Investigation of Metal Organic Frameworks for Renewable Energy Electrocatalysis

可再生能源电催化金属有机框架的研究

• 批准号: RGPIN-2019-05927
• 负责人: Kornienko, Nikolay
• 金额: $ 2.11万
• 依托单位: Université de Montréal
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2020
• 资助国家: 加拿大
• 起止时间: 2020-01-01 至 2021-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=715010
• 关键词: Investigation; Metal; Organic; Frameworks; Renewable

Catalyst development for renewable energy utilization is a pressing global issue. The goal for my research program is to investigate electrocatalytic metal organic frameworks (MOFs) with rationally designed three dimensional catalytically active pockets for conversion of electricity to fuels and chemicals. My objective is to demonstrate that efficiently driving reactions from CO2 and H2O starting materials to the desired products (i.e. CH3OH, CH4, CH3CH2OH) can be accomplished by establishing MOF-based electrochemical systems that incorporate enzyme-inspired reaction effects. These include intermediate stabilization, proton relays, and multiple reactant binding sites within the confined, molecularly tunable catalytic environments of the MOFs. An example is the use of a MOF functionalized with amino groups to stabilize high energy intermediates through hydrogen-bonding interactions and flatten the reaction free energy landscape to accelerate catalysis. Longer term (3-5 year) goals include incorporating proximal active sites to facilitate reactant dimerization to drive the reaction pathway towards C2 products from CO2. In addition, the invesitgation of nanoparticle@MOF core@shell materials will be undertaken. Such systems allow for independent tuning of a nanoparticle catalytically active surface and the immediate reaction environment conferred by the MOF shell. By utilizing the porous MOFs as molecularly tunable electrocatalytic materials, the strengths of heterogeneous (tuneability) and homogeneous (activity, stability) catalysts are combined while also incorporating a new bio-inspired element into the research. To realize the proposed materials, my research team will construct MOF-electrodes by growing MOF thin films directly on conductive substrates. These MOF electrodes will be used directly to catalyze CO-2 reduction in an aqueous electrochemical cell. Their activity and selectivity will be evaluated with electrochemical methods and with a combination of gas chromatography and NMR to detect reaction products. In tandem to synthesis and characterization of MOF electrocatalysts,

催化剂开发 可再生能源的利用是一个紧迫的全球问题。我的目标是 研究计划是研究电催化金属有机骨架 具有合理设计的三维催化活性口袋的(MOF) 将电能转化为燃料和化学品。我的目标是 证明有效地推动二氧化碳和水的反应 将原料转化为所需产品(即CH3OH，CH4， CH3CH2OH)可以通过建立基于MOF的 结合了酶激发的反应效果的电化学系统。 这些包括中间稳定化、质子继电器和多反应物。 受限的、分子可调的催化环境中的结合位置 在MOF中。一个例子是使用氨基功能化的MOF来 通过氢键相互作用稳定高能中间体 平坦化反应自由能景观，加速催化。较长期(3-5 年)的目标包括合并近端的活性中心以促进反应物 二聚反应驱动生成C2产物的反应途径 来自二氧化碳。此外，对纳米粒子@MOF的研究 将承接核壳材料。这样的系统允许独立 纳米粒子催化活性表面的调谐和瞬时 由MOF外壳提供的反应环境。 通过利用 多孔MOF作为分子可调谐的电催化材料， 异质性(可调整性)和同质性(活性、稳定性)的优势 催化剂被组合在一起，同时还加入了一种新的生物启发元素 这项研究。为了实现提议的材料，我的研究团队将 直接在导电材料上生长MOF薄膜构建MOF电极 底物。这些MOF电极将直接用于催化CO-2还原 在水基电化学池中。它们的活性和选择性将是 用电化学方法和气体组合进行评估 用层析和核磁共振检测反应产物。与合成和合成同步进行 MOF电催化剂的表征，