acs.nanolett.1c02705

DO - 10.1021/acs.nanolett.1c02705

M3 - RGC 21 - Publication in refereed journal

C2 - 34516143

SN - 1530-6984

VL - 21

SP - 7753

EP - 7760

JO - Nano Letters

JF - Nano Letters

IS - 18

ER -

In Situ Precise Tuning of Bimetallic Electronic Effect for Boosting Oxygen Reduction Catalysis

Abstract

Research Keywords

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