Compositional interplay of two different cobalt phosphates (Co(H2PO4)2; Co‐DP and Co(PO3)2; Co‐MP) loaded on morphologically engineered high surface area nanocarbon leads to an increased electrocatalytic efficiency for oxygen evolution reaction (OER) in near neutral conditions. This is reflected as significant reduction in the onset overpotential (301 mV) and enhanced current density (30 mA cm−2 @ 577 mV). In order to achieve uniform surface loading, organic‐soluble thermolabile cobalt‐bis(di‐tert‐butylphosphate) is synthesized in situ inside the nanocarbon matrix and subsequently pyrolyzed at 150 °C to produce Co(H2PO4)2/Co(PO3)2 (80:20 wt%). Annealing this sample at 200 or 250 °C results in the redistribution of the two phosphate systems to 55:45 or 20:80 (wt%), respectively. Detailed electrochemical measurements clearly establish that the 55:45 (wt%) sample prepared at 200 °C performs the best as a catalyst, owing to a relay mechanism that enhances the kinetics of the 4e− transfer OER process, which is substantiated by micro‐Raman spectroscopic studies. It is also unraveled that the engineered nanocarbon support simultaneously enhances the interfacial charge‐transfer pathway, resulting in the reduction of onset overpotential, compared to earlier investigated cobalt phosphate systems.

Controlled grafting of polyaniline from the surface of carbon nano dots using ‘grafting from’ strategy is reported. The nano structured polyaniline coated carbon nano dots produced show excellent electrochemical performance.

Here we present the synthesis of poly(acryloyl hydrazide), a versatile scaffold for the preparation of functional polymers, and its post-polymerisation modification using a wide range of conditions.

Mechanistic insights from operando Raman spectroelectrochemistry establishes that synergistic support–catalyst interactions is vital for rational design of electrocatalytic systems to achieve efficient hydrogen generation in alkaline medium.

Manipulating heterogeneous electrified interfaces with an external magnetic field (H ext) explicitly mandates the constant presence of H ext for achieving magnetoelectrocatalytic kinetic enhancements. Here, we demonstrate the highest kinetic enhancement of 650% in electrocatalytic hydrogen evolution reaction (HER), without the mandatory presence of H ext. A synergistic interface created in nanostructured hard carbon florets (NCF) decorated with ferro–paramagnetic nanoparticles (Co3O4, Co, and Ni–Co) is demonstrated to be critical for both (a) prominent enhancement in HER-kinetics when H ext = 200 mT and (b) sustaining the rapid HER when H ext = 0 mT. Significant lowering of magnetoresistance (22%) and magnetocharge-transfer resistance (84.8%) using a weak H ext = 100 mT leads to a 2.5-fold volumetric increment in hydrogen generation driven by 7% enhancement in electrokinetic activity. Furthermore, all such enhancements are strongly correlated with the magnetic coercivity of the catalyst, implying the role of interfacial mechanistic modulation of the HER by H ext. Additionally, microscopic dimensional enlargement of the structurally flexible NCF promotes such a long-term effect leading to larger magnetocurrent as compared to other carbon-based supports. Our work demonstrates the importance of spin polarization in magnetically active electrocatalytic interfaces and thereby offers a general practical strategy for energy-efficient hydrogen production.