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Impurities in electrolyte additives
Miscellaneous impurities in electrolyte additives:
1. Impurities are unavoidable, and what impurities matter.
2. Some compatible impurities.
3. Little influence on impurities sulfate fluorion phosphate carbonate dimer or trimer residual solvent
4. Very large impurities chloride ions: water alcohols, aldehydes, acids, substances containing active hydrogen impurities Metal ions: environmental pollutants:
5. The impact is not clear.
First of all, whether it is a benign influence or a small influence, it is not "do not control". All impurities need to be regulated, at least to know how much their content is, at least how much is allowed to depend on their nature.
New electrolyte additive helps stabilize cycling of 5V lithium metal batteries (EES)
In recent years, based on cobalt-free LiNi0.5Mn1.5O4 (LNMO) positive electrode (5 V class, vs. Li+/Li) and lithium metal anode (3.04 V vs. Ultrahigh pressure lithium metal batteries with standard hydrogen electrodes have attracted a lot of attention as promising candidates for the next generation of high energy density and sustainable batteries due to their theoretical energy density of up to ~650 Wh/kg. In contrast to the unstable layered oxide LiNixCoyMnzO2, the toxic Co element caused by the LNMO spinel structure is eliminated and the inherent safety is eliminated. However, their development is severely limited by the incompatibility between the state-of-the-art carbonate electrolyte and the two aggressive electrodes. Here, we have synthesized a new electrolyte additive,2, 2-difluoroethylmethyl sulfone (FS), which enables stable cycling of ultra-high pressure lithium metal batteries in conventional carbonate electrolytes. On the cathode side, unlike conventional electrolyte additives, FS can be selectively adsorbed on the LNMO surface to form a special assembled FS "buffer" layer that can effectively remove free carbonate molecules from the cathode surface. Therefore, during charging, the -CF2H group of FS is well decomposed by the anode to form an inorganic rich CEI, which effectively inhibits the micro-fracture and transition metal dissolution of LNMO. On the anode side, FS can also perform cathode decomposition well, resulting in an inorganic rich SEI for stable cycling of Li metal anodes. As a result, the carbonate electrolyte containing FS additives gives cobalt-free 5V-class lithium metal batteries unprecedented high performance, i.e. a 40um-Li /LNMO (load = 7 mg·cm2) full battery with a high capacity retention rate of 84% for 600 cycles at 1C using a commercial carbon-based low-concentration electrolyte. A complete battery consisting of a highly loaded cathode (20 mg·cm2) and an ultra-thin lithium anode (40 mm) has a capacity retention rate of 99% after 100 cycles at 0.25C. In addition, to our knowledge, previously unreported Li/LNMO bag-like batteries have been assembled and can run stably for more than 150 cycles. This paper is based on Rational molecular design of electrolyte additive endows stable cycling performance of cobalt-free 5 V-class lithium metal batteries, published in Energy & Environmental Science.
Uses of LiDFOB and TMSP Additives
The document describes two electrolyte additives for lithium-ion batteries: LiDFOB (Lithium Difluoro(oxalato)borate) and TMSP (Tris(trimethylsilyl) phosphite). LiDFOB is a multifunctional lithium-salt-type additive that primarily forms a dense, ion-conductive SEI film on the anode (graphite/silicon/lithium metal), improving initial Coulombic efficiency and cycle life, while also stabilizing the cathode interface under high voltage (≥4.5 V) and enhancing both low-temperature conductivity and high-temperature thermal stability. TMSP is a cathode film-forming additive designed for high‑nickel ternary systems (e.g., NCM811) at high voltages (4.4–4.6 V); it forms a thin, P/Si‑containing CEI layer on the cathode, scavenges HF to prevent corrosion, reduces interfacial impedance, and improves capacity retention by over 20% under 4.5 V cycling. When used together at 1% each, LiDFOB and TMSP synergistically build stable SEI and CEI layers, suppress structural degradation and gas generation in NCM811 cathodes even at 4.7 V, and improve cycle life by more than 30% while maintaining balanced performance across high and low temperatures.
NCM811 battery achieves stability at 4.8V
Researchers led by Professor Guangliang Liu at Shenzhen University have developed a mechanically adaptive polyimide (PI) coating for single-crystal NCM811 cathodes to stabilize high-voltage operation in sulfide-based all-solid-state batteries. Published in Advanced Science, the study introduces a nanoscale PI interface that provides a triple synergy of chemical anchoring, mechanical adaptability, and electrochemical self-optimization.
The PI coating chemically bonds to the cathode surface, removing detrimental residual lithium compounds and passivating the interface. Its viscoelastic nature dramatically lowers the cathode’s Young's modulus, allowing it to absorb volume changes and prevent microcrack formation. Remarkably, the PI interface exhibits a “negative aging” effect, where interfacial impedance decreases by 38% during cycling, indicating dynamic structural evolution that improves ion transport.
This innovation yields exceptional performance: at 4.3V, capacity retention reaches 83.6% after 400 cycles (vs. 33.2% for uncoated). Even under extreme conditions of 4.8V, a thicker PI coating maintains 85.9% capacity retention. This work offers a powerful solution to the critical interface challenges facing next-generation high-energy-density solid-state batteries.
This study identifies electron loss, rather than mere lithium loss, as the root cause of the initial irreversible capacity loss in lithium-ion batteries, and proposes a universal capacity compensation strategy mediated by the electrolyte. As a proof of concept, the researchers developed lithium polyphosphate as a soluble capacity compensation reagent. Lithium polyphosphate preferentially oxidizes at the cathode side, supplying electrons to offset the irreversible capacity loss while also helping to construct a stable cathode-electrolyte interphase. In an NCM811||graphite full cell, the electrolyte containing lithium polyphosphate delivered a first-cycle discharge capacity of 221.4 mAh g⁻¹ and an initial Coulombic efficiency of 86.7%, compared to 196.5 mAh g⁻¹ and 79.6% for the blank electrolyte. After 400 cycles, the cells retained 84.2% of their capacity, significantly outperforming the control group's 68.2%. The feasibility of lithium polyphosphate was also verified in LiFePO₄||graphite and LiCoO₂||graphite full cells. Compared with traditional solid-state prelithiation reagents such as Li₅FeO₄, lithium polyphosphate offers advantages in specific capacity, cost, electrolyte compatibility, operational feasibility, safety, and lifetime.
The Most Comprehensive In-Depth Analysis Ever (Including Latest Industry Trends)
Among the key materials of lithium-ion batteries, the electrolyte is often underestimated as a simple "ion transport medium," but its true role is that of a "system control hub" that integrates battery performance. By regulating the solvation structure and interface reaction pathways, it governs the formation of the SEI/CEI protective films, thereby determining the battery's fast-charging capability, cycle life, and safety. The essence of electrolyte design lies in skillfully balancing multiple inherent contradictions: achieving high ionic conductivity requires overcoming the limitations of solvent high viscosity; constructing a stable electrode interface necessitates utilizing the property of "selective decomposition" of electrolyte components; meanwhile, enhancing flame retardancy often comes at the cost of conductivity. More importantly, it is the critical bottleneck for the industrialization of next-generation high-energy-density batteries (such as high-nickel cathodes, silicon-based anodes, and lithium metal anodes), requiring specialized formulations to address specific pain points like high-voltage oxidation, significant volume expansion, and lithium dendrite growth. Ultimately, there is no "perfect" electrolyte, only the engineering-optimal solution found for a specific battery system and performance requirements, balancing conductivity, stability, safety, and compatibility.
