Citation: Yun Chen, Daijie Deng, Li Xu, Xingwang Zhu, Henan Li, Chengming Sun. Covalent bond modulation of charge transfer for sensitive heavy metal ion analysis in a self-powered electrochemical sensing platform[J]. Acta Physico-Chimica Sinica, ;2026, 42(1): 100144. doi: 10.1016/j.actphy.2025.100144 shu

Covalent bond modulation of charge transfer for sensitive heavy metal ion analysis in a self-powered electrochemical sensing platform

Yun Chen ^{1, 3, 4} ,
Daijie Deng ² ,
Li Xu ² ,
Xingwang Zhu ^1,, ,
Henan Li ^2,, ,
Chengming Sun ^{1, 3, 4}

1.
Research Institute of Smart Agriculture, Agricultural College, College of Environmental Science and Engineering, College of Mechanical Engineering, Yangzhou University, Yangzhou 225009, Jiangsu Province, China
2.
School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
3.
Cultivation and Construction Site of National Key Laboratory for Crop Genetics and Physiology in Jiangsu Province, Yangzhou University, Yangzhou 225009, Jiangsu Province, China
4.
Jiangsu Co-Innovation Center for Modern Production Technology of Grain Crops, Yangzhou University, Yangzhou 225009, Jiangsu Province, China

Corresponding author: Xingwang Zhu, zxw@yzu.edu.cn Henan Li, lhn@ujs.edu.cn
Received Date: 29 April 2025
Revised Date: 22 June 2025
Accepted Date: 31 July 2025

Rational design of photoelectric active materials for photoanodes in photocatalytic fuel cells is crucial for developing highly sensitive self-powered electrochemical sensors. Achieving directional migration and shortening transmission pathways of charge in photoanodes remains a fundamental challenge for enhancing the oxygen evolution reaction performance of photocatalytic fuel cells. Herein, tungsten species atomically dispersed on carbon-rich graphitic carbon nitride (W-CN-C) with the N–W–O covalent bond was designed as the photoanode for constructing a self-powered photocatalytic fuel cell sensing of heavy metal copper ions. W-CN-C was synthesized by self-assembly, exfoliation, and thermal-induced treatment process. The N–W–O covalent bonds by anchoring tungsten atoms on carbon-rich carbon nitride served as an interfacial charge transport channel, facilitating the separation and migration of charge carriers. The carbon content increase by forming a carbon-rich structure can enhance π-electron delocalization in the W-CN-C, significantly broadening sunlight utilization range. The dispersed tungsten atoms provide effectively active sites, promoting the kinetics of the oxygen evolution reaction between the W-CN-C photoanode and electrolyte interface. The synergistic effects significantly enhance the visible light absorption ability and charge separation and transfer efficiency, improving the photoelectric conversion efficiency of W-CN-C photoanode, exhibiting superior oxygen evolution reaction performance, leading to the amplified open circuit potential in the photocatalytic fuel cell system based on excellent oxygen reduction reaction performance of the Pt@C electrocatalyst cathode. The specific identification probe for copper ions was effectively anchored on the W-CN-C photoanode to construct a self-powered photocatalytic fuel cell sensing platform for copper ions detection. The complex formed by copper ions and the probe hindered electron transport at the W-CN-C photoanode, altering the output detection signal of the photocatalytic fuel cell, thus demonstrating a broad detection range spanning five orders of magnitude (2.0 × 10⁻²–9.2 × 10² nmol L⁻¹), a low limit of detection (7.0 pmol L⁻¹), high selectivity against common interferents, and applicability for detecting heavy metal copper ions in the aquatic environment. Furthermore, the platform allowed for self-powered and portable determination of copper ions using a multimeter as a signal output device, achieving a detection range of 0.25–1.3 × 10² nmol L⁻¹ and a limit of 84 pmol L⁻¹. This work proposes an approach for developing a high-performance photoanode utilizing atomically dispersed metals to introduce covalent bonds as charge transfer channels, paving the way for highly sensitive self-powered electrochemical sensors for environmental monitoring.
- Photocatalytic fuel cell,
- Self-powered electrochemical sensor,
- Oxygen evolution reaction,
- Carbon nitride,
- Charge transfer channel
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沈阳化工大学材料科学与工程学院沈阳 110142