Unleashing the Power of Capacitive Deionization:  Advancing Ion Removal with Biomass-Derived Porous Carbonaceous Electrodes

Hai Deng; Ziquan Wang; Minjun Kim; Yusuke Yamauchi; Stephen J. Eichhorn; Maria-Magdalena Titirici; Libo Deng

doi:10.1016/j.nanoen.2023.108914

Unleashing the Power of Capacitive Deionization: Advancing Ion Removal with Biomass-Derived Porous Carbonaceous Electrodes

Hai Deng
, Ziquan Wang
, Minjun Kim
, Yusuke Yamauchi
, Stephen J. Eichhorn
, Maria-Magdalena Titirici
, Libo Deng

Research output: Contribution to journal › Article (Academic Journal) › peer-review

102 Citations (Scopus)

Abstract

Capacitive deionization (CDI) is a promising electrochemical technique for removal and recycling of ions from micro-polluted wastewater but is still hindered by the co-ion expulsion effect and anode oxidation. In this study, these issues are addressed through optimization of both materials and electrochemical systems. A diverse set of porous carbons are prepared using biomass as precursor and KOH as the activation agent. It is found that direct carbonization and/or KOH activation induce a negative surface charge, whereas intense nitrogen-doping results in an inverse surface charge for all biomass-carbons, characterized by the potential of zero charge (Epzc). Density functional theory calculations suggest that the carboxyl group and quaternary N contribute most among other functional groups to the negative and positive charges, respectively. An Epzc-matching asymmetric CDI system is constructed employing negatively charged and positively charged carbons as the cathode and anode, respectively. This configuration, coupled with precise optimization of the cathode-to-anode mass ratio (m-/m+), unlock a high adsorption capacity of 17.2mgg-1 for NaCl, surpassing the symmetric system by 84.7%. A further fine tuning of the m-/m+ ratio results in a removal capacity of 167.4mgg-1 for Cu2+ ions, which is the highest reported for carbonaceous materials to date.

Original language	English
Article number	108914
Journal	Nano Energy
Volume	117
Early online date	16 Sept 2023
DOIs	https://doi.org/10.1016/j.nanoen.2023.108914
Publication status	E-pub ahead of print - 16 Sept 2023

Bibliographical note

Funding Information:
This work was supported by the Natural Science Foundation of Guangdong ( 2023A1515012267 ), the National Natural Science Foundation of China ( 22178223 ), the Royal Society/NSFC Cost Share Program ( IEC\NSFC\223372 ), the JST-ERATO Yamauchi Materials Space-Tectonics Project ( JPMJER2003 ) and the Australian Research Council ( ARC ) through a Linkage Project ( LP180100429 ). This work used the Queensland node of the NCRIS-enabled Australian National Fabrication Facility (ANFF). The authors would like to thank Suzhou Deyo Bot Advanced Materials Co., Ltd. for providing support for material characterization. S.J.E. is supported by the Engineering and Physical Sciences Research Council (Grant no. EP/V002651/1 ).

Funding Information:
This work was supported by the Natural Science Foundation of Guangdong (2023A1515012267), the National Natural Science Foundation of China (22178223), the Royal Society/NSFC Cost Share Program (IEC\NSFC\223372), the JST-ERATO Yamauchi Materials Space-Tectonics Project (JPMJER2003) and the Australian Research Council (ARC) through a Linkage Project (LP180100429). This work used the Queensland node of the NCRIS-enabled Australian National Fabrication Facility (ANFF). The authors would like to thank Suzhou Deyo Bot Advanced Materials Co. Ltd. for providing support for material characterization. S.J.E. is supported by the Engineering and Physical Sciences Research Council (Grant no. EP/V002651/1).

