Real-Time Monitoring of Surface Effects on the Oxygen Reduction Reaction Mechanism for Aprotic Na-O2Batteries

Jing Zhang; Xia Guang Zhang; Jin Chao Dong; Petar M. Radjenovic; David James Young; Jian Lin Yao; Ya Xian Yuan; Zhong Qun Tian; Jian Feng Li

doi:10.1021/jacs.1c10009

Real-Time Monitoring of Surface Effects on the Oxygen Reduction Reaction Mechanism for Aprotic Na-O₂Batteries

Jing Zhang, Xia Guang Zhang, Jin Chao Dong, Petar M. Radjenovic, David James Young, Jian Lin Yao, Ya Xian Yuan, Zhong Qun Tian, Jian Feng Li

CDU College of Engineering, IT and Environment

Research output: Contribution to journal › Article › peer-review

Abstract

Discharging of aprotic sodium-oxygen (Na-O2) batteries is driven by the cathodic oxygen reduction reaction in the presence of sodium cations (Na+-ORR). However, the mechanism of aprotic Na+-ORR remains ambiguous and is system dependent. In-situ electrochemical Raman spectroscopy has been employed to study the aprotic Na+-ORR processes at three atomically ordered Au(hkl) single-crystal surfaces for the first time, and the structure-intermediates/mechanism relationship has been identified at a molecular level. Direct spectroscopic evidence of superoxide on Au(110) and peroxide on Au(100) and Au(111) as intermediates/products has been obtained. Combining these experimental results with theoretical simulation has revealed that the surface effect of Au(hkl) electrodes on aprotic Na+-ORR activity is mainly caused by the different adsorption of Na+ and O2. This work enhances our understanding of aprotic Na+-ORR on Au(hkl) surfaces and provides further guidance for the design of improved Na-O2 batteries.

Original language	English
Pages (from-to)	20049-20054
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	143
Issue number	48
DOIs	https://doi.org/10.1021/jacs.1c10009
Publication status	Published - 8 Dec 2021

Access to Document

10.1021/jacs.1c10009

Cite this

@article{ed1a49ce03e1483988a751defcc6222a,

title = "Real-Time Monitoring of Surface Effects on the Oxygen Reduction Reaction Mechanism for Aprotic Na-O2Batteries",

abstract = "Discharging of aprotic sodium-oxygen (Na-O2) batteries is driven by the cathodic oxygen reduction reaction in the presence of sodium cations (Na+-ORR). However, the mechanism of aprotic Na+-ORR remains ambiguous and is system dependent. In-situ electrochemical Raman spectroscopy has been employed to study the aprotic Na+-ORR processes at three atomically ordered Au(hkl) single-crystal surfaces for the first time, and the structure-intermediates/mechanism relationship has been identified at a molecular level. Direct spectroscopic evidence of superoxide on Au(110) and peroxide on Au(100) and Au(111) as intermediates/products has been obtained. Combining these experimental results with theoretical simulation has revealed that the surface effect of Au(hkl) electrodes on aprotic Na+-ORR activity is mainly caused by the different adsorption of Na+ and O2. This work enhances our understanding of aprotic Na+-ORR on Au(hkl) surfaces and provides further guidance for the design of improved Na-O2 batteries.",

author = "Jing Zhang and Zhang, {Xia Guang} and Dong, {Jin Chao} and Radjenovic, {Petar M.} and Young, {David James} and Yao, {Jian Lin} and Yuan, {Ya Xian} and Tian, {Zhong Qun} and Li, {Jian Feng}",

note = "Funding Information: The authors acknowledge the financial support of this research from NSFC (21925404, 22002128, 21802111, 22021001, 21773166, and 21673152), the National Key Research and Development Program of China (2020YFB1505800 and 2019YFA0705400), and the “111” Project (B17027). Publisher Copyright: {\textcopyright} 2021 American Chemical Society. All rights reserved. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.",

year = "2021",

month = dec,

day = "8",

doi = "10.1021/jacs.1c10009",

language = "English",

volume = "143",

pages = "20049--20054",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "48",

}

TY - JOUR

T1 - Real-Time Monitoring of Surface Effects on the Oxygen Reduction Reaction Mechanism for Aprotic Na-O2Batteries

AU - Zhang, Jing

AU - Zhang, Xia Guang

AU - Dong, Jin Chao

AU - Radjenovic, Petar M.

AU - Young, David James

AU - Yao, Jian Lin

AU - Yuan, Ya Xian

AU - Tian, Zhong Qun

AU - Li, Jian Feng

N1 - Funding Information: The authors acknowledge the financial support of this research from NSFC (21925404, 22002128, 21802111, 22021001, 21773166, and 21673152), the National Key Research and Development Program of China (2020YFB1505800 and 2019YFA0705400), and the “111” Project (B17027). Publisher Copyright: © 2021 American Chemical Society. All rights reserved. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.

PY - 2021/12/8

Y1 - 2021/12/8

N2 - Discharging of aprotic sodium-oxygen (Na-O2) batteries is driven by the cathodic oxygen reduction reaction in the presence of sodium cations (Na+-ORR). However, the mechanism of aprotic Na+-ORR remains ambiguous and is system dependent. In-situ electrochemical Raman spectroscopy has been employed to study the aprotic Na+-ORR processes at three atomically ordered Au(hkl) single-crystal surfaces for the first time, and the structure-intermediates/mechanism relationship has been identified at a molecular level. Direct spectroscopic evidence of superoxide on Au(110) and peroxide on Au(100) and Au(111) as intermediates/products has been obtained. Combining these experimental results with theoretical simulation has revealed that the surface effect of Au(hkl) electrodes on aprotic Na+-ORR activity is mainly caused by the different adsorption of Na+ and O2. This work enhances our understanding of aprotic Na+-ORR on Au(hkl) surfaces and provides further guidance for the design of improved Na-O2 batteries.

AB - Discharging of aprotic sodium-oxygen (Na-O2) batteries is driven by the cathodic oxygen reduction reaction in the presence of sodium cations (Na+-ORR). However, the mechanism of aprotic Na+-ORR remains ambiguous and is system dependent. In-situ electrochemical Raman spectroscopy has been employed to study the aprotic Na+-ORR processes at three atomically ordered Au(hkl) single-crystal surfaces for the first time, and the structure-intermediates/mechanism relationship has been identified at a molecular level. Direct spectroscopic evidence of superoxide on Au(110) and peroxide on Au(100) and Au(111) as intermediates/products has been obtained. Combining these experimental results with theoretical simulation has revealed that the surface effect of Au(hkl) electrodes on aprotic Na+-ORR activity is mainly caused by the different adsorption of Na+ and O2. This work enhances our understanding of aprotic Na+-ORR on Au(hkl) surfaces and provides further guidance for the design of improved Na-O2 batteries.

UR - http://www.scopus.com/inward/record.url?scp=85120349523&partnerID=8YFLogxK

U2 - 10.1021/jacs.1c10009

DO - 10.1021/jacs.1c10009

M3 - Article

C2 - 34812610

AN - SCOPUS:85120349523

VL - 143

SP - 20049

EP - 20054

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 48

ER -

Real-Time Monitoring of Surface Effects on the Oxygen Reduction Reaction Mechanism for Aprotic Na-O₂Batteries

Abstract

Access to Document

Other files and links

Fingerprint

Cite this