利用废弃稀土荧光粉直接制备稀土掺杂高取向{001}晶面氧化钛纳米片阵列薄膜及其光催化研究

Rare earth is an important strategic resource. Due to the over-exploitation, Illegal exploitation and export control of rare earth minerals in China, the technologies on recycling and high value-added utilization of rare earth secondary resource have become a research focus at home and abroad. The Rare-Earth (RE)-doped TiO2 is an important semiconductor material that can be potentially applied in environment and energy field. However, there are some drawbacks in its traditional preparation and practical application such as high-cost, easy aggregation of nanoparticles and low photocatalytic activity. In this project, we will prepare controllably high exposed {001} facets RE-doped TiO2 nanosheets film with high photocatalytic activity and outstanding antimicrobial property via the sol-gel and mild solvothermal method in order to overcome the drawbacks of RE-doped TiO2 nanoparticles mentioned above. The waste rare earth fluorescent powders and suitable non-metallic ions were used as a dopant RE sources and dopant non-metallic ions sources, respectively. The relationship between the RE, non-metal ions co-doped and TiO2 nanosheets morphology crystal face exposure, spectral response range, photocatalytic and antibacterial properties will be investigated. The doping mechanism of waste rare earth fluoresent powders and the formation mechanism of highly oriented {001} crystal planes of TiO2 nanosheets will also be investigated, respectively. A low-cost, simple, efficient method for preparing controllably TiO2 nanosheet-arrays film will be established and he relationship between the organizational structure, photocatalytic and antibacterial properties will be revealed.

稀土是重要战略资源，在我国稀土矿产过度开采、乱采乱挖和实施出口管控的背景下，开发稀土二次资源再生和高值利用技术成为国内外的研究热点。稀土掺杂TiO2纳米材料在环境和能源领域具有广阔的应用前景，但其传统制备应用中还存在成本偏高、纳米粒子易团聚、光催化活性偏低等问题。针对上述问题，本项目提出直接利用废弃稀土荧光粉为稀土掺杂源，优选非金属离子调变剂，通过溶胶凝胶和溶剂热两步法，低成本可控制备具有优异光催化和抗菌性能的稀土掺杂高取向{001}晶面TiO2 纳米片阵列薄膜的研究思路，并深入研究稀土离子和非金属离子对 TiO2 纳米片的结构形态、晶面暴露、光谱响应范围、光催化及抗菌性能的影响规律，揭示废弃稀土荧光粉的掺杂机理和高取向性{001}晶面TiO2 纳米片的形成机制。本项目将建立一种低成本、简单高效的TiO2 纳米片的可控制备方法，揭示其材料成分、组织结构、光催化及抗菌性能之间的关系。

稀土是重要战略资源，在我国稀土矿产过度开采、污染严峻的背景下，开发稀土二次资源再生和高值利用技术成为国内外的研究热点。稀土掺杂TiO2纳米材料在环境和能源领域具有广阔应用前景，但传统制备方法存在成本偏高、纳米粒子易团聚、光催化活性偏低等问题。本项目旨在利用废弃稀土荧光粉为原料，制备稀土掺杂高取向{001}晶面氧化钛纳米片阵列薄膜，从而既实现稀土二次资源的高值利用，又避免纳米粉末制备应用过程中的有关缺点。.首先，利用H2SO4（或HCl）-H2O2选择性浸出技术回收废阴极射线管（CRT）稀土荧光粉中稀土元素，实现了高效清洁回收废CRT稀土荧光粉中稀土元素的目的，研究了HCl-H2O2选择性浸出过程中S2-元素的转化机理及废粉浸出动力学；其次，利用Na2O2碱熔盐氧化技术有效分解废荧光灯稀土荧光粉中含有的陶瓷相稀土组份，实现了其含有的稀土元素的高效溶出，研究了Na2O2碱熔盐氧化过程中稀土陶瓷相组份的碱熔机制及其溶出动力学。最后，利用废弃荧光粉中回收的稀土元素作为掺杂源，选择钛酸四丁酯为钛源、冰醋酸为溶剂、HF为晶面调变剂，通过低温溶剂热法，成功实现了在FTO玻璃表面可控制备具有{001}晶面高暴露率的稀土（Y、La等）掺杂TiO2纳米片阵列薄膜材料，研究了稀土掺杂、HF和反应时间等对TiO2结构形态、晶面暴露、光谱响应范围、光催化性能的影响规律，探索了稀土掺杂TiO2纳米片阵列薄膜的掺杂机理、生长机理以及光催化机理。.本项目探索了废弃荧光粉回收稀土元素的工艺技术路线，建立了一种低成本、简单高效可控制备稀土掺杂TiO2纳米片阵列薄膜材料的方法，揭示了废弃荧光粉酸浸和碱熔反应的动力学机制，阐明了纳米片的材料成分、组织结构、光催化性能之间的关系。以第一作者或通讯作者发表SCI论文6篇，其中ACS Sustainable Chemistry & Engineering、Journal of Cleaner Production、Resources, Conservation & Recycling等IF > 3的论文4篇；申请国家专利2项；主持和参与制定行业标准5项；引起国内外同行广泛关注和较好评价。