“…The emerging hydrogen economy for sustainable energy systems has increased the demand for more efficient hydrogen production technologies. − One alternative to the prominent water splitting technologies is the paired electrolysis via cathodic hydrogen evolution and anodic organic oxidation, especially naturally available alcohols, aldehydes, and amines. − This route can not only replace the low-valued oxygen product with the value-added carboxylic acid or nitrile products but also require lower energy cost due to the higher reactivities of the organics, which together decrease the composite cost of hydrogen. ,, Nickel oxyhydroxide (NiO x (OH) 2– x , x = 1–2 depending on the oxidation state of Ni and phase structure of the pristine Ni(OH) 2 ) is one of the most active catalysts toward the electrochemical selective oxidation of these organics. − ,,,− Its low cost, facile accessibility, scalable production, and widespread use in industrial alkaline electrolyzers have promoted the research focus as the potential electrocatalyst candidate. Thus, understanding the electrocatalytic mechanism on the nickel oxyhydroxide surfaces has become utterly important for the rational design of next-generation electrocatalysts with high efficiency and selectivity for organic oxidation …”