The project, titled “Controlling dimensionality and ligand connectivity to tune intercalation properties in transition metal oxychlorides,” addresses one of the central challenges facing rechargeable batteries: how to develop high-performing materials from elements that are abundant, affordable, and less vulnerable to supply-chain limitations. Lithium-ion batteries have become essential in electric vehicles, consumer electronics, and renewable-energy systems, but many of their constituent materials depend on geographically concentrated resources and complex refining networks.

Grimaud, an associate professor of chemistry who joined Boston College in 2022, leads a research group focused on the fundamental chemistry of electrochemical interfaces. These interfaces are the regions where electrodes and electrolytes meet, and they govern how ions move, how electrons flow, and how battery materials change during charging and discharging. A material that appears promising in isolation may perform poorly in a working battery if it reacts unfavorably with the surrounding electrolyte.

“The same battery material may succeed or fail depending on the electrolyte surrounding it,” Grimaud explained. His team is therefore studying not only the solid electrode materials themselves but also the chemical environment in which they operate. Electrolytes—liquids or solids that transport ions between battery electrodes—can influence the stability, reversibility, voltage, and lifetime of a cell. By designing electrolytes with adjustable chemical properties, researchers may be able to make previously unstable materials function reliably.

The new NSF-supported research will focus on mixed-anion materials containing both oxygen and chlorine. In conventional battery compounds, oxygen is often the dominant negatively charged element, or anion. Replacing or combining oxygen with another anion can change the electronic structure, bonding, crystal geometry, and reactivity of a material. Those changes may determine how easily lithium or sodium ions can enter and leave the structure, a process known as intercalation.

During intercalation, ions move reversibly into spaces within a host material without completely destroying its framework. This process is fundamental to the operation of many rechargeable batteries. When a battery charges, lithium or sodium ions migrate into the electrode; when it discharges, they move back while electrons travel through an external circuit. The speed, capacity, and durability of this process depend on the pathways available for ion movement and on whether the host structure can withstand repeated chemical and structural changes.

Grimaud’s team has already achieved reversible lithium intercalation in several oxychloride materials. In one demonstration, a compound composed of iron, oxygen, and chlorine delivered energy density and electrochemical performance comparable to an established iron-and-phosphate material. Iron, oxygen, and chlorine are relatively abundant and inexpensive elements, while phosphate-based materials can be tied to sourcing and refining constraints and may compete with agricultural uses for phosphate resources.

The researchers now aim to determine how the dimensionality of these compounds and the connectivity of their chemical building blocks affect ion storage. In materials science, dimensionality describes whether a structure forms isolated units, chains, sheets, or three-dimensional networks. Ligand connectivity refers to the way atoms or molecular groups bind to a central metal and to one another. Adjusting these features could allow scientists to tune a material’s voltage, capacity, conductivity, structural stability, and selectivity for lithium or sodium.

The implications extend beyond batteries. Grimaud said that precise control over the electronic and structural properties of oxychloride materials could open possibilities in electronics and quantum technologies, where unusual electrical, magnetic, or optical behaviors are valuable. The work may also support the development of sodium-ion batteries, which are attracting interest as a complement to lithium-based systems because sodium is widely distributed and potentially easier to source at large scale.

The CAREER Award will support both laboratory research and educational programs. Grimaud plans to use findings from the project to introduce Boston College students to the links between materials design, energy technology, and environmental consequences. He will also work with students in grades eight through twelve who participate in The Academy, a free enrichment program supported by Boston College’s Pine Manor Institute for Student Success. Laboratory activities will introduce these students to battery chemistry while encouraging them to consider how raw materials are sourced, refined, used, and eventually recycled.

As battery technologies expand rapidly, Grimaud argues that performance alone cannot define progress. Future materials must be evaluated alongside their social and ecological costs, including mineral availability, energy-intensive processing, waste, and geopolitical dependence. By combining fundamental chemistry with education and broader sustainability questions, the project aims to develop better battery materials while preparing a new generation of scientists to think critically about the technologies they create.

