In-situ evolution process understanding from a salan-ligated manganese cluster to supercapacitive application

The goal of material chemistry is to study the relationship among hierarchical structure, chemical reaction and precision preparation for materials, yet tracking pyrolysis process on multi-dimensional scale is still at primary stage. Here we propose packing mode analysis to understand evolution process in high temperature reaction. As a proof of concept, we first design a salan-ligated Mn₃ (Mn₃(3-MeOsalophen)₂(Cl)₂) cluster and pyrolyze it under an inert atmosphere directly to a mixed valence MnO_x embedded in a porous N-doped carbon skeleton (MnO_x/C). Meanwhile, combining thermogravimetry-mass spectrometry (TG-MS) with other characterization techniques, its pyrolysis process is precisely tracked real-time and Mn²⁺/Mn³⁺ ratios in the resulting materials are deduced, ensuring excellent electrochemical advantages. As a result, the as-preferred MnO_x/C-900 sample reaches 943 F/g at 1 A/g, maintaining good durability under 5, 000 cycles with 90% retention. The highlight of packing mode analysis strategy in this work would provide a favorable approach to explore the potential relationship between structure and performance in the future.