Cu/Zr-Silicate-1催化二氧化碳加氢制备甲醇及其反应机制的研究

批准号:
22002066
项目类别:
青年科学基金项目
资助金额:
24.0 万元
负责人:
杨晓丽
依托单位:
学科分类:
催化化学
结题年份:
2023
批准年份:
2020
项目状态:
已结题
项目参与者:
杨晓丽
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中文摘要
CO2催化加氢制备甲醇技术是实现“碳”资源循环利用,缓解环境和能源危机的重要途径。高分散负载型Cu基催化剂可促使该过程的高效进行,但Cu颗粒在反应条件下容易烧结,并伴随着反应路径的多样化导致甲醇选择性下降。因此,构建具有易于生成HCOO*中间体的铜-载体界面位点的高稳定性催化剂有利于CO2转化为甲醇。在前期利用分子筛稳定金属组分的研究基础上,本项目拟以Zr掺杂的Silicate-1杂原子分子筛为载体负载Cu活性组分,利用其规则的孔道结构以及骨架Zr和丰富的平衡阳离子环境,实现具有高稳定性的高效Cu/Zr-Silicate-1催化剂的可控合成。通过探索Cu的电子配位状态及与载体的界面结构以阐明催化剂的稳定机制,建立催化剂结构-功能之间的关系以探讨甲醇的生成机制。本项目的实施有望为CO2高效转化制备甲醇的催化剂设计与合成提供理论指导,同时为CO2资源化“液态阳光”能源战略研究起到推动作用。
英文摘要
Catalytic hydrogenation of carbon dioxide to methanol offers a significant way of realizing the recycling of “carbon” resource, as well as alleviating the environmental and energy crisis. Copper-based catalyst with highly dispersion promotes the efficiency of this process, but copper particles suffers from severe sintering under the reaction conditions, will subsequently lead to the selectivity reduction due to the diversification of the reaction paths. Therefore, the construction of a high-stability catalyst with Cu-support interface sites that are easy to produce HCOO* intermediates is conducive to the conversion of CO2 into methanol. Based on the previous research on the use of zeolites to stabilize metal components, this project intends to use Zr-doped Silicate-1 heteroatomic zeolite as support to load Cu active components and realize the controllable synthesis of efficient catalyst with high stability by taking advantage of its pore structure, framework Zr and balanced cation environment. By investigating the structural state and electronic coordination environment of Cu, the interaction between Cu and support as well as the stability mechanism of the catalyst will be explored. The structure-function relationship of catalyst will be established to reveal the mechanism of methanol formation. This project will provide theoretical guidance for the development of efficient catalysts for CO2 conversion to methanol and will drive the utilization of CO2 resource for the "liquid sunlight" energy strategy.
期刊论文列表
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专利列表
DOI:doi.org/10.1016/j.fuel.2023.127560
发表时间:2023
期刊:Fuel
影响因子:7.4
作者:Xiaoli Yang;Zein Li;Mingyu Guo;Tao Zhao;Xiong Su;Wei Jiang;Guangting Han;Haoxi Ben
通讯作者:Haoxi Ben
DOI:10.1002/ajoc.202100381
发表时间:2021-08
期刊:Asian Journal of Organic Chemistry
影响因子:2.7
作者:Xiaoli Yang;Haoxi Ben;Arthur J. Ragauskas
通讯作者:Xiaoli Yang;Haoxi Ben;Arthur J. Ragauskas
DOI:10.1016/j.cej.2022.136655
发表时间:2022-04
期刊:Chemical Engineering Journal
影响因子:15.1
作者:Xiaoli Yang;Jia Yang;Tao Zhao;W. Qian;Yalan Wang;A. Holmen;Wei Jiang;Der-Nien Chen;Haoxi Ben-Hao
通讯作者:Xiaoli Yang;Jia Yang;Tao Zhao;W. Qian;Yalan Wang;A. Holmen;Wei Jiang;Der-Nien Chen;Haoxi Ben-Hao
DOI:10.1016/j.apcatb.2021.120716
发表时间:2022-01
期刊:Applied Catalysis B: Environmental
影响因子:--
作者:Xiaoli Yang;Jia Yang;Yalan Wang;Tao Zhao;Haoxi Ben;Xuning Li;A. Holmen;Yanqiang Huang;De Chen
通讯作者:Xiaoli Yang;Jia Yang;Yalan Wang;Tao Zhao;Haoxi Ben;Xuning Li;A. Holmen;Yanqiang Huang;De Chen
DOI:10.1002/cey2.391
发表时间:2023-08
期刊:Carbon Energy
影响因子:20.5
作者:Xin Wang;X. Yang;Guangxian Pei;Jifa Yang;Junzhe Liu;Fengwang Zhao;Fayi Jin;Weiping Jiang
通讯作者:Xin Wang;X. Yang;Guangxian Pei;Jifa Yang;Junzhe Liu;Fengwang Zhao;Fayi Jin;Weiping Jiang
国内基金
海外基金
