Solid-state batteries (SSBs) employing a lithium metal anode are a promising candidate for next-generation energy storage systems, delivering higher power and energy densities. Interfacial instabilities due to non-uniform electrodeposition at the anode−solid electrolyte (SE) interface pose major constraints on the safety and endurance of SSBs. In this regard, non-uniform kinetic interactions at the anode−SE interface which are derived from cathode microstructural heterogeneity can have significant impact on anode stability. In this work, we present a comprehensive insight into microstructural heterogeneity-driven cathode−anode cross-talk and delineate the role of cathode architecture and SE separator design in dictating reaction heterogeneity at the anode−SE interface. We show that intrinsic and extrinsic parameters, such as cathode loading, separator thickness, particle morphologies of active material and SE, and temperature can have significant impact on reaction heterogeneity at the anode−SE interface and thus govern anode stability. Tradeoff between energy density and anode stability while achieving higher cathode loading and thinner SE separators is highlighted, and potential strategies to mitigate this problem are discussed. This work provides fundamental insights into cathode−anode cross-talk involving interfacial heterogeneities and enhancement in energy densities of SSBs via electrode engineering.
A s the world around us ushered in Industry 5.0, an industrial revolution driven by the common principle of improving sustainability, climate change has emerged as one of the most pressing problems. Attaining a decarbonized infrastructure is predicated on the adoption of pragmatic solutions to combat climate change that include intermittent renewable energy sources and electrochemical energy conversion systems with the grid reliant on energy storage technologies. 1−6 Electrochemical energy systems that promise suitable scaling attributes can be harnessed across a wide range, starting from the transportation sector to stationary and portable applications, while maintaining reliable operation in the event of fuel price spikes, supply chain shortages, power disruptions, and natural disasters, thus enhancing energy resilience. 7−9 However, this transition comes at the cost of inequitable distribution of benefits and burdens. 8 Historically marginalized communities often cannot afford and/or do not have access to cleaner energy sources. Electrochemical energy systems can also be scaled and sited strategically in response to local community needs, for example, where marginalized/affected communities are located, increasing availability and accessibility. 7 In these ways, electrochemical energy storage systems play an important role in promoting energy justice as schematically depicted in Figure 1. However, the exchange of scientific ideas and dialogue in this regard took a backseat with the onset of the COVID-19 pandemic from the beginning of 2020. The resulting crisis has tremendously impacted, inter alia, the sociopolitical scenario, economy, and livelihood of almost everyone in one way or the other. Most of the countries in the world took preventive measures to restrain the pandemic, but the long-term consequences of such undertakings were inconceivable at the beginning. The pandemic threatened to disrupt communication and collaboration among peers in the scientific community, which is one of the cruces of the scientific diaspora. 10 Unabated spread of the pandemic led to the cancellation of in-person events such as conferences, meetings, seminars, and invited talks, which are typical avenues of collaboration, amalgamation, and networking for professors, scientists, graduate students, postdocs, and early career researchers. However, science always finds new avenues in the face of adversity, and methods of virtual engagement were embraced in lieu of in-person engagements. A year into the pandemic, cloud-based video and audio communication platforms became sine qua non for conferences and meetings. These frameworks
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