功能化纳米结构材料在乏燃料后处理中的应用基础研究

This proposal is motivated by the national great needs to develop the new technologies for spent fuel reprocessing and high-level waste disposal. Based on the evaluation of nano-structured materials with efficient sorption properties and specific compositions, carbon nanomaterials are selected and consequently assembled with magnetic oxides, and then polymers or organosilicate molecules are grafted onto the nanocomposites by using plasma-induced grafting technique. Finally, the functionalized magnetic nano-structured materials are obtained for further sorption and separation experiments. The sorption and desorption behaviors of nuclides by the functionalized magnetic nano-structured materials will be systematically investigated. The relationship between sorption behaviors and the compositions as well as the microstructures of functionalized nanomaterials will be clarified. The physical and chemical properties of the micro-interface of the functionalized nanomaterials can be adjusted to improve the preferential sorption capacity for radionuclides. The radiation stability of the grafted fractions and the functionalized nanomaterials will also be studied, exploring changes of the micro-structure and sorption capacity of the functionalized nanomaterials before and after irradiation. The possible interacting mechanisms of radionuclides with the interface of functionalized nanomaterials will be investigated by using batch experiments, microscopic characterization, and quantum chemical computation. Through this project, the novel functionalized nanomaterials for radionuclide sorption and separation and related new technologies for spent fuel reprocessing will be hopefully developed. It is expected that this project will achieve innovative results, and be of strategic significance for enhancing the national capability of independent innovation in nuclear energy field.

乏燃料后处理是世界上最复杂和挑战性的问题之一，迫切需要发展新材料和新技术。功能化纳米材料由于其特殊性质在乏燃料后处理中具有广泛的潜在应用前景。本项目拟在碳纳米材料上组装磁性氧化物，再用等离子体技术在其表面接枝不同的聚合物或有机硅分子，构建新型功能化磁性纳米结构材料；研究放射性核素的吸/脱附行为和性能，阐明功能化纳米结构材料的吸附性能与纳米材料组成和组装结构的关系；调控微界面的物理、化学性质，提高材料对放射性核素的吸附选择性；研究表面接枝分子及其功能化纳米结构材料的辐照稳定性，探讨材料辐照前后微观结构和吸附性能的变化；采取宏观静态吸附、微观表征和理论计算相结合，研究不同放射性核素与功能化纳米结构材料在固液界面的相互作用机理。项目结果将为纳米结构材料在乏燃料后处理中的应用提供实验与理论依据，促进我国乏燃料后处理技术的进步。

乏燃料后处理是世界上最复杂和挑战性的问题之一，乏燃料具有很强的放射性，如果处置不当将引发难以估量的灾难，迫切需要发展新材料和新技术。针对上述科学问题，项目组主要发展了等离子体技术和纳米技术在乏燃料处理方面的基础科学和应用基础研究。针对放射性废液中放射性核素浓度低、治理难的关键科学问题，利用低温等离子体技术和纳米技术将功能有机分子修饰在纳米材料表面，提高了对放射性核素的高效和选择性富集能力，并进一步用理论计算化学分析了放射性核素与纳米功能材料的作用机理，形成了利用等离子体和纳米技术研究放射性污染治理的特色，相关结果发表在Chem. Soc. Rev.，Environ. Sci. Technol.，Geochim. Cosmochim. Acta，Adv. Mater，ACS Nano等期刊上，3篇论文（EST, 2016, 50, 4459; 2015, 49, 4255; GCA, 2016, 180, 51）被评为中国百篇最具影响国际学术论文，1篇论文（GCA, 2014, 140, 621）被评为fast breaking paper，多篇论文被评为热点或高被引论文（EST, 2016, 50, 3658; 2016, 50, 4459; GCA, 2015, 165, 86; ESN, 2017, 1, 222; EP, 2016, 219, 107; JHM, 2014, 280, 399; 2016, 309, 107; CEJ, 2016, 293, 311; 2016, 287, 448; Carbon, 2016, 99, 123等）。上述研究结果对于分析和评价纳米结构材料在乏燃料后处理中的应用提供实验与理论依据，促进我国乏燃料后处理技术的进步。近四年发表SCI论文200多篇，被SCI他引3000多次。3名博士生获中科院院长奖，1篇学位论文被评为中科院优博论文，王祥科教授2014-2017连续四年被汤森路透（科睿唯安）评为环境与生态、工程技术领域全球高被引科学家，2015年被评为教育部长江学者特聘教授，2016年入选科技部中青年科技创新领军人才和北京市百名科技领军人才，2017年入选第3批国家“万人计划”科技创新领军人才，受J. Hazard. Mater.，Radiochim. Acta，Sci. China Chem.等期刊邀请担任期刊编委等。