Catalytic Oxidation of K2S via Atomic Co and Pyridinic N Synergy in Potassium-Sulfur Batteries

Chao Ye; Jieqiong Shan; Dongliang Chao; Pei Liang; Yan Jiao; Junnan Hao; Qinfen Gu; Kenneth Davey; Haihui Wang; Shi-Zhang Qiao

doi:10.1021/jacs.1c06255

Catalytic Oxidation of K₂S via Atomic Co and Pyridinic N Synergy in Potassium-Sulfur Batteries

Chao Ye
, Jieqiong Shan
, Dongliang Chao
, Pei Liang
, Yan Jiao
, Junnan Hao
, Qinfen Gu
, Kenneth Davey
, Haihui Wang^*
, Shi-Zhang Qiao^*

^*Corresponding author for this work

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

79 Citations (Scopus)

Abstract

Potassium-sulfur batteries hold practical promise for next-generation batteries because of their high theoretical gravimetric energy density and low cost. However, significant impediments are the sluggish K₂S oxidation kinetics and a lack of atomic-level understanding of K₂S oxidation. Here, for the first time, we report the catalytic oxidation of K₂S on a sulfur host with Co single atoms immobilized on nitrogen-doped carbon. On the basis of combined spectroscopic characterizations, electrochemical evaluation, and theoretical computations, we show a synergistic effect of dynamic Co-S and N-K interactions to catalyze K₂S oxidation. The resultant potassium-sulfur battery exhibited high capacities of 773 and 535 mAh g^-1 under high current densities of 1 and 2 C, respectively. These findings provide atomic-scale insights for the rational design of highly efficient sulfur hosts. © 2021 American Chemical Society.

Original language	English
Pages (from-to)	16902-16907
Journal	Journal of the American Chemical Society
Volume	143
Issue number	41
Online published	8 Oct 2021
DOIs	https://doi.org/10.1021/jacs.1c06255
Publication status	Published - 20 Oct 2021
Externally published	Yes

Funding

This work was supported financially by the Australian Research Council (ARC) through Discovery Project FL170100154. DFT computations were undertaken with the services from the National Computational Infrastructure (NCI) and Phoenix High Performance Computing at The University of Adelaide. The authors thank Dr. Bruce Cowie and Dr. Anton Tadich at the ANSTO for help with the NEXAFS test. Part of the experiment was performed at PD and soft-X-ray beamline, Australian Synchrotron, ANSTO. The authors gratefully acknowledge Dr. Bo You for guidance with materials synthesis.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Access Output

10.1021/jacs.1c06255

Other Access Options

Check CityUHK Library

Permanent Link

Right click to copy link

Cite this

@article{2958af3fe88542528717115c08b15b51,

title = "Catalytic Oxidation of K2S via Atomic Co and Pyridinic N Synergy in Potassium-Sulfur Batteries",

abstract = "Potassium-sulfur batteries hold practical promise for next-generation batteries because of their high theoretical gravimetric energy density and low cost. However, significant impediments are the sluggish K2S oxidation kinetics and a lack of atomic-level understanding of K2S oxidation. Here, for the first time, we report the catalytic oxidation of K2S on a sulfur host with Co single atoms immobilized on nitrogen-doped carbon. On the basis of combined spectroscopic characterizations, electrochemical evaluation, and theoretical computations, we show a synergistic effect of dynamic Co-S and N-K interactions to catalyze K2S oxidation. The resultant potassium-sulfur battery exhibited high capacities of 773 and 535 mAh g-1 under high current densities of 1 and 2 C, respectively. These findings provide atomic-scale insights for the rational design of highly efficient sulfur hosts. {\textcopyright} 2021 American Chemical Society.",

author = "Chao Ye and Jieqiong Shan and Dongliang Chao and Pei Liang and Yan Jiao and Junnan Hao and Qinfen Gu and Kenneth Davey and Haihui Wang and Shi-Zhang Qiao",

year = "2021",

month = oct,

day = "20",

doi = "10.1021/jacs.1c06255",

language = "English",

volume = "143",

pages = "16902--16907",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "41",

}

TY - JOUR

T1 - Catalytic Oxidation of K2S via Atomic Co and Pyridinic N Synergy in Potassium-Sulfur Batteries

AU - Ye, Chao

AU - Shan, Jieqiong

AU - Chao, Dongliang

AU - Liang, Pei

AU - Jiao, Yan

AU - Hao, Junnan

AU - Gu, Qinfen

AU - Davey, Kenneth

AU - Wang, Haihui

AU - Qiao, Shi-Zhang

PY - 2021/10/20

Y1 - 2021/10/20

N2 - Potassium-sulfur batteries hold practical promise for next-generation batteries because of their high theoretical gravimetric energy density and low cost. However, significant impediments are the sluggish K2S oxidation kinetics and a lack of atomic-level understanding of K2S oxidation. Here, for the first time, we report the catalytic oxidation of K2S on a sulfur host with Co single atoms immobilized on nitrogen-doped carbon. On the basis of combined spectroscopic characterizations, electrochemical evaluation, and theoretical computations, we show a synergistic effect of dynamic Co-S and N-K interactions to catalyze K2S oxidation. The resultant potassium-sulfur battery exhibited high capacities of 773 and 535 mAh g-1 under high current densities of 1 and 2 C, respectively. These findings provide atomic-scale insights for the rational design of highly efficient sulfur hosts. © 2021 American Chemical Society.

AB - Potassium-sulfur batteries hold practical promise for next-generation batteries because of their high theoretical gravimetric energy density and low cost. However, significant impediments are the sluggish K2S oxidation kinetics and a lack of atomic-level understanding of K2S oxidation. Here, for the first time, we report the catalytic oxidation of K2S on a sulfur host with Co single atoms immobilized on nitrogen-doped carbon. On the basis of combined spectroscopic characterizations, electrochemical evaluation, and theoretical computations, we show a synergistic effect of dynamic Co-S and N-K interactions to catalyze K2S oxidation. The resultant potassium-sulfur battery exhibited high capacities of 773 and 535 mAh g-1 under high current densities of 1 and 2 C, respectively. These findings provide atomic-scale insights for the rational design of highly efficient sulfur hosts. © 2021 American Chemical Society.

UR - https://www.scopus.com/pages/publications/85117496187

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85117496187&origin=recordpage

U2 - 10.1021/jacs.1c06255

DO - 10.1021/jacs.1c06255

M3 - RGC 21 - Publication in refereed journal

C2 - 34623812

SN - 0002-7863

VL - 143

SP - 16902

EP - 16907

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 41

ER -