TY - JOUR
T1 - Room-Temperature Aluminum-Sulfur Batteries with a Lithium-Ion-Mediated Ionic Liquid Electrolyte
AU - Yu, Xingwen
AU - Boyer, Mathew J.
AU - Hwang, Gyeong S.
AU - Manthiram, Arumugam
N1 - Funding Information:
This work was supported by the Materials Sciences and Engineering Division of the US Department of Energy Office of Science under award number DE-SC0005397 . G.S.H. also greatly acknowledges the Robert A. Welch Foundation ( F-1535 ) for partial financial support of the computational work and the Texas Advanced Computing Center for providing high-performance computing resources. The authors thank Mr. Sanjay Nanda and Ms. Haley Stowe for their assistance with the XPS data collection and the quantum chemical calculations, respectively.
Publisher Copyright:
© 2017 Elsevier Inc.
PY - 2018/3/8
Y1 - 2018/3/8
N2 - Aluminum-sulfur (Al-S) chemistry is attractive for the development of future-generation electrochemical energy storage technologies. However, to date, only limited reversible Al-S chemistry has been demonstrated. This paper demonstrates a highly reversible room-temperature Al-S battery with a lithium-ion (Li+-ion)-mediated ionic liquid electrolyte. Mechanistic studies with electrochemical and spectroscopic methodologies revealed that the enhancement in reversibility by Li+-ion mediation is attributed to the chemical reactivation of aluminum polysulfides and/or sulfide by Li+ during electrochemical cycling. The results obtained with X-ray photoelectron spectroscopy and density functional theory calculations suggest the presence of a Li3AlS3-like product with a mixture of Li2S- and Al2S3-like phases in the discharged sulfur cathode. With Li+-ion mediation, the cycle life of room-temperature Al-S batteries is greatly improved. The cell delivers an initial capacity of ∼1,000 mA hr g−1 and maintains a capacity of up to 600 mA hr g−1 after 50 cycles. Batteries represent an indispensable technology for electrifying the transportation sector and for storing electricity produced from renewable sources. Ambient-temperature non-aqueous sulfur battery chemistries are becoming increasingly appealing for these applications. Although lithium-sulfur batteries have been extensively investigated in recent years, aluminum-sulfur (Al-S) chemistry is more attractive from an economical, sustainability, and safety point of view. However, because of a lack of effective electrolytes, only limited reversibility has been realized so far with Al-S chemistry. This paper presents a lithium-ion mediation strategy for enhancing the reversibility of Al-S chemistry at ambient temperatures. A lithium-ion-mediated ionic liquid electrolyte remarkably improves the electrochemical performance of Al-S batteries. Based on a series of experimental and computational simulation analyses, the relevant mechanisms are presented. Manthiram and colleagues have validated a Li+-ion mediation approach to enhance the electrochemical reversibility of ambient-temperature aluminum-sulfur (Al-S) battery chemistry. They systematically investigated the relevant mechanisms with combined experimental and theoretical methodologies. Al-S chemistry is attractive for the development of high-energy, low-cost, safe, next-generation electrochemical energy storage technologies.
AB - Aluminum-sulfur (Al-S) chemistry is attractive for the development of future-generation electrochemical energy storage technologies. However, to date, only limited reversible Al-S chemistry has been demonstrated. This paper demonstrates a highly reversible room-temperature Al-S battery with a lithium-ion (Li+-ion)-mediated ionic liquid electrolyte. Mechanistic studies with electrochemical and spectroscopic methodologies revealed that the enhancement in reversibility by Li+-ion mediation is attributed to the chemical reactivation of aluminum polysulfides and/or sulfide by Li+ during electrochemical cycling. The results obtained with X-ray photoelectron spectroscopy and density functional theory calculations suggest the presence of a Li3AlS3-like product with a mixture of Li2S- and Al2S3-like phases in the discharged sulfur cathode. With Li+-ion mediation, the cycle life of room-temperature Al-S batteries is greatly improved. The cell delivers an initial capacity of ∼1,000 mA hr g−1 and maintains a capacity of up to 600 mA hr g−1 after 50 cycles. Batteries represent an indispensable technology for electrifying the transportation sector and for storing electricity produced from renewable sources. Ambient-temperature non-aqueous sulfur battery chemistries are becoming increasingly appealing for these applications. Although lithium-sulfur batteries have been extensively investigated in recent years, aluminum-sulfur (Al-S) chemistry is more attractive from an economical, sustainability, and safety point of view. However, because of a lack of effective electrolytes, only limited reversibility has been realized so far with Al-S chemistry. This paper presents a lithium-ion mediation strategy for enhancing the reversibility of Al-S chemistry at ambient temperatures. A lithium-ion-mediated ionic liquid electrolyte remarkably improves the electrochemical performance of Al-S batteries. Based on a series of experimental and computational simulation analyses, the relevant mechanisms are presented. Manthiram and colleagues have validated a Li+-ion mediation approach to enhance the electrochemical reversibility of ambient-temperature aluminum-sulfur (Al-S) battery chemistry. They systematically investigated the relevant mechanisms with combined experimental and theoretical methodologies. Al-S chemistry is attractive for the development of high-energy, low-cost, safe, next-generation electrochemical energy storage technologies.
KW - aluminum-sulfur battery
KW - density functional theory calculation
KW - electrochemical mechanism
KW - ionic liquid electrolyte
KW - Li-ion mediation
UR - http://www.scopus.com/inward/record.url?scp=85043494322&partnerID=8YFLogxK
U2 - 10.1016/j.chempr.2017.12.029
DO - 10.1016/j.chempr.2017.12.029
M3 - Article
AN - SCOPUS:85043494322
SN - 2451-9308
VL - 4
SP - 586
EP - 598
JO - Chem
JF - Chem
IS - 3
ER -