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

通过这个奖项，化学系的化学催化项目正在支持dr。威斯康星大学麦迪逊分校的Song Jin和Jordan Schmidt将理论与实验相结合，设计、开发和理解新的电化学方法，从分子氧中生成过氧化氢（H2O2）。过氧化氢（H2O2）是一种环境友好的氧化剂，具有许多工业和环境应用。一般来说，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H2O2的商业化生产存在成本、能耗和安全问题。为了在经济上具有竞争力，目前的工艺是在一些大型的、集中的制造工厂中实行的。相比之下，小规模、分散、现场用电直接从氧气中生产H2O2可能是更有效和可持续的方法。然而，电化学处理H2O2的方法需要更高效、成本更低才可行。该项目的成功可以促进H2O2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外展组成部分，并寻求通过包容性培训建立一支更加多样化的科学队伍。Song Jin和Jordan Schmidt及其团队将理论与实验相结合，利用未开发的金属化合物电催化剂的独特属性，设计、开发和理解基于金属硫族化合物的新型选择性电催化剂，用于在酸性和中性溶液中进行选择性双电子氧还原反应（2e ORR）。这种选择性2e ORR电催化剂可以促进H2O2的分散电化学生产，H2O2是一种无害环境的氧化剂，在工业、环境和医疗保健环境中有着广泛的应用。密度泛函理论计算和动力学模型为过渡金属硫族化合物的活性和选择性提供了详细的见解，并为后续的合成和性能评估确定了有前途的候选结构。电化学和（原位）光谱研究揭示了催化剂的活性、选择性和依赖于电位的反应中间体，计算检验提供了对催化机理的机理见解，并进一步设计了控制催化剂选择性和稳定性的原则。理解和合理设计复杂金属化合物催化剂，以实现各种选择性电催化反应，可以为复杂结构基序如何影响催化剂活性和选择性提供基础和可转移的见解。该项目的成功还可以促进高效的分散电化学生产H2O2，因此具有广泛的科学和社会影响的潜力。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 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.