Quantum Insights into the Energy Storage and Environmental Sustainability

The current energy crisis and climate concerns urgently require our materials science community to accelerate the discovery and development of more promising materials for designing next-generation energy storage and electrocatalytic systems. The goal of our research has been to employ and develop advanced quantum methods to promote the reactivity and selectivity of renewable energy ecosystems by providing atomic-level understanding.

In this talk, we will first share our recent efforts on the energy storage front, where theoretical designs on material surfaces and interfaces have been conducted to facilitate the optimization of current lithium-air batteries (LABs).¹ Emphasis is placed on understanding the system dynamics through the implementation of methods including ab initio grand canonical Monte Carlo and enhanced free energy sampling algorithms. Through our computational simulations, we found the selection of aprotic solvents in electrolyte dominates the discharge/charge pathways of LABs. In general, high donor number (DN) electrolytes (such as DMSO) can rapidly transport the discharge products (LiO₂ monomers) away from the electrode surface, thus avoiding the deactivation and passivation of the electrode. To address the issues of environmental pollution, we also recently developed a hybrid microenvironment for highly selective conversion of CO₂ into C₃H₈ by coating imidazole-functionalized (*Im) ionic liquids on solid-state electrodes.² The *Im layer is effective to increase the electronic conductivity of solid-state catalyst, meanwhile it strengthens the *CO₂ and *CO adsorption on the catalysts by providing columbic force and hydrogen bonds to form ultimate propane products. In comparison, the pristine Mo₃P (without *Im layer) appears to be a mediocre CO₂RR catalyst, producing significant CO and H₂ as major products. Through designing such a hybrid catalyst with ionic liquids, we open new avenues to find more achievable catalysts for CO₂RR. Overall, our quantum methods and insights open the door for technological advancements in materials to accelerate the development of renewable and green energy.

1. Z. Jiang, and A. M. Rappe, “Uncovering the Electrolyte-dependent Transport Mechanism of LiO₂ in Li-oxygen Batteries” J. Am. Chem. Soc. 2022, 144, 48, 22150-22158.

2. M. Esmaeilirad, Z. Jiang, A. M. Harzandi, A. Kondori, M. T. Saray, C. U. Segre, R. Shahbazian-Yassar, A. M. Rappe, and M. Asadi, “Imidazolium Functionalized Tri-molybdenum Phosphide for Electrosynthesis of Propane” Nat. Energy 2023, 8, 891-900.