聚电解质薄膜负载纳米粒子的 制备及其催化性能研究
文献类型：学位论文
| 作者 | 储诚灿 |
| 学位类别 | 硕士 |
| 答辩日期 | 2015-04 |
| 授予单位 | 中国科学院研究生院 |
| 授予地点 | 中国科学院长春应用化学研究所 |
| 导师 | 苏朝晖 |
| 关键词 | 聚电解质多层膜 纳米粒子 催化 |
| 中文摘要 | 静电层层自组装技术是构筑聚合物薄膜的简单、灵活、廉价的方法，而实现其功能化具有重大的实际应用意义。本论文以静电层层自组装聚电解质薄膜为模型，系统研究利用聚电解质多层膜中存在的抗衡离子合成核壳结构和合金结构的双金属及半导体纳米粒子的方法，考察其在电化学催化和光催化领域内的应用，探究聚合物载体的功能性及其与纳米粒子的协同催化效应。 首先，利用层层自组装多层膜替代传统的载体材料，通过离子交换-原位还原和种子生长方法，原位制备了聚电解质/Au点缀Pt纳米粒子(Pt^Au)复合膜。该复合薄膜用于电催化甲醇氧化反应时，相比于聚电解质/Pt纳米粒子复合膜表现出优异的电催化活性、抗毒化能力和稳定性。 接着，以静电层层自组装的薄膜为聚合物基体，利用薄膜内的抗衡离子同时引入AuCl4-和PtCl62-，探索AuPt合金纳米粒子的原位合成，发现在合适的动力学条件下多层膜基体可以抑制Au和Pt的相分离，直接得到热力学不稳定的AuPt合金粒子，且其组成在大范围内易于调控；进一步研究发现这种负载AuPt合金粒子的薄膜相比于单金属展现出协同催化效应、具有更高的催化活性。 最后，采用离子交换/原位沉淀的方法，在聚电解质多层膜内原位合成了CdS纳米粒子，发现利用多层膜的富集效应和多孔结构可以解决传统聚合物载体的传质问题，展示出聚合物载体的功能性及其与纳米粒子的协同催化效应，使得复合膜的光催化活性与目前最好的商业化产品相当 |
| 英文摘要 | Electrostatic layer-by-layer assembly technique is a facile, versatile, inexpensive approach to fabrication of polymer films, and functionalization of these multilayer films has significant practical implication. In this dissertation, we systematically research synthesis of core-shell, alloy and semiconductor nanoparticles in-situ in polyelectrolyte multilayers (PEMs) with the assistance of the counterions, investigating their application in electrocatalysis and photocatalysis in order to explore effects of the polymer support, in particular the synergetic effects between polymer support and the nanoparticles. Firstly, we substituted PEMs for traditional support materials for the catalys in direct methanol fuel cells. PEM-supported Au-decorated-Pt (denoted as Pt^Au) nanoparticles were fabricated via ion exchange/in-stiu reduction cycles and a stepwise seed-mediated growth method, which were found to be truly effective electrocatalyst for the oxidation of methanol in the acidic electrolyte, exhibiting better electrocatalytic efficiency, superior tolerance to poisoning and electrochemical durability compared with the monometallic Pt nanoparticles. Then, we attempted to synthesize AuPt alloy nanoparticles in situ in the PEM as matrixes via an ion-exchange and co-reduction process, in which the PEM support was found to suppress the Au-Pt phase separation, and thus enabled formation of AuPt alloy nanoparticles, which are metastable, over a wide composition range. Furthermore, the PEM-supported AuPt alloy nanoparticles exhibited higher catalytic activity than Au and Pt monometallic ones for the reduction of 4-nitrophenol by NaBH4, showing synergistic effects between Au and Pt. Finally, CdS nanoparticles were synthesized within the PEM through ion-exchange/in-situ precipitation process. Enrichment effects and porous structure of the PEM could mitigate the mass transfer problem of traditional polymer supports, demonstrating functionality of the PEM support and synergetic effects between nanoparticles and polymer support. As a result, the photocatalytic activity of the PEM-supported CdS nanoparticles reached the highest level of commercial products. |
| 语种 | 中文 |
| 公开日期 | 2016-05-03 |
| 源URL | [http://ir.ciac.jl.cn/handle/322003/64459]  |
| 专题 | 长春应用化学研究所_长春应用化学研究所知识产出_学位论文 |
| 推荐引用方式 GB/T 7714 | 储诚灿. 聚电解质薄膜负载纳米粒子的 制备及其催化性能研究[D]. 中国科学院长春应用化学研究所. 中国科学院研究生院. 2015. |
入库方式： OAI收割
来源：长春应用化学研究所
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。