In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis

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 oxidatio...

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Main Authors: Zhang, Junming, Xu, Weichang, Liu, Yuan, Hung, Sung-Fu, Liu, Wei, Lam, Zhenhui, Tao, Hua Bing, Yang, Hongbin, Cai, Weizheng, Xiao, Hai, Chen, Hongyu, Liu, Bin
Other Authors: School of Chemical and Biomedical Engineering
Format: Journal Article
Language:English
Published: 2022
Subjects:
Online Access:https://hdl.handle.net/10356/160329
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author Zhang, Junming
Xu, Weichang
Liu, Yuan
Hung, Sung-Fu
Liu, Wei
Lam, Zhenhui
Tao, Hua Bing
Yang, Hongbin
Cai, Weizheng
Xiao, Hai
Chen, Hongyu
Liu, Bin
author2 School of Chemical and Biomedical Engineering
author_facet School of Chemical and Biomedical Engineering
Zhang, Junming
Xu, Weichang
Liu, Yuan
Hung, Sung-Fu
Liu, Wei
Lam, Zhenhui
Tao, Hua Bing
Yang, Hongbin
Cai, Weizheng
Xiao, Hai
Chen, Hongyu
Liu, Bin
author_sort Zhang, Junming
collection NTU
description 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.
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spelling ntu-10356/1603292023-12-12T08:24:31Z In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis Zhang, Junming Xu, Weichang Liu, Yuan Hung, Sung-Fu Liu, Wei Lam, Zhenhui Tao, Hua Bing Yang, Hongbin Cai, Weizheng Xiao, Hai Chen, Hongyu Liu, Bin School of Chemical and Biomedical Engineering School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) Nanyang Environment and Water Research Institute Engineering::Chemical engineering Bimetallic Surface Electronic Effect 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). 2022-07-19T06:36:23Z 2022-07-19T06:36:23Z 2021 Journal Article Zhang, J., Xu, W., Liu, Y., Hung, S., Liu, W., Lam, Z., Tao, H. B., Yang, H., Cai, W., Xiao, H., Chen, H. & Liu, B. (2021). In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis. Nano Letters, 21(18), 7753-7760. https://dx.doi.org/10.1021/acs.nanolett.1c02705 1530-6984 https://hdl.handle.net/10356/160329 10.1021/acs.nanolett.1c02705 34516143 2-s2.0-85116120402 18 21 7753 7760 en RG4/20 MOET2EP10120-0002 A20E5c0080 Nano Letters © 2021 American Chemical Society. All rights reserved.
spellingShingle Engineering::Chemical engineering
Bimetallic Surface
Electronic Effect
Zhang, Junming
Xu, Weichang
Liu, Yuan
Hung, Sung-Fu
Liu, Wei
Lam, Zhenhui
Tao, Hua Bing
Yang, Hongbin
Cai, Weizheng
Xiao, Hai
Chen, Hongyu
Liu, Bin
In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis
title In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis
title_full In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis
title_fullStr In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis
title_full_unstemmed In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis
title_short In situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis
title_sort in situ precise tuning of bimetallic electronic effect for boosting oxygen reduction catalysis
topic Engineering::Chemical engineering
Bimetallic Surface
Electronic Effect
url https://hdl.handle.net/10356/160329
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