Talk will highlight recent efforts to 1.) limit the extent of hydrogen evolution reaction (HER) and 2.) leverage products generated by HER to improve the reversibility of Zn plating/stripping in aqueous Zn-ion batteries. Emphasis is placed on the role of molecular dynamics and quantum chemistry calculations to address these issues. Topics covered include the development of mixed Zn-K and Zn-Li aqueous electrolytes and sacrificial additives.

Our research examines the electrochemical behavior of aqueous zinc metal batteries (AZMB), focusing on the pathways of electrons at current collectors during charging. We aim to elucidate the factors that determine an electron's fate, as it can participate in zinc electrodeposition, form a passivation film or solid electrolyte interphase, or engage in the hydrogen evolution reaction. These processes are inherently complex and interconnected, presenting significant challenges for understanding charge distribution.

A novel, scalable, conformal graphene encapsulation solution, co-developed at Argonne and Northwestern University, allows enhanced control of the material/electrolyte interface of Cathode Active Materials (CAM) thanks to a pinhole-free thin graphene layer. It improves cycle life, gassing, rate capability, and voltage and temperature range. This solution also enables next-generation CAM such as earth-abundant chemistries, offering wide temperature operability and immediate usability in existing production lines.

Next-generation battery cathodes require high-voltage operation (=4.5V) for greater capacity, cyclability, and thermal tolerance, but existing materials degrade quickly due to structural and electrochemical strain. We present a new cathode with a coherent architecture blending ordered and disordered frameworks with controllable Ni oxidation, enabling stable operation up to 4.7V with minimal capacity fade. Using multiscale diffraction and imaging, we demonstrate that this design is electrochemically and structurally robust, preventing surface degradation and lattice strain. This innovation offers a pathway to overcome voltage limitations and achieve high-performance, long-lasting cathodes.

Lithium (Li) metal has been highly regarded as an ultimate anode for high-energy rechargeable batteries. However, Li suffers from two main serious issues: (1) continuous formation of unstable solid electrolyte interphase and (2) Li dendritic growth. These issues have their roots in Li corrosions chemically and electrochemically. In searching for solutions, recently we have developed several novel Li-containing polymers (named as lithicones) via molecular layer deposition (MLD). The lithicone-protected Li showed compelling long-term cyclability in Li||Li symmetric cells and could dramatically boost the performance of Li||NMC811 (LiNi0.8Mn0.1Co0.1O2) cells, in terms of sustainable capacity and capacity retention. 

We are developing high-performance lithium-ion batteries using a vanadium-based oxide anode for heavy-duty applications such as mining, construction, and military vehicles. These batteries enable faster charging, longer cycle life, and improved low-temperature performance. By utilizing this proprietary vanadium-based anode, we aim to achieve 10x faster charging (<6 mins to 80% SOC), 10x the cycle life (>10,000 cycles), and the ability to charge below freezing (-40°C), while also enhancing safety with the use of a metal oxide anode.

Polymers can serve as composite materials with oxides to provide unprecedented high ionic conductivity and low interfacial resistance for the all solid-state batteries. Here we introduced two approaches, 1) design of single ion conducting polymer electrolytes (SIE); 2) design of crosslinkers. Significant improvements in Li transference number, electrochemical stability, and cycling life are observed with these designs. To improve the anodic stability of polymer electrolytes, a fundamental shift in the building blocks from -CH2-CH2-O- is needed. This is where borate structures come into play, offering both high intrinsic stability and superior interfacial stability.

In contrast to solid-liquid electrochemical interfacial processes, solid-state batteries must cope with heterogeneous solid-solid interfaces under mechanical constraints. In this talk, I will discuss the development of ultrafast XCT, photoacoustic microscopy, and confocal Raman microscopy, to directly visualize the dynamic evolution of physicochemical fields. An electrode-adaptive Real 2D (R2D) modeling strategy will also be introduced. These lead to innovative ways to manage and control heterogeneity, thus improving electrochemical performance.

Sodium-ion batteries are gaining increased attention due to considerations that include their cost-effectiveness, sustainability and supply-chain resilience. In this presentation we will discuss insights from 3-electrode cell experiments being conducted at Argonne National Laboratory using layered-oxide cathodes, hard-carbon anodes, and carbonate-based electrolytes. Performance characteristics such as cell capacity fade, impedance rise, voltage-profile changes and the effect of hard-carbon hysteresis and sodium-plating during electrochemical cycling will be discussed.

Through a breakthrough alloy anode innovation, the energy densities of sodium ion batteries can be increased by a factor of 2x and avoid battery safety hazards, offering competitive advantages in e-mobility and energy storage markets. This session will showcase datasets from state-of-the-art commercial scale sodium ion batteries, with unprecedented energy densities, performance, and rigorous safety testing results of U.S.-made advanced sodium ion batteries.

Na-ion cathodes undergo severe chemo-mechanical deformations, which lead to poor capacity retention. Chemo-mechanical deformations can originate from interfacial and structural instabilities. There is a critical scientific need for a comprehensive understanding of the reaction-transport behavior and mechanics of cathodes in Na-ion chemistry. I will present instability mechanisms in battery electrodes by probing operando mechanical deformations during cycling.