TY - JOUR
T1 - Supermolecule-mediated defect engineering of porous carbons for zinc-ion hybrid capacitors
AU - Zhang, Wenli
AU - Yin, Jian
AU - Jian, Wenbin
AU - Wu, Ying
AU - Chen, Liheng
AU - Sun, Minglei
AU - Schwingenschlögl, Udo
AU - Qiu, Xueqing
AU - Alshareef, Husam N.
N1 - KAUST Repository Item: Exported on 2022-10-17
Acknowledgements: The authors acknowledge the financial support from the National Natural Science Foundation of China (22108044), the Research and Development Program in Key Fields of Guangdong Province (2020B1111380002), the Guangdong Basic and Applied Basic Research Foundation (2019A1515011512, 2021A1515010172), the Basic Research and Applicable Basic Research in Guangzhou City (202201010290), the Guangdong Provincial Key Laboratory of Plant Resources Biorefinery (2021GDKLPRB07), and King Abdullah University of Science and Technology (KAUST), Saudi Arabia. We acknowledge the help of Dr. Chunjie Cao from Carl Zeiss (Shanghai) for the X-ray micro Computed Tomography analysis.
PY - 2022/9/23
Y1 - 2022/9/23
N2 - Zinc ion hybrid capacitors hold great potential for future energy storage that requires both high energy density and high power capability. However, the charge storage mechanism of porous carbon cathode is ambiguous in Zn2+ ion-containing aqueous solutions, albeit porous carbon usually stores charge by electric double-layer capacitance. Herein, we developed a supermolecule-mediated direct pyrolysis carbonization strategy to convert sustainable sodium lignosulfonate resources into three-dimensional highly heteroatom-doped porous carbons with large mesopores. Through this strategy, we obtained lignin-derived porous carbons with high heteroatom dopings (14.9 at% nitrogen and 4.7 at% oxygen) and relatively high specific surface areas. Furthermore, the nitrogen doping configurations were mainly edge-nitrogen dopants even under high pyrolysis temperatures (> 900 °C). Lignin-derived nitrogen-doped porous carbon showed a high gravimetric specific capacitance of 266 F g−1 with high rate capability, which is endowed by the increased surface pseudocapacitance. First-principles calculations and molecular dynamics simulations indicate that the edge nitrogen and oxygen dopants contribute to the reversible adsorption/desorption of zinc ions and protons. Pores size less than 6.8 Å can cause a significant diffusion energy barrier for the hydrated zinc ions, thus degrading the capacitance and rate capability.
AB - Zinc ion hybrid capacitors hold great potential for future energy storage that requires both high energy density and high power capability. However, the charge storage mechanism of porous carbon cathode is ambiguous in Zn2+ ion-containing aqueous solutions, albeit porous carbon usually stores charge by electric double-layer capacitance. Herein, we developed a supermolecule-mediated direct pyrolysis carbonization strategy to convert sustainable sodium lignosulfonate resources into three-dimensional highly heteroatom-doped porous carbons with large mesopores. Through this strategy, we obtained lignin-derived porous carbons with high heteroatom dopings (14.9 at% nitrogen and 4.7 at% oxygen) and relatively high specific surface areas. Furthermore, the nitrogen doping configurations were mainly edge-nitrogen dopants even under high pyrolysis temperatures (> 900 °C). Lignin-derived nitrogen-doped porous carbon showed a high gravimetric specific capacitance of 266 F g−1 with high rate capability, which is endowed by the increased surface pseudocapacitance. First-principles calculations and molecular dynamics simulations indicate that the edge nitrogen and oxygen dopants contribute to the reversible adsorption/desorption of zinc ions and protons. Pores size less than 6.8 Å can cause a significant diffusion energy barrier for the hydrated zinc ions, thus degrading the capacitance and rate capability.
UR - http://hdl.handle.net/10754/683053
UR - https://linkinghub.elsevier.com/retrieve/pii/S2211285522009041
UR - http://www.scopus.com/inward/record.url?scp=85139276682&partnerID=8YFLogxK
U2 - 10.1016/j.nanoen.2022.107827
DO - 10.1016/j.nanoen.2022.107827
M3 - Article
SN - 2211-2855
VL - 103
SP - 107827
JO - Nano Energy
JF - Nano Energy
ER -