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Supercritical Nitrogen Processing for the Purification of Reactive Porous Materials

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History Matters in Solid-State Hydrogen Storage: Hidden State Variables and Pathway-Dependent Reactivity in Mg-Based

Chen Chen¹, Quanhui Hou², Liangjuan Gao³

¹Department of Mechanics, Jinzhong University, Jinzhong 030606, China.

Molecules (Basel, Switzerland)

|June 12, 2026

Summary

Magnesium-based hydrides for hydrogen storage are not fully defined by composition. Their reactivity depends on historical processing, creating hidden states that influence hydrogen sorption pathways and explain reproducibility issues.

Keywords:

catalyst state hidden state variables hydrogen sorption mechanism interface engineering magnesium hydride metastability pathway-dependent reactivity solid-state hydrogen storage

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Area of Science:

Materials Science
Chemical Engineering
Energy Storage

Background:

Magnesium-based hydrides are promising for solid-state hydrogen storage due to high capacity and low cost.
Practical performance of these materials varies significantly, defying simple compositional explanations.
Discrepancies in activation, kinetics, and capacity are common despite similar chemical labels.

Purpose of the Study:

To reframe the understanding of magnesium-based hydride reactivity from a composition-centered to a pathway-centered perspective.
To explain the observed variability in material performance by considering 'hidden state variables' introduced during synthesis and cycling.
To propose a new framework for materials development that accounts for historical processing and reaction pathways.

Main Methods:

Review of existing literature on magnesium-based hydrides and hydrogen storage.
Analysis of how synthesis, activation, and cycling history influence material properties.
Conceptual framework development linking material history to hydrogen sorption pathways.

Main Results:

Material behavior is critically dependent on historical states (defects, strain, interfaces, catalyst state) not captured by composition alone.
Metastability acts as a bridge, allowing historical variables to influence reactions.
Hydrogen sorption is pathway-dependent, with history dictating entry, transport, and interface mechanisms.

Conclusions:

The reproducibility problem in magnesium hydride research stems from comparing materials with different historical reactive states (pathway mismatch).
A pathway-aware design framework, considering metadata and boundaries, is essential for cumulative progress.
Future advancements require not only optimized compositions but also well-defined, controlled, and preserved reactive pathways.