Herein, we present Metal‐Organic Gel intercalated with chitosan, a “green” precursor for the synthesis of intrinsic N‐doped Fe entrenched (CHI‐TMA−Fe‐CW) and Fe distributed mesoporous graphitic carbon structures (CHI‐TMA−Fe‐CW−M1) with appreciable Oxygen Reduction Reaction (ORR) activity in alkaline medium. Modulation of the synthetic protocol as a function of reaction kinetics and gelation time while maintaining identical pyrolysis conditions (900 °C, flowing N2 atmosphere) improves the microstructure, surface area and Fe distribution of the graphitic structures (CHI‐TMA−Fe‐CW−M1). CHI‐TMA−Fe‐CW has a Fe entrenched graphitic nanocapsule like morphology while Fe distributed mesoporous graphitic carbon sheets, with a specific surface area value of 565 m2g−1 obtained by modulating the synthesis chemistry in CHI‐TMA−Fe‐CW−M1. The higher percentage of graphitic N in CHI‐TMA−Fe‐CW−M1 apparent from the XPS data validate that the modified synthetic method favours creation of more graphitic N sites contributing for better catalytic performance. CHI‐TMA‐Fe‐CW−M1 catalyst exhibited comparable electrocatalytic activity with that of the commercially available Pt/C via an efficient four‐electron‐dominant ORR pathway with a positive onset potential value of 0.925 V vs RHE. Good durability of CHI‐TMA−Fe‐CW−M1 after 5000 cycles further confirm the prospects of MOG‐chitosan and the feasibility to be used as a potential catalyst for ORR.
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