TY - JOUR
T1 - Boosting the reaction kinetics in aprotic lithium-carbon dioxide batteries with unconventional phase metal nanomaterials
AU - Zhou, Jingwen
AU - Wang, Tianshuai
AU - Chen, Lin
AU - Liao, Lingwen
AU - Wang, Yunhao
AU - Xi, Shibo
AU - Chen, Bo
AU - Lin, Ting
AU - Zhang, Qinghua
AU - Ye, Chenliang
AU - Zhou, Xichen
AU - Guan, Zhiqiang
AU - Zhai, Li
AU - He, Zhen
AU - Wang, Gang
AU - Wang, Juan
AU - Yu, Jinli
AU - Ma, Yangbo
AU - Lu, Pengyi
AU - Xiong, Yuecheng
AU - Lu, Shiyao
AU - Chen, Ye
AU - Wang, Bin
AU - Lee, Chun-Sing
AU - Cheng, Jianli
AU - Gu, Lin
AU - Zhao, Tianshou
AU - Fan, Zhanxi
PY - 2022/10/4
Y1 - 2022/10/4
N2 - Given the high energy density and eco-friendly characteristics, lithium-carbon dioxide (Li-CO2) batteries have been considered to be a next-generation energy technology to promote carbon neutral and space exploration. However, Li-CO2 batteries suffer from sluggish reaction kinetics, causing large overpotential and poor energy efficiency. Here, we observe enhanced reaction kinetics in aprotic Li-CO2 batteries with unconventional phase 4H/face-centered cubic (fcc) iridium (Ir) nanostructures grown on gold template. Significantly, 4H/fcc Ir exhibits superior electrochemical performance over fcc Ir in facilitating the round-trip reaction kinetics of Li+-mediated CO2 reduction and evolution, achieving a low charge plateau below 3.61 V and high energy efficiency of 83.8%. Ex situ/in situ studies and theoretical calculations reveal that the boosted reaction kinetics arises from the highly reversible generation of amorphous/low-crystalline discharge products on 4H/fcc Ir via the Ir-O coupling. The demonstration of flexible Li-CO2 pouch cells with 4H/fcc Ir suggests the feasibility of using unconventional phase nanomaterials in practical scenarios.
AB - Given the high energy density and eco-friendly characteristics, lithium-carbon dioxide (Li-CO2) batteries have been considered to be a next-generation energy technology to promote carbon neutral and space exploration. However, Li-CO2 batteries suffer from sluggish reaction kinetics, causing large overpotential and poor energy efficiency. Here, we observe enhanced reaction kinetics in aprotic Li-CO2 batteries with unconventional phase 4H/face-centered cubic (fcc) iridium (Ir) nanostructures grown on gold template. Significantly, 4H/fcc Ir exhibits superior electrochemical performance over fcc Ir in facilitating the round-trip reaction kinetics of Li+-mediated CO2 reduction and evolution, achieving a low charge plateau below 3.61 V and high energy efficiency of 83.8%. Ex situ/in situ studies and theoretical calculations reveal that the boosted reaction kinetics arises from the highly reversible generation of amorphous/low-crystalline discharge products on 4H/fcc Ir via the Ir-O coupling. The demonstration of flexible Li-CO2 pouch cells with 4H/fcc Ir suggests the feasibility of using unconventional phase nanomaterials in practical scenarios.
KW - electrochemical mechanism
KW - Ir nanostructures
KW - Li-CO2 battery
KW - reaction kinetics
KW - unconventional phase
UR - http://www.scopus.com/inward/record.url?scp=85138601064&partnerID=8YFLogxK
UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85138601064&origin=recordpage
U2 - 10.1073/pnas.2204666119
DO - 10.1073/pnas.2204666119
M3 - RGC 21 - Publication in refereed journal
C2 - 36161954
SN - 1091-6490
VL - 119
JO - Proceedings of the National Academy of Sciences
JF - Proceedings of the National Academy of Sciences
IS - 40
M1 - e2204666119
ER -
