Enhancing CO2 Reduction by Controlling the Ensemble of Active Sites

通过控制活动站点的整体来加强二氧化碳减排

• 批准号: 1930013
• 负责人: Chao Wang
• 金额: $ 45.7万
• 依托单位: Johns Hopkins University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-09-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1930013&HistoricalAwards=false
• 关键词: Enhancing; CO2; Reduction; Controlling; Ensemble

Artificial carbon recycling, using waste CO2 as a starting material, is a promising solution for energy and environmental sustainability. The investigators aim to develop catalysts which more efficiently incorporate CO2 into precursors for commercial products or into liquid fuels such as ethanol, thus re-using CO2 generated as waste from burning fossil fuels. The main challenge to efficiently catalyzing these reactions is balancing the binding of the reactants with the release of the products. The investigators predict that using a core of a weakly binding first metal, with dispersed atoms of a strongly binding second metal over its surface, will result in an optimum balance of binding properties and increase the efficiency of the catalyzed reaction. The investigators will vary amount of the strongly binding metal on the catalyst's surface, then characterize its structure and test its effectiveness. The catalyst compositions and design rules resulting from this investigation are expected to encourage incorporating waste CO2 into fuels and commercial products. The investigators' educational goals are to provide hands-on laboratory training to graduate and undergraduate students and to promote learning for K-12 students with a strong focus on underrepresented groups by partnering with the Women in Science and Engineering and Family Academic Program organizations. The investigators aim to develop fundamental understanding of the CO2 reduction electrocatalysis on practical high-surface-area catalysts by synthesizing mixed-metal nanoparticle catalysts containing a weakly binding M1 core (M1 = Au, Ag, Cu) with varying amounts of strongly binding M2 atoms (M2 = Ni, Pd, Pt) dispersed over the surface. They will test the hypothesis that catalysts with discrete, atomically dispersed ensembles of M2 on the surface of M1, will exhibit the advantages of both M1 and M2 and will show to enhanced energy efficiency and reaction rate for CO2 reduction as compared to monometallic catalysts. The activity of these catalysts will be evaluated using batch electrolysis and gas-diffusion electrode cells. The surface structure and absorption properties will be probed using state-of-the-art electron microscopy and X-ray spectroscopic characterizations, surface-specific electrochemical analysis and product-resolved electrocatalytic studies. These experimental efforts will be focused using results from density functional theory and cluster expansion calculations. The methods and concepts established during this study are expected to be generally applicable to other catalytic materials and reactions, shedding new light on the development of heterogeneous catalysts using the knowledge acquired in the investigation of these bimetallic M2@M1 nanoparticles.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.

利用废弃的二氧化碳作为起始材料的人工碳回收是能源和环境可持续性的一个有前途的解决方案。研究人员的目标是开发催化剂，更有效地将二氧化碳转化为商业产品的前体或乙醇等液体燃料，从而重新利用燃烧化石燃料产生的二氧化碳废物。有效催化这些反应的主要挑战是平衡反应物的结合与产物的释放。研究人员预测，使用弱结合第一金属的核心，在其表面上分散有强结合第二金属的原子，将导致结合性能的最佳平衡，并提高催化反应的效率。研究人员将改变催化剂表面上强结合金属的量，然后表征其结构并测试其有效性。从这项调查中得到的催化剂组合物和设计规则，预计将鼓励将废二氧化碳纳入燃料和商业产品。调查人员的教育目标是为研究生和本科生提供动手实验室培训，并通过与科学与工程和家庭学术计划组织的女性合作，促进K-12学生的学习，重点关注代表性不足的群体。研究人员的目标是通过合成混合金属纳米颗粒催化剂，对实际高表面积催化剂上的CO2还原电催化作用进行基本了解，该催化剂含有弱结合的M1核心（M1 = Au，Ag，Cu），并具有分散在表面上的不同量的强结合的M2原子（M2 = Ni，Pd，Pt）。他们将测试这样的假设，即在M1表面上具有离散的、原子分散的M2集合体的催化剂将表现出M1和M2两者的优点，并且与单组分催化剂相比，将显示出提高的能量效率和用于CO2还原的反应速率。这些催化剂的活性将使用分批电解和气体扩散电极池进行评价。的表面结构和吸收特性将使用最先进的电子显微镜和X射线光谱表征，表面特定的电化学分析和产品解决电催化研究进行探测。这些实验工作将集中使用密度泛函理论和集群扩展计算的结果。本研究中建立的方法和概念有望普遍适用于其他催化材料和反应，利用在这些研究中获得的知识，对非均相催化剂的发展提供了新的认识。M1纳米颗粒。该奖项反映了NSF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进行评估，被认为值得支持的搜索.

项目成果

Asymmetrical C–C Coupling for Electroreduction of CO on Bimetallic Cu–Pd Catalysts

• DOI: 10.1021/acscatal.2c00646
• 发表时间: 2022-04
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Hao Shen;Yunzhe Wang;Tanmoyendu Chakraborty;Guangye Zhou;Canhui Wang;Xianbiao Fu;Yuxuan Wang;Jinyi Zhang;Chenyang Li;Fei Xu;Liang Cao;Tim Mueller;Chao Wang