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Vol. 17 (2025)

Gradient-Layered MXene/Hollow Lignin Nanospheres Architecture Design for Flexible and Stretchable Supercapacitors

https://doi.org/10.1007/s40820-024-01512-3
Haonan Zhang
Jiangsu Provincial Key Lab of Sustainable Pulp and Paper Technology and Biomass Materials, NanJing Forestry University, Nanjing 210037, People’s Republic of China
Cheng Hao
Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street, Toronto, ON M5S 3E5, Canada
Tongtong Fu
Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street, Toronto, ON M5S 3E5, Canada
Dian Yu
Department of Materials Science and Engineering, University of Toronto, 184 College Street, Toronto, ON M5S 3E4, Canada
Jane Howe
Department of Materials Science and Engineering, University of Toronto, 184 College Street, Toronto, ON M5S 3E4, Canada
Kaiwen Chen
College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, People’s Republic of China
Ning Yan
Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street, Toronto, ON M5S 3E5, Canada
Hao Ren
Jiangsu Provincial Key Lab of Sustainable Pulp and Paper Technology and Biomass Materials, NanJing Forestry University, Nanjing 210037, People’s Republic of China
Huamin Zhai
Jiangsu Provincial Key Lab of Sustainable Pulp and Paper Technology and Biomass Materials, NanJing Forestry University, Nanjing 210037, People’s Republic of China

Corresponding Author: Hao Ren

renhao@njfu.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 43

Abstract

With the rapid development of flexible wearable electronics, the demand for stretchable energy storage devices has surged. In this work, a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres (HLNPs)-intercalated two-dimensional transition metal carbide (Ti3C2Tx MXene) for fabricating highly stretchable and durable supercapacitors. By depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient, a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene lamella. Moreover, the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility, thus better utilizing the pseudocapacitive property of lignin. All these strategies effectively enhanced the capacitive performance of the electrodes. In addition, HLNPs, which acted as a protective phase for MXene layer, enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the electrodes. Flexible electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600% uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm−2 (241 F g−1) and 514 mF cm−2 (95 F g−1), respectively. Moreover, their capacitances were well preserved after 1000 times of 600% stretch-release cycling. This study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.


Highlights:
1 A novel gradient-layered architecture based on single-pore hollow lignin nanospheres (HLNPs)-intercalated MXene layers was created to fabricate highly stretchable (600%) and durable (1000 cycling) supercapacitor electrodes.
2 The architecture reduced the overstacking of MXene, and the micro-chamber structure of HLNPs better utilized lignin’s pseudocapacitive property to improve ion and electron accessibility (specific capacitance reached 1273 mF cm−2).
3 HLNPs enhanced mechanical durability and capacitive stability of the integrated wrinkled electrodes during the stretch-release cycling.

Keywords

Hollow lignin nanospheres MXene Gradient-layered architecture Wrinkled electrodes Stretchable supercapacitors
Zhang, Haonan, Cheng Hao, Tongtong Fu, Dian Yu, Jane Howe, Kaiwen Chen, Ning Yan, Hao Ren, and Huamin Zhai. 2024. “Gradient-Layered MXene/Hollow Lignin Nanospheres Architecture Design for Flexible and Stretchable Supercapacitors”. Nano-Micro Letters 17 (October):43. https://doi.org/10.1007/s40820-024-01512-3.
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