Key Takeaways & Executive Findings
- •• Defect-rich nanocarbon catalyst (CoSA/CoNP-NSDNC) synthesized using NSCo single atoms and Co nanoparticle clusters on fullerene-derived carbon framework, enabling efficient H2O2 electrosynthesis. • The CoSA/CoNP-NSDNC catalyst exhibits high H2O2 selectivity (~90%) over a wide potential range with an onset potential of 0.72 V versus RHE, achieving Faraday efficiency close to 95% in acidic conditions. • Demonstrates potential for environmental applications, achieving high H2O2 production (4206.96 mmol g−1 h−1) in a flow cell setup, along with efficient degradation of organic pollutants in Fenton-like reactions. • Synergistic effect of non-noble metal nanoparticles, single-atom sites, and topological defects provides a new direction for designing carbon-based catalysts for efficient H2O2 electrosynthesis.
Abstract
Non-noble-based single atomic catalysts have exhibited significant potential in electrochemical production of H2O2 via two-electron oxygen reduction reactions (2e− ORR). However, constructing highly efficient and acid-resistant catalysts remains a challenge but significant. In this work, fullerene (C60) with abundant pentagonal inherent defects was employed as a carbon substrate to synthesize defect-rich nanocarbon electrocatalysts doped with NSCo single atoms and accompanied by metallic Co nanoparticles (CoSA/CoNP-NSDNC) for the first time. The electrochemical experiments demonstrate that the active sites of CoSA/CoNP-NSDNC are formed through the synergistic interaction between NSCo single atoms and Co nanoparticle clusters embedded within the carbon framework. The obtained CoSA/CoNP-NSDNC catalyst exhibits an onset potential as 0.72 V versus RHE and achieves up to 90% H2O2 selectivity over a wide potential range of 500 mV. Moreover, the as-obtained CoSA/CoNP-NSDNC configured as the cathode in a self-assembled flow cell under acidic conditions achieves a high H2O2 production rate of 4206.96 mmol gcat⁻1 h⁻1 with a Faraday efficiency of ∼ 95% and exhibit ultra fast degradation of organic pollutants. This work focuses on the synergistic effect of non-noble metal nanoparticles, metal single-atom sites, and topological defects on the 2e− ORR process, which provides a new direction for designing carbon-based catalysts for efficient H2O2 electrosynthesis.
1. Introduction
Hydrogen peroxide (H2O2) plays a vital role in various industries, particularly in environmental protection and sustainable development. Currently, over 98% of H2O2 is synthesized through the anthraquinone process, which is energy-intensive and generates significant organic waste [1, 2]. Additionally, the concentration of industrially produced H2O2 must be increased to 70 wt% to reduce storage and transportation costs. However, H2O2’s propensity to decompose easily introduces potential safety risks during these processes [3–6]. Therefore, the advancement of energy-saving, green, safe, and efficient H2O2 synthesis methods is of importance. Electrochemical oxygen reduction offers low energy consumption and produces clean, pollution-free products, making it a highly promising method for H2O2 production, which has attracted significant research attention [7–10]. The development of efficient two-electron (2e−) electrocatalysts is essential for advancing this technology. However, despite considerable progress in alkaline conditions, many electrocatalysts still exhibit limited selectivity and H2O2 yield under acidic conditions.
Noble metal catalysts (e.g., Pt, Au) have shown exceptional performance in H2O2 production [10–12]. However, these noble metals are costly and gradually lose activity due to continuous corrosion in acidic electrolytes, presenting a significant challenge for their sustainable use in catalytic applications [13, 14]. Fullerene (C60) is a novel carbon material with inherent pentagonal topological defects, which endows it with high electron affinity and excellent electron transfer capability. Mu et al. demonstrated that alkali etching of C60 can produce pentagon-rich carbon materials, which exhibit excellent electrochemical properties, highlighting the advantages of fullerenes in the oxygen reduction reactions (ORR) field [15]. Therefore, fullerene-based catalysts obtained by pyrolysis and derivatives are one of the most promising carbon-based materials for ORR electrocatalysts due to their high defect density and heteroatom doping potential [16]. Despite these benefits, unmodified carbon materials lacking surface functionalization generally display low activity toward 2e− ORR, making it important to develop strategies to enhance their catalytic performance.
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Yuzhong Huang, Chang Zhang, Xingyu Wang, Yuji Wu, Jun Lv, Jian Zhang, Wangqiang Shen, Xing Lu (2025). Synergistic Single-Atom and Clustered Cobalt Sites on N/S Co-Doped Defect Nano-Carbon for Efficient H2O2 Electrosynthesis. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01657-9
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Frequently Asked Questions
What is the main innovation of this study?
The study introduces a novel defect-rich nanocarbon catalyst (CoSA/CoNP-NSDNC) that combines cobalt single atoms and cobalt nanoparticle clusters on a fullerene-derived carbon framework, achieving efficient H2O2 electrosynthesis via the two-electron oxygen reduction reaction.
How does the CoSA/CoNP-NSDNC catalyst perform in acidic conditions?
The catalyst exhibits high H2O2 selectivity (~90%) over a wide potential range, with an onset potential of 0.72 V vs. RHE and a Faraday efficiency close to 95% in acidic conditions, demonstrating excellent acid resistance.
What is the significance of using fullerene as a carbon substrate?
Fullerene (C60) provides abundant pentagonal topological defects, which enhance electron transfer and create active sites for the oxygen reduction reaction, making it an ideal substrate for designing high-performance carbon-based catalysts.
What are the potential applications of this catalyst?
The catalyst shows promise for environmental applications, including efficient degradation of organic pollutants via Fenton-like reactions, and can be used in flow cell setups for high-rate H2O2 production.
How does the synergistic effect between single atoms and nanoparticles contribute to performance?
The synergy between NSCo single atoms and Co nanoparticle clusters embedded in the carbon framework enhances the catalytic activity and selectivity for H2O2 production, as demonstrated by electrochemical experiments.
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