Ternary MOF-Based Redox Active Sites Enabled 3D-on-2D Nanoarchitectured Battery-Type Electrodes for High-Energy-Density

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Cite as Nano-Micro Lett. (2021) 13:17 Received: 11 June 2020 Accepted: 21 August 2020 © The Author(s) 2020

https://doi.org/10.1007/s40820-020-00528-9

Ternary MOF‑Based Redox Active Sites Enabled 3D‑on‑2D Nanoarchitectured Battery‑Type Electrodes for High‑Energy‑Density Supercapatteries Goli Nagaraju1,2, S. Chandra Sekhar1, Bhimanaboina Ramulu1, Sk. Khaja Hussain1,2, D. Narsimulu1, Jae Su Yu1 *

HIGHLIGHTS  • Redox chemistry enabled Ni–Co–Mn (NCM)-based MOF nanoarchitectures are used as battery-type electrodes. • The NCM-based MOFs demonstrate high areal capacity and good cycling stability. • The fabricated hybrid supercapattery showed high energy and power densities of 1.21 mWh cm−2 and 32.49 mW cm−2, respectively. ABSTRACT  Designing rationally combined metal–organic frameworks (MOFs) with multifunctional nanogeometries is of significant

Dual layered Ni-Co-Mn-based MOF

Ni foam N-O AC

research interest to enable the electrochemical properties in advanced energy storage devices. Herein, we explored a new class of binder-

(−)

Separator

free dual-layered Ni–Co–Mn-based MOFs (NCM-based MOFs) with three-dimensional (3D)-on-2D nanoarchitectures through a polarityinduced solution-phase method for high-performance supercapatteries. The hierarchical NCM-based MOFs having grown on nickel foam

KOH

exhibit a battery-type charge storage mechanism with superior areal

(+) Supercapattery

capacity (1311.4 μAh c­ m−2 at 5 mA cm−2), good rate capability (61.8%; 811.67 μAh c­ m−2 at 50 mA cm−2), and an excellent cycling durability. The superior charge storage properties are ascribed to the synergistic features, higher accessible active sites of dual-layered nanogeometries, and exalted redox chemistry of multi metallic guest species, respectively. The bilayered NCM-based MOFs are further employed as a battery-type electrode for the fabrication of supercapattery paradigm with biomass-derived nitrogen/oxygen doped porous carbon as a negative electrode, which demonstrates excellent capacity of 1.6 mAh ­cm−2 along with high energy and power densities of

1.21 mWh ­cm−2 and 32.49 mW ­cm−2, respectively. Following, the MOF-based supercapattery was further assembled with a renewable solar power harvester to use as a self-charging station for various portable electronic applications. KEYWORDS  Metal–organic frameworks; Dual layers; Redox chemistry; Supercapattery; Renewable energy

* Jae Su Yu, [email protected] 1 Institute for Wearable Convergence Electronics, Department of Electronic Engineering, Kyung Hee University, 1732 Deogyeong‑daero, Gihung‑gu, Yongin‑si, Gyeonggi‑do 17104, Republic of Korea 2 Department of Chemical Engineering, College of Engineering, Kyung Hee University, 1732 Deogyeong‑daero, Gihung‑gu, Yongin‑si, Gyeonggi‑do 17104, Republic of Korea Vol.:(0123456789)

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1 Introduction With the rapid growth of environmental issues, deteriorative fossil fuels and increasing energy demands, finding efficient methods to harvest intermittent natured renewable energy has greatly accelerated the de