基于卟啉结构位置锚定与复合金属核壳构效的高分散纳米Au-Cu催化剂构筑及性能研究

批准号:
22008031
项目类别:
青年科学基金项目
资助金额:
24.0 万元
负责人:
方嘉声
依托单位:
学科分类:
反应工程
结题年份:
2023
批准年份:
2020
项目状态:
已结题
项目参与者:
方嘉声
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中文摘要
探索特定固载机制提高贵金属负载能力、热稳定性及位置锚定效果,是纳米催化领域的研究热点。本项目通过功能合成卟啉基MOF空心管,利用卟啉结构平面共轭对称四坐标氮位点与金属离子间强静电、配位键合作用,结合原位还原技术及稳定的金属-卟啉结构,构建Au-Cu二元金属复合体系,定向锚定纳米Au-Cu粒子,实现高分散、高稳定纳米Au晶体的固载。介孔CeO2的界面修饰发挥结构限域,与内载体在碳化热解中相互作用,固化重构活性位,构筑复合金属核壳构效下体系特殊层间交联孔结构,得到新型纳米Au-Cu催化剂。以无溶剂苯甲醇选择性氧化反应为探针,研究Au-Cu晶体结构、分布特征、金属-载体相互作用及体系核壳构效层间交联孔结构调控与其协同催化性能间内在构效关系,揭示其对提高金属活性位固化效果和改善反应性能的作用机制。本项目的实施有助于创新纳米贵金属催化剂的制备思路,发展纳米金属固化锚定新方法,具有潜在经济和社会效益。
英文摘要
Exploring specific immobilization mechanisms to improve the loading capacity, thermal stability and location anchoring effect of noble metals, is always the research hotspot of nanocatalysis field. The project firstly prepares the porphyrin-functionalized MOF hollow tubes and effectively anchors Au and Cu ions by strong electrostatic interaction and coordination bond effect of well-defined square-planar conjugate symmetric four-coordinate nitrogen sites originated from porphyrin structure. Combined with in-situ reduction technology and stable metal-porphyrin structure, the Au-Cu binary metallic composite system is constructed and Au-Cu nanoparticles are directionally anchored, which achieves the effective spatial distribution of extremely dispersed and stable Au nanocrystals. The interface modification of mesoporous CeO2 exerts the structural confinement effect and interacts with internal carriers during the carbonization pyrolysis, so as to solidify and reconstruct metallic active sites. Meanwhile, unique interlayer crosslinked channel structures driven by the architecture effect of metallic composite core-shell system are constructed, and the target catalysts with highly dispersed Au-Cu nanoparticles are obtained. With the reaction of solvent-free selective oxidation of benzyl alcohol as the probe, the intrinsic structure-activity relationship among the crystal structure and distribution characteristics of Au-Cu nanoparticles, the metal-carrier interaction, and the interlayer crosslinked channel structure under the regulation of metallic composite core-shell system and its corresponding synergistic catalysis performance is studied. And investigation of the mechanism between boosted location anchoring effect of metallic active sites and improved catalytic capability of catalysts is revealed. The implementation of this project will be conducive to the improvement of innovative preparation concept of noble-metal nanocatalysts, and the development of location anchoring and solidifying technologies for metallic nanocrystals, with potential economic and social benefits.
期刊论文列表
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专利列表
DOI:10.1016/j.cej.2022.137436
发表时间:2022
期刊:Chemical Engineering Journal
影响因子:15.1
作者:Shuo Zhao;Yuepeng Liu;Yanyun Wang;Jiasheng Fang;Yiqiang Qi;Yuming Zhou;Lihong Liu;Shuping Zhuo
通讯作者:Shuping Zhuo
DOI:10.1016/j.colsurfa.2023.132305
发表时间:2023-08
期刊:Colloids and Surfaces A: Physicochemical and Engineering Aspects
影响因子:--
作者:Jiasheng Fang;Qiqi Diao;Ming Chen;Shuo Zhao;Yanliang Li;Kun Wei;Zhenting Huang;Q. Zhuo
通讯作者:Jiasheng Fang;Qiqi Diao;Ming Chen;Shuo Zhao;Yanliang Li;Kun Wei;Zhenting Huang;Q. Zhuo
DOI:--
发表时间:2023
期刊:化工进展
影响因子:--
作者:方嘉声;陈铭;黄振庭;卫昆;陈玉兰
通讯作者:陈玉兰
DOI:10.1016/j.jcis.2022.02.057
发表时间:2022-02
期刊:Journal of colloid and interface science
影响因子:9.9
作者:Shuo Zhao;Yuepeng Liu;Yanyun Wang;Jiasheng Fang;Yiqiang Qi;Yuming Zhou;Xiaohai Bu;Shuping Zhuo
通讯作者:Shuo Zhao;Yuepeng Liu;Yanyun Wang;Jiasheng Fang;Yiqiang Qi;Yuming Zhou;Xiaohai Bu;Shuping Zhuo
DOI:10.1016/j.ijhydene.2021.05.018
发表时间:2021-07-02
期刊:INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
影响因子:7.2
作者:Liu, Yuepeng;Zhao, Shuo;Zhuo, Shuping
通讯作者:Zhuo, Shuping
国内基金
海外基金