Publisher Copyright:
© 2023 Elsevier Ltd

Keywords

Capacitive deionization
Porous carbon
Surface charge
Mass ratio

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Cite this

@article{dff9f42dfa7048ec8adb0fa64ec261c8,

title = "Unleashing the Power of Capacitive Deionization: Advancing Ion Removal with Biomass-Derived Porous Carbonaceous Electrodes",

abstract = "Capacitive deionization (CDI) is a promising electrochemical technique for removal and recycling of ions from micro-polluted wastewater but is still hindered by the co-ion expulsion effect and anode oxidation. In this study, these issues are addressed through optimization of both materials and electrochemical systems. A diverse set of porous carbons are prepared using biomass as precursor and KOH as the activation agent. It is found that direct carbonization and/or KOH activation induce a negative surface charge, whereas intense nitrogen-doping results in an inverse surface charge for all biomass-carbons, characterized by the potential of zero charge (Epzc). Density functional theory calculations suggest that the carboxyl group and quaternary N contribute most among other functional groups to the negative and positive charges, respectively. An Epzc-matching asymmetric CDI system is constructed employing negatively charged and positively charged carbons as the cathode and anode, respectively. This configuration, coupled with precise optimization of the cathode-to-anode mass ratio (m-/m+), unlock a high adsorption capacity of 17.2mgg-1 for NaCl, surpassing the symmetric system by 84.7\%. A further fine tuning of the m-/m+ ratio results in a removal capacity of 167.4mgg-1 for Cu2+ ions, which is the highest reported for carbonaceous materials to date.",

keywords = "Capacitive deionization, Porous carbon, Surface charge, Mass ratio",

author = "Hai Deng and Ziquan Wang and Minjun Kim and Yusuke Yamauchi and Eichhorn, \{Stephen J.\} and Maria-Magdalena Titirici and Libo Deng",

note = "Funding Information: This work was supported by the Natural Science Foundation of Guangdong ( 2023A1515012267 ), the National Natural Science Foundation of China ( 22178223 ), the Royal Society/NSFC Cost Share Program ( IEC\textbackslash{}NSFC\textbackslash{}223372 ), the JST-ERATO Yamauchi Materials Space-Tectonics Project ( JPMJER2003 ) and the Australian Research Council ( ARC ) through a Linkage Project ( LP180100429 ). This work used the Queensland node of the NCRIS-enabled Australian National Fabrication Facility (ANFF). The authors would like to thank Suzhou Deyo Bot Advanced Materials Co., Ltd. for providing support for material characterization. S.J.E. is supported by the Engineering and Physical Sciences Research Council (Grant no. EP/V002651/1 ). Funding Information: This work was supported by the Natural Science Foundation of Guangdong (2023A1515012267), the National Natural Science Foundation of China (22178223), the Royal Society/NSFC Cost Share Program (IEC\textbackslash{}NSFC\textbackslash{}223372), the JST-ERATO Yamauchi Materials Space-Tectonics Project (JPMJER2003) and the Australian Research Council (ARC) through a Linkage Project (LP180100429). This work used the Queensland node of the NCRIS-enabled Australian National Fabrication Facility (ANFF). The authors would like to thank Suzhou Deyo Bot Advanced Materials Co. Ltd. for providing support for material characterization. S.J.E. is supported by the Engineering and Physical Sciences Research Council (Grant no. EP/V002651/1). Publisher Copyright: {\textcopyright} 2023 Elsevier Ltd",

year = "2023",

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doi = "10.1016/j.nanoen.2023.108914",

language = "English",

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T1 - Unleashing the Power of Capacitive Deionization

T2 - Advancing Ion Removal with Biomass-Derived Porous Carbonaceous Electrodes

AU - Deng, Hai

AU - Wang, Ziquan

AU - Kim, Minjun

AU - Yamauchi, Yusuke

AU - Eichhorn, Stephen J.

