|
|
|
设计构筑新型功能性有机无机杂化纳米材料，并将其用于铀、钍、钚等锕系元素的高效分离和富集。该类材料在海水提铀、放射性废液处理以及环境污染修复等领域具有应用潜力。截止目前，课题组已针对如下四类材料展开系统深入研究：(1) 介孔硅材料。采用理论与实验相结合的手段设计新型功能化介孔硅材料，功能基团包括氨基、磷酸酯、咪唑及邻菲罗啉二酰胺等；系统研究这些材料对U(VI)，Th(IV)等锕系离子的吸附分离行为，并利用同步辐射技术结合先进谱学手段深入研究表面配位结构与吸附机理。(2) MOFs & COFs。设计新型功能化MOFs & COFs及其复合物；研究其对U(VI)，Th(IV)，Pu(IV)等锕系离子的高效高选择性分离；深入挖掘影响MOFs & COFs吸附能力的关键因素；着力解决高酸度下吸附效率低和材料水热稳定性差等关键科学问题。(3) 氧化石墨烯(GO)。构筑石墨烯复合材料；研究石墨烯及其复合物对U(VI)，Th(IV)等锕系离子的分离与富集，同时利用光电催化手段研究复合材料对U(VI)的还原固定。(4) 二维片层MXene。通过插层等活化手段提高MXene材料对U(VI)等锕系离子的吸附能力；研究材料对U(VI)等的封装和还原固定，同时构筑MXene复合材料，提高应用针对性。
磷酸酯基功能化介孔硅对U(VI)的高效去除(左)及氨基磷酸酯基双官能团化介孔硅对Th(IV)的协同吸附(右)。
缺陷(左)及金属节点(右)对MOFs吸附U(VI)的影响
Fe/GO复合物(左)及TiO2/GO/Fe3O4复合物对U(VI)的还原固定。
V2CTx 型MXene对U(VI)的吸附及与机理。
代表性研究成果：
1. LiyongYuan, Ming Tian, Jianhui Lan, Xingzhong Cao, Xiaolin Wang, Zhifang Chai, JohnK. Gibson, and Weiqun Shi*. Defects Engineering in Metal−Organic Frameworks: ANew Strategy to Develop Applicable Actinide Sorbents. Chem. Commun. 2018, 54,370-373.
2. LinWang, Wuqing Tao, Liyong Yuan, Zhirong Liu, Qing Huang, Zhifang Chai, John K.Gibson and Weiqun Shi*. Rational control of the interlayer space insidetwo-dimensional titanium carbides for highly efficient uranium removal andimprisonment. Chem. Commun. 2017, 53, 12084-12087.
3. NanZhang, Li-yong Yuan*, Wen-Lu Guo, Shi-Zhong Luo*, Zhi-Fang Chai, Wei-Qun Shi*.Extending the Using of Highly Porous Functionalized MOFs to Th(Ⅵ) capture. ACS Appl. Mater. Interfaces. 2017,9(30), 25216-25224.
4. Zi-JieLi, Zhi-Wei Huang, Wen-Lu Guo, Lin Wang, Li-Rong Zheng, Zhi-Fang Chai, Wei-QunShi*. Enhanced photocatalytic removal of uranium(VI) from aqueous solution bymagnetic TiO2/Fe3O4 and its graphene composite. Environ. Sci &Technol. 2017,51, 5666-5674.
5. ZhiweiHuang, Zijie Li, Lirong Zheng, Limin Zhou, Zhifang Chai, Xiaolin Wang, WeiqunShi*. Interaction Mechanism of Uranium(Ⅵ) with Three-Dimensional Graphene Oxide-ChitosanComposite: Insights from Batch Experiments, IR, XPS, and EXAFS Spectroscopy. Chem.Eng. J. 2017, 328(15), 1066-1074.
6. Li-YongYuan, Lin Zhu, Cheng-Liang Xiao*, Qun-Yan Wu, Nan-Zhang, Ji-Pan Yu, Zhi-FangChai, Wei-Qun Shi*. Large pore 3-D cubic mesoporous (KIT-6) hybrid bearinghard-soft donor combined ligand for enhancing U(VI) capture: an experimentaland theoretical investigation. ACS Appl. Mater. Interfaces. 2017, 9, 3774-3784.
7. LinWang, Li-yong Yuan, Ke Chen, Yujuan Zhang, Qihuang Deng, Shiyu Du, Qing Huang*,Lirong Zheng, Jing Zhang, Zhifang Chai, Michel W. Barsoum, Xiangke Wang, WeiqunShi*. Loading actinides in multi-layered structures for nuclear wastetreatment: the first case study of uranium capture with vanadium carbide MXene. ACS Appl. Mater. Interfaces. 2016, 8, 16396-16403.
8. Zi-JieLi, Lin Wang, Li-Yong Yuan, Cheng-Liang Xiao, Lei Mei, Li-Rong Zheng, JingZhang, Ju-Hua Yang, Yu-Liang Zhao, Zhen-Tai Zhu, Zhi-Fang Chai* and Wei-QunShi*. Efficient removal of uranium from aqueous solution by zero-valent ironnanoparrticle and its graphene composite. J. Hazard. Mater. 2015, 290, 26-33. (高被引论文，Top1%)
9. Zhi-QiangBai, Li-Yong Yuan, Lin Zhu, Zhi-Rong Liu*, Sheng-Qi Chu, Li-Rong Zheng, JingZhang, Zhi-Fang Chai, Wei-Qun Shi*. Introduction of Amino GroupsintoAcid-resistant MOFs for Enhanced U(VI) Sorption. (The first two authorscontributed equally to this work.) J. Mater. Chem. A. 2015, 3, 525-534. (HotArticle)
10. Li-YongYuan, Zhi-Qiang Bai, Ran Zhao, Ya-Lan Liu, Zijie Li, Sheng-Qi Chu, Li-RongZheng, Jing Zhang, Yu-Liang Zhao, Zhi-Fang Chai*, Wei-Qun Shi*, Introduction ofBifunctional Groups into Mesoporous Silicafor Enhancing Uptake of Thorium (IV)from Aqueous Solution. ACS Appl. Mater. Interfaces. 2014, 6, 4786-4796
11. Li-Yong Yuan, Ya-Lan Liu, Wei-Qun Shi*,Zi-jie Li, Jian-Hui Lan, Yi-Xiao Feng, Yu-Liang Zhao, Ya-Li Yuan, Zhi-FangChai. A Novel Mesoporous Materialfor Uranium Extraction, DihydroimidazoleFunctionalized SBA-15. J. Mater .Chem. 2012, 22, 17019-17026.
12. Zi-Jie Li, Fei Chen, Li-Yong Yuan, Ya-Lan Liu,Yu-Liang Zhao, Zhi-Fang Chai, Wei-Qun Shi*. Uranium(VI) adsorption on grapheneoxide nanosheets from aqueous solution. Chem. Eng. J. 2012, 210, 539-546. (高被引论文，Top1%)
13. Li-YongYuan,Ya-Lan Liu, Wei-Qun Shi*, Yu-Long Lv, Jian-Hui Lan, Yu-Liang Zhao,Zhi-Fang Chai. High Performance of Phosphonate-Functionalized Mesoporous Silicafor U(VI) Adsorption from Aqueous Solution. Dalton Trans. 2011, 40, 7446-7453.