Synergistic Fe−Se Atom Pairs as Bifunctional Oxygen Electrocatalysts Boost Low‐Temperature Rechargeable Zn‐Air Battery

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Abstract

Herein, we successfully construct bifunctional electrocatalysts by synthesizing atomically dispersed Fe−Se atom pairs supported on N‐doped carbon (Fe−Se/NC). The obtained Fe−Se/NC shows a noteworthy bifunctional oxygen catalytic performance with a low potential difference of 0.698 V, far superior to that of reported Fe‐based single‐atom catalysts. The theoretical calculations reveal that p‐d orbital hybridization around the Fe−Se atom pairs leads to remarkably asymmetrical polarized charge distributions. Fe−Se/NC based solid‐state rechargeable Zn‐air batteries (ZABs−Fe−Se/NC) present stable charge/discharge of 200 h (1090 cycles) at 20 mA cm ⁻² at 25 °C, which is 6.9 times of ZABs−Pt/C+Ir/C. At extremely low temperature of −40 °C, ZABs−Fe−Se/NC displays an ultra‐robust cycling performance of 741 h (4041 cycles) at 1 mA cm ⁻², which is about 11.7 times of ZABs−Pt/C+Ir/C. More importantly, ZABs−Fe−Se/NC could be operated for 133 h (725 cycles) even at 5 mA cm ⁻² at −40 °C.

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Engineering unsymmetrically coordinated Cu-S 1 N 3 single atom sites with enhanced oxygen reduction activity

Huishan Shang, Xiangyi Zhou, Juncai Dong … (2020)

Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts. Herein, a practical strategy was reported to rationally design single copper atoms coordinated with both sulfur and nitrogen atoms in metal-organic framework derived hierarchically porous carbon (S-Cu-ISA/SNC). The atomic interface configuration of the copper site in S-Cu-ISA/SNC is detected to be an unsymmetrically arranged Cu-S1N3 moiety. The catalyst exhibits excellent oxygen reduction reaction activity with a half-wave potential of 0.918 V vs. RHE. Additionally, through in situ X-ray absorption fine structure tests, we discover that the low-valent Cuprous-S1N3 moiety acts as an active center during the oxygen reduction process. Our discovery provides a universal scheme for the controllable synthesis and performance regulation of single metal atom catalysts toward energy applications.

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Author and article information

Contributors

Dingsheng Wang: (View ORCID Profile)

Journal

Title: Angewandte Chemie International Edition

Abbreviated Title: Angew Chem Int Ed

Publisher: Wiley

ISSN (Print): 1433-7851

ISSN (Electronic): 1521-3773

Publication date Created: April 03 2023

Publication date (Electronic): March 03 2023

Publication date (Print): April 03 2023

Volume: 62

Issue: 15

Affiliations

[1 ] School of Chemical and Material Engineering Jiangnan University 214122 Wuxi Jiangsu China

[2 ] State Key Laboratory of Powder Metallurgy Central South University 410083 Changsha China

[3 ] Energy Materials Computing Center School of Energy and Mechanical Engineering Jiangxi University of Science and Technology 330013 Nanchang China

[4 ] Department of Chemistry Tsinghua University 100084 Beijing China

[5 ] College of Materials Science and Engineering Shenzhen University 518060 Shenzhen China

[6 ] State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and environment China University of Petroleum 102249 Beijing China

Article

DOI: 10.1002/anie.202219191

SO-VID: a9c1dd94-ce96-48ab-8e1b-f7bbfc72b812

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http://onlinelibrary.wiley.com/termsAndConditions#vor

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