AU - Titirici, Maria-Magdalena

AU - Deng, Libo

N1 - Funding Information: This work was supported by the Natural Science Foundation of Guangdong ( 2023A1515012267 ), the National Natural Science Foundation of China ( 22178223 ), the Royal Society/NSFC Cost Share Program ( IEC\NSFC\223372 ), the JST-ERATO Yamauchi Materials Space-Tectonics Project ( JPMJER2003 ) and the Australian Research Council ( ARC ) through a Linkage Project ( LP180100429 ). This work used the Queensland node of the NCRIS-enabled Australian National Fabrication Facility (ANFF). The authors would like to thank Suzhou Deyo Bot Advanced Materials Co., Ltd. for providing support for material characterization. S.J.E. is supported by the Engineering and Physical Sciences Research Council (Grant no. EP/V002651/1 ). Funding Information: This work was supported by the Natural Science Foundation of Guangdong (2023A1515012267), the National Natural Science Foundation of China (22178223), the Royal Society/NSFC Cost Share Program (IEC\NSFC\223372), the JST-ERATO Yamauchi Materials Space-Tectonics Project (JPMJER2003) and the Australian Research Council (ARC) through a Linkage Project (LP180100429). This work used the Queensland node of the NCRIS-enabled Australian National Fabrication Facility (ANFF). The authors would like to thank Suzhou Deyo Bot Advanced Materials Co. Ltd. for providing support for material characterization. S.J.E. is supported by the Engineering and Physical Sciences Research Council (Grant no. EP/V002651/1). Publisher Copyright: © 2023 Elsevier Ltd

PY - 2023/9/16

Y1 - 2023/9/16

N2 - Capacitive deionization (CDI) is a promising electrochemical technique for removal and recycling of ions from micro-polluted wastewater but is still hindered by the co-ion expulsion effect and anode oxidation. In this study, these issues are addressed through optimization of both materials and electrochemical systems. A diverse set of porous carbons are prepared using biomass as precursor and KOH as the activation agent. It is found that direct carbonization and/or KOH activation induce a negative surface charge, whereas intense nitrogen-doping results in an inverse surface charge for all biomass-carbons, characterized by the potential of zero charge (Epzc). Density functional theory calculations suggest that the carboxyl group and quaternary N contribute most among other functional groups to the negative and positive charges, respectively. An Epzc-matching asymmetric CDI system is constructed employing negatively charged and positively charged carbons as the cathode and anode, respectively. This configuration, coupled with precise optimization of the cathode-to-anode mass ratio (m-/m+), unlock a high adsorption capacity of 17.2mgg-1 for NaCl, surpassing the symmetric system by 84.7%. A further fine tuning of the m-/m+ ratio results in a removal capacity of 167.4mgg-1 for Cu2+ ions, which is the highest reported for carbonaceous materials to date.

AB - Capacitive deionization (CDI) is a promising electrochemical technique for removal and recycling of ions from micro-polluted wastewater but is still hindered by the co-ion expulsion effect and anode oxidation. In this study, these issues are addressed through optimization of both materials and electrochemical systems. A diverse set of porous carbons are prepared using biomass as precursor and KOH as the activation agent. It is found that direct carbonization and/or KOH activation induce a negative surface charge, whereas intense nitrogen-doping results in an inverse surface charge for all biomass-carbons, characterized by the potential of zero charge (Epzc). Density functional theory calculations suggest that the carboxyl group and quaternary N contribute most among other functional groups to the negative and positive charges, respectively. An Epzc-matching asymmetric CDI system is constructed employing negatively charged and positively charged carbons as the cathode and anode, respectively. This configuration, coupled with precise optimization of the cathode-to-anode mass ratio (m-/m+), unlock a high adsorption capacity of 17.2mgg-1 for NaCl, surpassing the symmetric system by 84.7%. A further fine tuning of the m-/m+ ratio results in a removal capacity of 167.4mgg-1 for Cu2+ ions, which is the highest reported for carbonaceous materials to date.

KW - Capacitive deionization

KW - Porous carbon

KW - Surface charge

KW - Mass ratio

U2 - 10.1016/j.nanoen.2023.108914

DO - 10.1016/j.nanoen.2023.108914

M3 - Article (Academic Journal)

SN - 2211-2855

VL - 117

JO - Nano Energy

JF - Nano Energy

M1 - 108914

ER -