Acta Phys. -Chim. Sin.

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Metal-center optimization and phosphate functionalization of porphyrinic COFs/CNT hybrids for photothermal-photocatalytic uranium extraction from seawater

Jingyi Jiang1, Hangxing Wu1, Bin Zuo1, Ruoyu Wang1, Pengde Li1, Guoze Yan1, Xianxiang Li1, Wuwan Xiong3, Xiaobing Wang4, Yang Guo5, Xingtao Xu1, Shijie Li1,2   

  1. 1 Marine Science and Technology College, Zhejiang Key Laboratory of Pollution Control for Port-Petrochemical Industry, National Engineering Research Center for Marine Aquaculture, Zhejiang Ocean University, Zhoushan 316022, Zhejiang Province, China;
    2 Pingyang Institute of Science and Technology Innovation, Wenzhou 325400, Zhejiang Province, China;
    3 School of Environmental and Chemical Engineering, Zhaoqing University, Zhaoqing 526061, Guangdong Province, China;
    4 School of Chemistry and Civil Engineering, Shaoguan University, Shaoguan 512005, Guangdong Province, China;
    5 Key Laboratory of Soil Environmental Management and Pollution Control, Nanjing Institute of Environmental Sciences, Ministry of Ecology and Environment, Nanjing 210042, Jiangsu Province, China
  • Received:2026-08-09 Revised:2026-10-06 Accepted:2026-10-07
  • Contact: Bin Zuo, Xingtao Xu, Shijie Li E-mail:zuobin@zjou.edu.cn;xingtao.xu@zjou.edu.cn;lishijie@zjou.edu.cn

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Abstract: Uranium extraction from seawater is of great strategic significance for ensuring the sustainable development of nuclear energy. However, the extremely low uranium concentration and high concentrations of competing ions in seawater pose multiple challenges for materials, including difficult recognition, slow mass transfer, and insufficient photocatalytic efficiency. To address these issues, this study constructed a phosphate-functionalized nickel porphyrin covalent organic framework/carbon nanotube composite material (Ni-COF-PA/CNT) for efficient photothermal-photocatalytic synergistic uranium extraction from seawater. First, using metal-free and CNT-free COFs as the baseline framework, Ni, Co, and Cu were selected as representative porphyrin metal centers. Based on the regulation of energy-band matching and interfacial charge transfer by their different d-electron structures, M-COF/CNT platforms were constructed and screened, leading to the identification of Ni-COF/CNT as the composite system with the best overall performance. Subsequently, using the Ni-based framework as the target, Ni-COF-PA/CNT was further constructed, revealing the synergistic enhancement effects of phosphate functionalization and CNT integration on uranyl recognition, interfacial charge transport, and photothermal mass transfer. Benefiting from the synergistic coupling among Ni active centers, phosphate-group recognition sites, and the conductive/photothermal CNT framework, Ni-COF-PA/CNT achieved a light-assisted uranium uptake capacity of 339 mg g-1 in a 20 mg L−1 U(VI) solution prepared with deionized water, a Langmuir-fitted maximum adsorption capacity of 1517.66 mg g-1 and a highest experimentally measured capacity of 1307 mg g-1 within the tested concentration range, and an adsorption amount of 3.45 mg g-1 after 7 days of exposure in real seawater. This study provides new insights into the design of multifunctional synergistic uranium-extraction materials for complex seawater systems.

Key words: Uranium extraction, Covalent organic framework, Carbon nanotube, Phosphate functionalization, Light-assisted uranium uptake