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Open AccessDOI: 10.1016/S1872-5805(NCM2026-41-02-07)Original Research

The doping of coal-based activated carbon with both B and N for use as the cathode of high performance aqueous zinc-ion hybrid capacitors

LIU Shuyuan¹,TIAN Zhen¹,WANG Yanzhong¹,ZHOU Rui¹,ZHENG Zhichao¹

School of Materials Science and Engineering, North University of China, Taiyuan 030051, China

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Published In
Academic Research Journal
Published:January 15, 2025Edition:Vol 40, Issue 1 • pp. 100-112Citation:LIU Shuyuan et al. (2025), Academic Research Journal
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Key Takeaways & Executive Findings

  • • B and N co-doped coal-based activated carbon achieves a high specific capacity of 371.4 mAh g−1 at 1 A g−1 for aqueous zinc-ion capacitors. • The material retains 74% of its initial capacity after 10,000 cycles, demonstrating excellent cycling stability. • Density functional theory calculations reveal that pyridinic N is crucial for enhancing Zn2+ storage and electrochemical reversibility. • This work provides insights for designing high-capacity and ultrafast pseudocapacitive carbon cathodes for ZICs.
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Abstract

Aqueous zinc-ion capacitors (ZICs) have significant potential as energy storage systems because of their high specific capacity and superior reliability. Heteroatom-doped carbon materials were known to substantially increase the capacitance of ZICs, however the mechanism remains poorly understood. Coal-based activated carbon was functionalized with B and N to serve as the cathode material in ZICs. This modification gave the material a high specific capacity of 371.4 mAh g−1 at 1 A g−1 and it retained 74% of its initial capacity after 10 000 cycles. Experimental results and density functional theory calculations revealed that pyridinic N plays a crucial role in increasing Zn2+ storage, demonstrating superior electrochemical reversibility. This work gives valuable insight into the design of high-capacity and ultrafast pseudocapacitive carbon cathodes for ZICs.

1. Introduction

The development of sustainable, high-performance energy storage systems is important to address the uneven production and geographic distribution of primary energy sources such as solar and wind energy[1]. To address this challenge, hybrid capacitors have been developed as an advanced electrochemical energy storage system, offering high-rate capability, enhanced energy density, superior power output, and excellent cycling stability. In 2005, Fuji Heavy Industries introduced the concept of the “lithium-ion capacitors (LICs)” with the aim of achieving a synergistic effect that exceeds the sum of its individual components. The LICs consist of a prelithiated graphite anode and an activated carbon cathode[2–4]. However, the shortage of lithium metal and its flammability predicted serious economic risks and environmental problems in the long run. Consequently, researchers began exploring multivalent metal-ion hybrid capacitors based on alternative metals as a viable substitute for LICs. These alternatives include monovalent metals (e.g. Na+, K+) and multivalent metals (e.g. Mg2+, Zn2+, Ca2+, Al3+), which are abundant in the Earth’s crust and offer higher electron transfer per mole of ions. However, devices based on Mg2+, Ca2+ and Al3+ usually show poor electrochemical performance in aqueous electrolytes by generating electrochemically inert by-products passivated at the electrode surface. In contrast, zinc-ion capacitors (ZICs) have excellent reversibility, high stability[5] and high theoretical specific capacity (823 mAh g−1)[6−7]. Meanwhile, the low redox potential of Zn/Zn2+ extends the operating voltage window of the capacitor, thereby increasing energy and power density[8−9]. However, the ZICs still suffer from unsatisfactory charge storage capability and durability due to the sluggish ion-migration kinetics in carbon cathodes. Thus, the design of highly electroactive and robust carbon nanostructures is crucial for achieving superior electrochemical performance in ZICs.

Carbon-based materials have been extensively studied and utilized as cathodes for ZICs owing to numerous advantages that include low cost, environmental friendliness, and tunable structure. Among these materials, coal-based activated carbon (CAC) has garnered significant attention due to its cost-effectiveness and abundant availability. As a carbonaceous material, CAC possesses a wealth of surface functional groups, making it an excellent raw material for high-quality activated carbon[10–12].

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Cite This Research Paper
LIU Shuyuan, TIAN Zhen, WANG Yanzhong, ZHOU Rui, ZHENG Zhichao (2025). The doping of coal-based activated carbon with both B and N for use as the cathode of high performance aqueous zinc-ion hybrid capacitors. SinoTechIntel Verified Research. https://doi.org/10.1016/S1872-5805(NCM2026-41-02-07)
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Frequently Asked Questions

What is the specific capacity of the B and N co-doped coal-based activated carbon cathode?

The B and N co-doped coal-based activated carbon cathode achieves a high specific capacity of 371.4 mAh g−1 at a current density of 1 A g−1.

How does the cycling stability of this material compare?

The material retains 74% of its initial capacity after 10,000 cycles, indicating excellent long-term cycling stability.

What role does pyridinic nitrogen play in the performance?

Density functional theory calculations reveal that pyridinic N is crucial for enhancing Zn2+ storage and electrochemical reversibility, leading to superior performance.

Why are zinc-ion capacitors considered promising energy storage systems?

Zinc-ion capacitors offer high specific capacity, excellent reversibility, high stability, and a low redox potential for Zn/Zn2+, which extends the operating voltage window and increases energy and power density.

What is the significance of using coal-based activated carbon?

Coal-based activated carbon is cost-effective, abundant, and possesses a wealth of surface functional groups, making it an excellent raw material for high-quality activated carbon cathodes.

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