Subject of Research: Battery materials chemistry, transition metal oxychlorides, lithium- and sodium-ion batteries, electrochemical interfaces, and tunable electrolytes

Image Credits: Boston College

Keywords

Chemistry, energy, electrochemistry, electrochemical cells, batteries, battery materials, lithium-ion batteries, sodium-ion batteries, materials science, quantum technologies, National Science Foundation, Boston College

Lithium-manganese-rich oxides have long been recognized as attractive candidates for cathode materials due to their abundance, low cost, and reduced environmental impact compared to cobalt-containing alternatives. Nonetheless, their practical deployment has been marred by the intrinsic Jahn-Teller distortions originating from Mn³⁺ ions. These distortions induce structural changes leading to rapid capacity fading and battery degradation during cycling. Until now, managing these distortions typically involved macroscopic strategies such as doping or protective coatings, which often addressed symptoms rather than the root electronic causes.

The pioneering research from WPI-AIMR offers a paradigm shift by focusing on the atomic-scale orbital configurations responsible for manganese instability. By leveraging the concept of “orbital geometric frustration” at specially designed noncollinear interfaces within the cathode material, the team effectively neutralized the cooperative Jahn-Teller distortions. This approach disrupts the collective lattice distortions at a fundamental electronic level, thereby preserving the crystal structure integrity and significantly extending the lifecycle of the cathode.

This exceptional interfacial control allows the creation of a heterostructure wherein collinear and noncollinear phases coexist, mediating the orbital states of Mn³⁺ ions and stabilizing them against deformation. The resulting cathode material, a reinforced form of LiMnO₂, exhibits near-perfect cycling stability, demonstrating virtually zero capacity loss even after 500 charge-discharge cycles—an unprecedented performance metric in manganese oxide cathodes.

A remarkable aspect of this advancement lies in the bridging of disciplines: by weaving concepts from solid-state physics, specifically electronic orbital topology, into electrochemical material design, the researchers establish a novel methodology for overcoming performance-limiting phenomena in battery electrodes. This synergy transcends traditional materials engineering, signaling a transformative approach towards designing energy storage systems from the electronic level upwards.

Beyond the fundamental scientific triumph, this breakthrough bears vast implications for the development and commercialization of electrified transportation and stationary energy storage. Cobalt, historically essential for high-performance cathodes, is beset by supply-chain constraints and ethical mining concerns. In contrast, manganese is naturally abundant, widely accessible, and inherently more sustainable. Thus, manganese-based cathodes engineered with this orbital approach promise to curtail production costs, enhance battery durability, and promote greener manufacturing practices.

Electric vehicles equipped with batteries containing these robust manganese cathodes could soon achieve extended service lifetimes and consistent performance without the risk of accelerated degradation. This technological leap would alleviate consumer anxieties related to battery replacement costs and range reliability, accelerating adoption rates in the automotive sector. Additionally, wind and solar energy assets could benefit from cost-effective grid-scale storage solutions, enabling more substantial integration of renewable resources into electricity grids and boosting efforts toward carbon neutrality.

Looking ahead, the research team envisions expanding the application of their interfacial orbital engineering strategy to other battery chemistries. Notably, manganese-based oxides hold significant potential for sodium-ion batteries, which may offer complementary benefits in terms of raw material availability and cost. By applying similar atomic-scale manipulation techniques, the pathway to high-performance, long-lived sodium-ion cathodes becomes increasingly viable.

The journal article detailing these findings was published in the Journal of the American Chemical Society on February 11, 2026, under the title “Interface-Mediated Jahn-Teller Effect in a Structure-Reinforced LiMnO2 Cathode.” This work not only reshapes the conceptual framework for cathode design but also lays a robust foundation for next-generation energy storage materials that merge fundamental physics with applied chemistry.

As this research ripples through the scientific community, its implications for sustainable energy technology are profound, marking a crucial step towards electrified mobility and renewable energy infrastructure that are affordable, safe, and environmentally conscious. The synthesis of interfacial orbital frustration to suppress deleterious Jahn-Teller effects heralds a new epoch in battery innovation—one where atomic-level engineering yields macroscopic benefits to society and the planet.

Subject of Research:
Article Title: Interface-Mediated Jahn-Teller Effect in a Structure-Reinforced LiMnO2 Cathode
News Publication Date: February 11, 2026
Web References: http://dx.doi.org/10.1021/jacs.5c20036
Image Credits: © Hanghui Liu et al.

Keywords

Cathodes, Batteries, Manganese, Electrochemistry, Physics, Materials science