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A high-performance photoelectrochemical water oxidation system with phosphorus doping g-C3N4 and simultaneous metal phosphide cocatalyst formation via a gas treatment

DOI:10.1002/cssc.201802382 期刊:ChemSusChem 出版年份:2019 更新时间:2025-09-23 15:23:52
摘要: Graphitic carbon nitride (g-C3N4) has been widely explored as photocatalyst for water splitting. The anodic water oxidation reaction (WOR) remains the major obstacle for such process, with particular issues on low surface area of g-C3N4, poor light absorption as well as low charge transfer efficiency. In this work, such longtime concerned issues have been partially addressed with band gap and surface engineering of nanostructured graphitic C3N4. Specifically, surface area and charge transfer efficiency are significantly enhanced via architecturing g-C3N4 on nanorod TiO2 to avoid the aggregation of layered g-C3N4. Moreover, a simple phosphide gas treatment of TiO2/g-C3N4 configuration not only narrows the band gap of g-C3N4 by 0.57 eV into visible range, but also in-situ generates a metal phosphide (M=Fe, Cu) water oxidation cocatalyst. This TiO2/g-C3N4/FeP configuration significantly improves charge separation and transfer capability. As a result, our photoelectrochemical system yields outstanding visible light (> 420 nm) photocurrent: ca. 0.3 mA·cm-2 at 1.23 V and 1.1 mA·cm-2 at 2.0 V vs RHE, the highest using g-C3N4 as photoanode. We expect that our TiO2/g-C3N4/FeP configuration generating via simple phosphide gas treatment will bring in new insight for robust g-C3N4 for water oxidation.
作者: Dong-Dong Qin,Jing-Jing Quan,Shi-Fang Duan,Jovan San Martin,Yixiong Lin,Xiaolin Zhu,Xiao-Qiang Yao,Jin-Zhan Su,Ingrid Rodríguez-Gutiérrez,Chun-Lan Tao,Yong Yan
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To address the low surface area, poor light absorption, and low charge transfer efficiency of g-C3N4 for photoelectrochemical water oxidation by developing a high-performance system through phosphorus doping and cocatalyst formation via gas treatment.

The developed TiO2/g-C3N4/FeP configuration via phosphide gas treatment significantly enhances photoelectrochemical performance for water oxidation by improving light absorption, charge separation, and transfer efficiency, achieving the highest reported photocurrent for g-C3N4-based photoanodes, with good stability.

The paper does not explicitly state limitations, but potential areas include the stability of the electrodes (photocurrent decay observed), scalability of the gas treatment process, and comparison with other semiconductors showing lower absolute charge transfer efficiency.

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