Otun, Kabir OpeyemiDiop, Ndeye FatouMaphiri, Vusani MuswaFasakin, OladepoKitenge, Vianney NgoyiThior, SouleymaneManyala, Ncholu I.2026-01-222026-01-222025-05-05Otun, K.O., Diop, N.F., Maphiri, V.M. et al. 2025, 'Nanoarchitectonics with redox active site modulation in bimetallic MIL-125 (Ti, Mn) MOF for enhanced supercapacitor performance', Journal of Alloys and Compounds, vol. 1029, art. 180753, pp. 1-15. https://doi.org/10.1016/j.jallcom.2025.180753.0925-8388 (print)1873-4669 (online)10.1016/j.jallcom.2025.180753http://hdl.handle.net/2263/107483Metal-organic frameworks (MOFs) with dual metal centres have received considerable attention as electrode materials for supercapacitor applications due to their redox-active sites and unique structural architecture. Herein, we present a simple one-step solvothermal approach to synthesize and optimize bimetallic MIL-125(Ti,Mn) MOF, where redox active site modulation enhances its electrochemical performance in asymmetric supercapacitors. The unique structure of MIL-125(Ti,Mn), featuring a spindle-like morphology anchored by flake-like sheets, facilitates interaction between active sites and electrolyte ions and modulates the redox active sites, leading to improved electrochemical performance. As such, the optimized MIL-125(Ti)-Mn-2 electrode demonstrates a high specific capacity of 137.2 mAhg−1 at 1 A g–1 and a capacity retention of more than 76.3 % after 5000 cycles. Furthermore, an asymmetric supercapacitor built with Mn-MIL-125(Ti)-2 and activated carbon achieved a high specific energy of 22.74 Wh kg–1 at a specific power of 996 W kg–1, while also demonstrating excellent stability with 71.2 % capacitance retention over 10,000 cycles at 10 Ag−1. This one-pot incorporation strategy offers a novel route to modulate the structure of MIL-125(Ti) via Mn2+ doping for enhanced supercapacitor performance.en© 2025 The Authors. This work is licensed under the Creative Commons Attribution License.MIL-125(Ti)Bimetallic MOFsAsymmetric deviceSupercapacitorsMetal-organic framework (MOF)Article