Key Takeaways & Executive Findings
- •• • Achieved a H2O2 production rate of 653 μmol/(g·h) in ultrapure water and actual seawater without sacrificial agents, demonstrating dual-medium viability for decentralized H2O2 synthesis. • • Visible-light-driven benzylamine oxidation reached 92% conversion and >99% selectivity, showcasing dual functionality for fine chemical synthesis under mild conditions. • • Surface oxygen-containing functional groups enhance charge separation and shift the conduction band to a more negative potential, directly improving photocatalytic efficiency. • • Ion interference studies revealed that Ca2+ and K+ markedly inhibit H2O2 production, whereas Mg2+ and Na+ have minimal impact, guiding seawater pretreatment strategies.
Abstract
Photocatalytic production of hydrogen peroxide (H2O2) from sustainable biomass-derived carbon catalysts offers a renewable route to valuable chemicals, yet the regulatory role of surface functional groups on reaction kinetics remains underexplored. Here, hydrothermal carbon spheres (CS) rich in oxygen-containing functional groups demonstrated a remarkably high H2O2 production rate of 653 μmol/(g·h) in both pure water and actual seawater, without any sacrificial agent. The catalyst also exhibited outstanding activity in visible-light-driven photocatalytic oxidation of benzylamine to imines, achieving 92% conversion and >99% selectivity. Comprehensive analysis revealed that CS was rich in surface oxygen-containing functional groups, a feature strongly associated with its high photocatalytic efficiency. The observed positive Zeta potential of CS in seawater likely diminished electrostatic repulsion against positively charged intermediates, facilitating their accumulation at the liquid-solid interface. This work proposes a strategic framework for developing metal-free photocatalysts from biomass, offering a sustainable pathway for photocatalytic applications.
1. Introduction
Industrial H2O2 production relies on the energy-intensive anthraquinone process, which generates hazardous by-products and poses sustainability challenges. Photocatalysis using solar energy to convert O2 and H2O into H2O2 has emerged as a green alternative, but conventional photocatalysts often suffer from poor selectivity, low efficiency, or reliance on sacrificial agents. Seawater, constituting 97% of global water resources, offers an abundant and accessible medium, yet its dissolved salts can interfere with light absorption, electron transport, and band structure, impairing performance.
This study addresses these bottlenecks by employing hydrothermal carbon spheres (CS) rich in oxygen-containing functional groups, which enhance charge separation and tune the conduction band position. The catalyst achieves a high H2O2 production rate of 653 μmol/(g·h) in both pure water and seawater without sacrificial agents, and simultaneously drives selective benzylamine oxidation with 92% conversion and >99% selectivity. These findings provide a strategic framework for developing metal-free, biomass-derived photocatalysts for sustainable H2O2 production and fine chemical synthesis.
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CHANG Yuhong, HAN Xue, ZHANG Yanxia, LI Guofang, HU Tianjun, CHEN Wenwen, PEI Linjuan, JIA Jianfeng (2026). Hydrothermal Carbon with Abundant Oxygen-Containing Functional Groups for Photocatalytic H2O2 Generation in Water and Seawater. Journal of Fuel Chemistry and Technology. https://doi.org/10.1016/S1872-5813(25)60622-0
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Frequently Asked Questions
What is the maximum H2O2 production rate achieved by the CS catalyst, and under what conditions?
The CS catalyst achieves a H2O2 production rate of 653 μmol/(g·h) in both ultrapure water and actual seawater, without any sacrificial agent, under aerobic and light irradiation conditions.
How do specific seawater ions affect the photocatalytic H2O2 production?
Mg2+ and Na+ ions exhibit minimal influence on H2O2 generation, whereas Ca2+ and K+ ions markedly inhibit its production. This suggests that seawater pretreatment should consider removing or mitigating Ca2+ and K+ to maintain high efficiency.
What is the dual-functional performance of the CS catalyst in organic synthesis?
The CS catalyst demonstrates exceptional performance in visible-light-driven benzylamine oxidation, achieving 92% conversion and >99% selectivity to imines, indicating its potential for selective organic transformations under mild conditions.
What is the proposed mechanism for H2O2 generation over the CS catalyst?
Experimental results elucidate a dual-pathway mechanism involving both water oxidation and oxygen reduction for H2O2 generation, facilitated by the oxygen-containing functional groups that enhance charge separation and adjust the conduction band position.
How does the surface charge of CS in seawater influence its photocatalytic activity?
The positive Zeta potential of CS in seawater likely diminishes electrostatic repulsion against positively charged intermediates, thereby facilitating their accumulation at the liquid-solid interface and enhancing the overall photocatalytic efficiency.
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