Investigating the Multifunctional Role of Tris(trimethylsilyl)phosphite as an Electrolyte Additive via Operando Gas Chromatography/Mass Spectrometry and X-ray Photoelectron Spectroscopy

IF 6.2 Q2 ENERGY & FUELS
Christiane Groher, Damian Marlon Cupid, Qixiang Jiang, Erwin Rosenberg, Jürgen Kahr
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引用次数: 0

Abstract

The multifunctional electrolyte additive tris(trimethylsilyl)phosphite (TMSP) is investigated with a combination of operando gas chromatography/mass spectrometry and X-ray photoelectron spectroscopy techniques, supported by cycling experiments and electrochemical impedance spectroscopy (EIS) measurements. Indications for hydrofluoric acid (HF) scavenging by TMSP could be found in the gas phase as well as on the electrode surfaces; however, it is observed that the use of TMSP leads to the production of HF, which it eventually scavenges. The investigation of the interphase formation shows that the decomposition products of TMSP are integrated into the interphases of both electrodes. This is accompanied by the formation of trimethylsilane as a decomposition product in the gas phase. TMSP also promotes the two-electron reduction of ethylene carbonate (EC), which is deduced both from an increased amount of ethene in the gas phase and from Li2CO3 on the electrode surface. The electrochemical investigations show that cells with TMSP have a lower interphase resistance after continued cycling. However, only the cells with 1 wt% of TMSP in the electrolyte outperform the TMSP-free reference cells. It is concluded that adding more than 1 wt% of TMSP increases the parasitic reactions of the additive to an extent that it partially counteracts its beneficial effect.

Abstract Image

利用Operando气相色谱/质谱和x射线光电子能谱研究三甲基硅基亚磷酸酯作为电解质添加剂的多功能作用
采用气相色谱/质谱和x射线光电子能谱技术,结合循环实验和电化学阻抗谱(EIS)测量,对多功能电解质添加剂三甲基硅基亚磷酸酯(TMSP)进行了研究。TMSP清除氢氟酸(HF)的迹象可以在气相和电极表面发现;然而,观察到TMSP的使用导致HF的产生,并最终清除HF。对间相形成的研究表明,TMSP的分解产物被整合到两个电极的间相中。这是伴随着形成三甲基硅烷作为分解产物在气相。TMSP还促进了碳酸乙烯(EC)的双电子还原,这是由气相中乙烯量的增加和电极表面Li2CO3的增加推断的。电化学研究表明,在持续循环后,具有TMSP的电池具有较低的间期电阻。然而,只有电解质中TMSP含量为1wt %的电池表现优于不含TMSP的参考电池。结果表明,添加超过1wt %的TMSP会使添加剂的寄生反应增加,从而部分抵消了其有益作用。
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来源期刊
CiteScore
8.20
自引率
3.40%
发文量
0
期刊介绍: Advanced Energy and Sustainability Research is an open access academic journal that focuses on publishing high-quality peer-reviewed research articles in the areas of energy harvesting, conversion, storage, distribution, applications, ecology, climate change, water and environmental sciences, and related societal impacts. The journal provides readers with free access to influential scientific research that has undergone rigorous peer review, a common feature of all journals in the Advanced series. In addition to original research articles, the journal publishes opinion, editorial and review articles designed to meet the needs of a broad readership interested in energy and sustainability science and related fields. In addition, Advanced Energy and Sustainability Research is indexed in several abstracting and indexing services, including: CAS: Chemical Abstracts Service (ACS) Directory of Open Access Journals (DOAJ) Emerging Sources Citation Index (Clarivate Analytics) INSPEC (IET) Web of Science (Clarivate Analytics).
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