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Mo≣Mo paddlewheel complexes bearing solubilizing groups were synthesized for their tunable physical properties relevant to energy storage applications. 

Placing cationic groups in the secondary coordination sphere of dimolybdenum paddlewheel complexes has allowed for quantification of electrostatic field effects on the MoMo quadruple bond. 

Resonant X-ray diffraction measurements were used to examine Cu site differentiation within a Cu₄S cluster that distorts its geometry to activate N₂O, thus mimicking the behavior of the biological Cu_Zactive site. 

Abstract Several renewable energy schemes aim to use the chemical bonds in abundant molecules like water and ammonia as energy reservoirs. Because the O-H and N-H bonds are quite strong (>100 kcal/mol), it is necessary to identify substances that dramatically weaken these bonds to facilitate proton-coupled electron transfer processes required for energy conversion. Usually this is accomplished through coordination-induced bond weakening by redox-active metals. However, coordination-induced bond weakening is difficult with earth’s most abundant metal, aluminum, because of its redox inertness under mild conditions. Here, we report a system that uses aluminum with a redox non-innocent ligand to achieve significant levels of coordination-induced bond weakening of O-H and N-H bonds. The multisite proton-coupled electron transfer manifold described here points to redox non-innocent ligands as a design element to open coordination-induced bond weakening chemistry to more elements in the periodic table.