CAS: Design and Mechanistic Understanding of Selective Electrocatalysts Based on Earth-Abundant Metal Compounds

化学系的化学催化研究项目将支持威斯康星大学麦迪逊分校的Song Jin博士和Jordan施密特博士将联合收割机理论与实验相结合，设计、开发和理解从分子氧生成过氧化氢（H2 O2）的新电化学方法。过氧化氢（H2 O2）是一种环保氧化剂，具有许多工业和环境应用。它也是一种推荐的消毒剂，包括用于导致COVID-19大流行的新型冠状病毒。目前H2 O2的商业生产的特征在于显著的成本、能量消耗和安全问题。为了在经济上具有竞争力，目前的工艺只在少数几个大型的集中制造厂中实施。相比之下，使用电力直接从氧气中小规模、分散、现场生产H2 O2可能是一种更有效和可持续的方法。然而，H2 O2的电化学方法需要更有效且成本更低才可行。该项目的成功可以促进H2 O2的高效分散生产，并对环境，可持续性和医疗保健领域产生广泛的技术影响。该项目包括一个重要的教育推广部分，并寻求通过包容性培训建立一个更多样化的科学工作队伍。宋金博士和乔丹施密特博士及其团队将理论和实验相结合，利用未开发的金属化合物电催化剂的独特属性来设计，开发，了解基于金属硫族化物的新型选择性电催化剂，用于选择性双电子氧还原反应（2 e ORR）在酸性和中性溶液中。这种选择性2 e ORR电催化剂可以促进分散的H2 O2的电化学生产，H2 O2是一种环境友好的氧化剂，在工业、环境和医疗保健环境中具有多种应用。密度泛函理论计算和动力学模型提供了详细的洞察活动和选择性，并确定有前途的候选结构之间的过渡金属硫族化物的后续合成和性能评价。电化学和（原位）光谱研究揭示了催化剂的活性，选择性，和潜在的依赖性反应中间体，与计算检查提供机械的见解催化机制（S）和进一步的设计原则，管理催化剂的选择性和稳定性。理解和合理设计复杂的金属化合物催化剂，使各种选择性的电催化反应，可以导致基本的和可转移的见解复杂的结构基序如何影响催化剂的活性和选择性。该项目的成功还可以促进高效分散的电化学生产H2 O2，因此，具有广泛的科学和社会影响的潜力。该奖项反映了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。

With this award,the Chemical Catalysis Program of the Division of Chemistry is supporting Drs. Song Jin and Jordan Schmidt of the University of Wisconsin-Madison to combine theory and experiment to design, develop, and understand new electrochemical methods to generated hydrogen peroxide (H2O2) from molecular oxygen. Hydrogen peroxide (H2O2) is an environmentally benign oxidant with many industrial and environmental applications. It is also a recommended disinfectant in general, including for the novel coronavirus responsible for the COVID-19 pandemic. The current commercial production of H2O2 is characterized by significant cost, energy consumption, and safety concerns. To be economically competitive the current process is practiced in a few large, centralized manufacturing plants. In comparison, small scale, decentralized, on-site production of H2O2 directly from oxygen using electricity could be a more effective and sustainable approach. However, electrochemical approaches to H2O2 need to be much more efficient and less costly to be viable. The success of this project can facilitate the efficient decentralized production of H2O2 and have broad technological impacts related to the environment, sustainability, and the healthcare fiels. This project includes a significant educational outreach component and seeks to build a more diverse scientific workforce through inclusive training.Drs. Song Jin and Jordan Schmidt and their team combine theory and experiment to exploit the unique attributes of unexplored metal compound electrocatalysts to design, develop, and understand new and selective electrocatalysts based on metal chalcogenides for the selective two-electron oxygen reduction reaction (2e ORR) in acidic and neutral solutions. Such selective 2e ORR electrocatalysts can facilitate decentralized electrochemical production of H2O2, an environmentally benign oxidant with diverse applications in industrial, environmental, and healthcare settings. Density functional theory calculations and kinetic models provide detailed insights into activity and selectivity and identify promising candidate structures among transition metal chalcogenides for subsequent synthesis and performance evaluation. Electrochemical and (in situ) spectroscopic studies reveal catalyst activity, selectivity, and potential-dependent reaction intermediates, with computational examination providing mechanistic insights into the catalytic mechanism(s) and further design principles governing catalyst selectivity and stability. Understanding and rationally designing complex metal compound catalysts for enabling various selective electrocatalytic reactions can lead to fundamental and transferrable insights into how complex structural motifs influence catalyst activity and selectivity. The success of this project can also facilitate the efficient decentralized electrochemical production of H2O2 and, as such, has the potential for broad scientific and societal impact.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.