The conversion of metal-organic frameworks (MOFs) into inorganic nanomaterials is considered as an attractive means to produce highly efficient electrocatalysts for alternative-energy related applications. Yet, traditionally employed MOF-conversion conditions (e.g., pyrolysis) commonly involve multiple complex high-temperature reaction processes, which often make it challenging to control the composition, pore structure, and active-sites of the MOF-derived catalysts. Herein, a general, simple, room-temperature method is presented for a controlled electrochemical conversion of MOF (EC-MOF) films into porous, amorphous metal sulfides (a-MS x ). Detailed X-ray photoelectron spectroscopy analysis and control over independent EC-MOF parameters (e.g., scan-rate and potential window) enable to gain insights on the MOFconversion mechanisms, and in turn to fine-tune the porosity and composition of the obtained MS x . As a result, a highly active amorphous cobalt sulfide (a-CoS x ) electrocatalyst can be designed for hydrogen evolution reaction in neutral pH. Furthermore, the adjustable nature of the EC-MOF method allows to draw conclusions about the correlation between the concentration of catalytically active species (S 2 2sites) and the hydrogen evolution properties of the a-CoS x . Given the method's generality and the diversity of available MOF structures, EC-MOF provides a compelling platform for a rational design of a wide variety of active electrocatalytic materials.

Hydrazine is a promising energy-dense fuel for alkaline fuel cells. To design efficient and affordable electrocatalysts for the hydrazine oxidation reaction (HzOR), one needs to control both the active site and the supporting scaffold. We now report a family of electrocatalysts for alkaline HzOR, consisting of atomically dispersed FeÀ N 4 sites (as iron corroles of varying sizes) on hierarchically porous, electronically conductive carbon scaffolds that were prepared by self-templating from a novel barium-based precursor. The orthogonal design of active sites and flow-enhancing scaffolds allowed the rational optimization of their combination, to achieve excellent HzOR activity. These catalysts demonstrate the utility and versatility of metallocorroles for electrocatalysis in the nitrogen cycle, as well as the importance of pore tuning for optimization of the current density.

In article number https://doi.org/10.1002/adfm.201707244, Idan Hod and co‐workers report a method for electrochemical conversion of metal‐organic frameworks (EC‐MOF) as a general strategy for preparing amorphous metal‐sulfide (a‐MSx) electrocatalysts. The adjustable nature of the EC‐MOF method enables to unveil the MOF‐conversion mechanisms and fine‐tune the catalytic activity of the resulting a‐MSx. Consequently, EC‐MOF provides a powerful platform for designing a wide variety of active electrocatalysts.