Schroeder Marshall A, Kumar Nitin, Pearse Alexander J, Liu Chanyuan, Lee Sang Bok, Rubloff Gary W, Leung Kevin, Noked Malachi
†Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, United States.
§Sandia National Laboratories, Albuquerque, New Mexico 87185, United States.
ACS Appl Mater Interfaces. 2015 Jun 3;7(21):11402-11. doi: 10.1021/acsami.5b01969. Epub 2015 May 19.
One of the greatest obstacles for the realization of the nonaqueous Li-O2 battery is finding a solvent that is chemically and electrochemically stable under cell operating conditions. Dimethyl sulfoxide (DMSO) is an attractive candidate for rechargeable Li-O2 battery studies; however, there is still significant controversy regarding its stability on the Li-O2 cathode surface. We performed multiple experiments (in situ XPS, FTIR, Raman, and XRD) which assess the stability of the DMSO-Li2O2 interface and report perspectives on previously published studies. Our electrochemical experiments show long-term stable cycling of a DMSO-based operating Li-O2 cell with a platinum@carbon nanotube core-shell cathode fabricated via atomic layer deposition, specifically with >45 cycles of 40 h of discharge per cycle. This work is complemented by density functional theory calculations of DMSO degradation pathways on Li2O2. Both experimental and theoretical evidence strongly suggests that DMSO is chemically and electrochemically stable on the surface of Li2O2 under the reported operating conditions.
实现非水锂氧电池的最大障碍之一是找到一种在电池工作条件下化学和电化学稳定的溶剂。二甲基亚砜（DMSO）是可充电锂氧电池研究中一个有吸引力的候选溶剂；然而，关于其在锂氧阴极表面的稳定性仍存在重大争议。我们进行了多项实验（原位XPS、FTIR、拉曼和XRD），评估了DMSO-Li2O2界面的稳定性，并报告了对先前发表研究的看法。我们的电化学实验表明，通过原子层沉积制备的铂@碳纳米管核壳阴极的基于DMSO的工作锂氧电池具有长期稳定的循环性能，特别是每个循环有>45次40小时的放电循环。这项工作得到了Li2O2上DMSO降解途径的密度泛函理论计算的补充。实验和理论证据都强烈表明，在所报道的工作条件下，DMSO在Li2O2表面化学和电化学稳定。
