CAS: Optimization of CO2 to Methanol Production through Rapid Nanoparticle Synthesis Utilizing MOF Thin Films and Mechanistic Studies.

在化学系化学催化项目的支持下，杨百翰大学的Kara Stowers正在研究如何改进铜催化剂的合成和组成，以减少二氧化碳，这是一个重要的可持续化学目标。由二氧化碳产生的甲醇可以用作燃料和材料原料，使这种化学反应有助于重新平衡碳循环（即将温室气体二氧化碳循环到这种减少的建筑块形式）。目前，铜基催化剂在与二氧化碳反应时反应迟钝，在将其转化为甲醇时不稳定。为了改进这些铜基催化剂，将使用模板方法快速创建和测试用于催化的新纳米颗粒组成和结构。本研究旨在建立一种灵活可调的催化剂开发方法，包括了解催化剂与工业相关材料的基本分子相互作用，以提高催化剂的稳定性和活性。更高效的催化剂将促进向可持续闭环燃料经济的过渡，减少我们对不可再生化石燃料的依赖。此外，这项研究将包括研究生和本科生水平的学生培训，以帮助培养下一代科学家和工程师，致力于解决紧迫的环境挑战。该项目还为大一女生提供有针对性的机会，让她们尽早参与研究，并获得导师的指导。在这个奖项下，杨百翰大学的Kara Stowers和她的研究团队正在研究模板介导的铜基纳米颗粒催化剂的合成，用于将二氧化碳转化为甲醇。该项目解决了现有催化剂的弱点，以提高二氧化碳的转化率，并进一步促进甲醇作为可再生能源载体。科学目标是：(i)优化cu基纳米颗粒的界面活性位点以提高催化活性，（ii）确定提供稳定的纳米颗粒聚集的合成条件，以及（iii）优化cu基纳米颗粒的双金属组成以提高反应选择性。实验方法使用自旋涂层在环境压力和温度下合成金属有机框架（MOF）作为薄膜模板，这应该允许在模板去除后在工业相关支架上快速和可重复地生成纳米颗粒阵列。使用mof作为模板，在调整金属簇中心和双金属组合方面提供了极大的灵活性，并有望实现铜氧化物纳米颗粒组成的可重复修饰。该团队还致力于控制这些纳米颗粒框架内的空间和尺寸分布以及氧化态。这项工作的预期结果是促进铜基纳米颗粒催化剂的合理设计，这些催化剂具有更高的催化活性，并且通过减少聚集和优化双金属成分来提高催化效率，从而提高催化稳定性。在工业相关的载体上通过薄膜合成金属铜纳米颗粒应该为催化剂的合成和测试提供一种快速和可扩展的策略。这项研究对该领域的影响预计将是改进二氧化碳转化技术，以及为快速、可扩展的催化剂开发进行纳米颗粒分析的新策略。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

With the support of the Chemical Catalysis program in the Division of Chemistry, Kara Stowers of Brigham Young University is studying how to improve the synthesis and composition of copper catalysts for reducing carbon dioxide, an important sustainable chemistry goal. Methanol produced from carbon dioxide could be used as a fuel and material feedstock, rendering this chemistry useful for rebalancing the carbon cycle (i.e. cycling the greenhouse gas CO2 to this reduced building block form). Currently copper-based catalysts are sluggish when reacting with carbon dioxide and unstable when converting it to methanol. To improve these copper-based catalysts, an templating method will be used to rapidly create and test new nanoparticle compositions and structures for catalysis. This research aims to establish a flexible and tunable method for catalyst development, including understanding the fundamental molecular interactions of the catalyst with industrially relevant materials, with the goal of increasing catalyst stability and activity. More efficient catalysts would facilitate the transition to a sustainable closed-loop fuel economy and reduce our reliance on non-renewable fossil fuels. Additionally, this research will include student training at both the graduate and undergraduate level to help prepare the next generation of scientists and engineers dedicated to addressing pressing environmental challenges. The project also provides targeted opportunities for female freshman undergraduates to begin early engagement in research and to be provided with mentors.Under this award, Kara Stowers and her research team at Brigham Young University are studying the template-mediated synthesis of copper-based nanoparticle catalysts for the conversion of carbon dioxide to methanol. This project addresses existing catalyst weaknesses in order to improve carbon dioxide conversion and further facilitate methanol as a renewable energy carrier. The scientific goals are to (i) optimize the interface active sites of Cu-based nanoparticles to increase catalytic activity, (ii) identify synthesis conditions that provide stability against nanoparticle aggregation, and (iii) optimize bimetallic compositions of Cu-based nanoparticles to increase reaction selectivity. The experimental approach uses spin-coating to synthesize a metal organic framework (MOF) as a thin film template at ambient pressure and temperature, which should allows for the rapid and reproducible generation of arrays of nanoparticles onto industrially relevant supports after template removal. Using MOFs as a template affords extreme flexibility in tuning of metal cluster centers and bimetallic combinations, and is expected to allow for the reproducible modification of Cu-oxide nanoparticle composition. The team also aims to control spatial and size distributions and oxidation states within these nanoparticulate frameworks. The projected outcomes of the work are to facilitate rational design of Cu-based nanoparticle catalysts with improved catalytic activity, and with improved catalytic stability from reduced aggregation and bimetallic compositions optimized for improved catalytic efficiency. Synthesis of copper metal nanoparticles via thin films on industrially relevant supports should offer an expeditious and scalable strategy for catalyst synthesis and testing. The impact of this research on the field is expected to be in improved technologies for carbon dioxide conversion as well as in a new strategy to carry out nanoparticle assays for rapid, scalable catalyst development.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.