CAS: Single-Molecule Specific Voltammetry: Quantifying Reaction Products of Electrocatalysis at Single Particle Level

在化学测量成像计划的支持下&，以及大分子，超分子和纳米化学计划的部分共同资助;化学催化;化学结构，动力学和机制- A，张教授和他在马萨诸塞州-达特茅斯大学的研究小组正在开发一种新的化学分析工具，以详细研究与二氧化碳（CO2）转化相关的电化学反应机制。减少有害物质，这是缓解气候变化的一条有希望的途径。具体来说，该团队正在开发一种名为单分子特异性（SMS）伏安法的新技术，以探测单个纳米颗粒作为CO2还原反应催化剂的性能。这项研究可能会提高我们设计有效将二氧化碳转化为燃料的电催化剂的能力。一个广泛的教育项目向本科生和研究生介绍了这项研究，并包括外展活动，以激励代表性不足的K-12学生在南马萨诸塞州追求STEM领域的职业生涯。该项目旨在开发一个平台，以量化单个纳米颗粒上电化学CO2还原的产物，并揭示纳米电催化剂的形态依赖性性能和稳定性。一氧化碳（CO）在Au纳米颗粒上的形成被用作模型反应。具体而言，该研究旨在解决以下目标：（1）证明单分子特异性（SMS）伏安法定量单个纳米颗粒上CO形成的能力。(2)颗粒间和颗粒内不均匀性对单一电催化剂上CO生成的影响的评估。(3)确定CO2还原反应期间纳米颗粒不稳定性的机制。通过结合SMS伏安法、超分辨率荧光和电子显微镜，研究团队正在努力阐明CO形成的形态依赖性活性，并超分辨率单个纳米电催化剂上的面依赖性活性位点。提高对电催化剂的活性和稳定性之间的相关性的理解以及CO2还原中纳米颗粒不稳定性的起源是平行的目标。这些研究工作的设想，以提供合理设计的nanoelectrocatalysts为CO2还原reactions.This奖项反映了NSF的法定使命，并已被认为是值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持所需的知识。

With support from the Chemical Measurement & Imaging program, and partial co-funding from programs in Macromolecular, Supramolecular, and Nanochemistry; Chemical Catalysis; and Chemical Structure, Dynamics, and Mechanisms – A, Professor Chang and his research team at the University of Massachusetts - Dartmouth are developing a new chemical analysis tool to enable detailed studies of electrochemical reaction mechanisms associated with conversion of carbon dioxide (CO2) to less harmful materials, a promising route to mitigating climate change. Specifically, the team is developing a novel technique, named single-molecule specific (SMS) voltammetry, to probe the performance of single nanoparticles as catalysts for CO2 reduction reactions. The research may advance our ability to design electrocatalysts that efficiently convert CO2 into fuels. A broad educational program introduces this research to undergraduate and graduate students, and includes outreach activities to inspire underrepresented K-12 students in South Massachusetts to pursue careers in STEM fields.This project aims to develop a platform to quantify the products of electrochemical CO2 reduction on single nanoparticles, and to reveal the morphology-dependent performance and stability of nanoelectrocatalysts. Carbon monoxide (CO) formation on Au nanoparticles is used as a model reaction. Specifically, the research is addressing the following objectives: (1) Demonstration of the ability of single-molecule specific (SMS) voltammetry to quantify CO formation on single nanoparticles. (2) Assessment of the effects of interparticle and intraparticle heterogeneity on CO formation on single electrocatalysts. (3) Identification of the mechanism(s) of nanoparticle instability during CO2 reduction reactions. By combining SMS voltammetry, super-resolution fluorescence, and electron microscopies, the research team is striving to elucidate the morphology-dependent activity for CO formation and super-resolve the facet-dependent active sites on single nanoelectrocatalysts. Improved understanding of the correlation between the activity and stability of electrocatalysts and the origin of nanoparticle instability in CO2 reduction are parallel aims. These research efforts are envisioned to provide the knowledge needed for rational design of nanoelectrocatalysts for CO2 reduction reactions.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.