Collaborative Research: Beyond the Single-Atom Paradigm: A Priori Design of Dual-Atom Alloy Active Sites for Efficient and Selective Chemical Conversions

合作研究：超越单原子范式：双原子合金活性位点的先验设计，用于高效和选择性化学转化

• 批准号: 2334970
• 负责人: Charles Sykes
• 金额: $ 32万
• 依托单位: Tufts University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-03-01 至 2027-02-28
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2334970&HistoricalAwards=false
• 关键词: Collaborative; Research; Beyond; Single; Atom

With support from the Chemical Structure, Dynamics, and Mechanisms A (CSDM-A) program in the Division of Chemistry, Matthew Montemore of Tulane University and Charles Sykes of Tufts University are performing computational and experimental investigations of a novel class of dual-atom catalysts using quantum chemistry, machine learning, and atomic-scale characterization. These novel materials, termed dual-atom alloys, consist of an energetically stable pair of different metal atoms embedded in the surface of a host metal. Compared to single-atom alloys, a similar class of materials with well-defined active sites, dual-atom alloy active sites are anticipated to be more reactive and enable more challenging reactions including targeted bond scission. However, accelerating the discovery of novel alloys requires addressing numerous challenges including identifying promising combinations of metals from the large materials space of potential pairings, understanding their structure/function relationships, and creating an effective feedback loop between experiment and computation. Dr. Montemore and his students will use machine learning combined with density functional theory (DFT) to identify candidate structures based on surface stability and low energy barriers for specific chemical reactions. Dr. Sykes and his students will experimentally synthesize, characterize, and test the predicted structures. Their discoveries could lead to the development of an entirely new class of catalysts where well-defined metal atomic structures can be combined with predictive models to accelerate a range of multistep reaction mechanisms. In addition to these broad scientific impacts, this project will also support a virtual reality K-12 outreach workshop, provide mentorship for Hispanic scientists and engineers, and inspire students from underserved high schools by facilitating a Reverse Science Fair.Dual-atom alloys leverage several of the advantages of single-atom alloys: a well-defined active site that allows clear correspondence across computation, surface science, and reactor studies; opportunities to deviate from linear correlations in reaction energetics; and unique electronic structure. Just as with single-atom alloys, in which surface science experiments and computation preceded catalyst synthesis and testing, Montemore and Sykes will couple theory and surface science experiments to explore dual-atom alloy structure-reactivity space. This research is expected to lead to the development of structure-function relationships on a broad set of well-defined active sites, which would then serve as a guide to the larger heterogenous catalysis community. Furthermore, these studies have the potential to uncover new classes of materials with high catalytic performance, a particular need for reactions that are challenging with traditional heterogeneous catalysts, such as selective cross-couplings.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.

在化学结构，动力学和机制A（CSDM-A）方案的支持下，图兰大学的Matthew Montemore和Tufts University的Charles Sykes正在使用量子化学，机器学习，机器学习，和原子质尺度表征进行新颖的双原子催化剂进行计算和实验研究。这些新型材料称为双原子合金，由嵌入宿主金属表面的一对稳定的不同金属原子组成。与单原子合金相比，具有定义明确的活性位点的类似类似的材料，预计双原子合金活性位点将具有更具反应性，并且能够更具挑战性的反应，包括靶向债券分裂。 但是，加速新型合金的发现需要应对众多挑战，包括从潜在配对的大材料空间中识别出有希望的金属组合，了解其结构/功能关系，并在实验和计算之间创建有效的反馈回路。 Montemore博士和他的学生将使用机器学习与密度功能理论（DFT）相结合，以基于表面稳定性和特定化学反应的低能障碍物来识别候选结构。 Sykes博士和他的学生将在实验中综合，表征和测试预测的结构。他们的发现可能导致一类全新的催化剂的发展，其中定义明确的金属原子结构可以与预测模型相结合，以加速一系列多步反应机制。除了这些广泛的科学影响外，该项目还将支持虚拟现实K-12外展研讨会，为西班牙裔科学家和工程师提供指导，并通过促进反向科学博览会来激发来自服务不足的高中的学生。Diual-atom Alloys合金利用了单位质量的几种效果，可以进行良好的现场研究：既明确的现场又一次反应，又可以进行反应跨度的计算，计算;有机会偏离反应能量学中线性相关性；和独特的电子结构。就像单原子合金一样，在催化剂合成和测试之前，Montemore和Sykes将表面科学实验和计算在该合金之前进行理论和表面科学实验，以探索双原子合金结构反应空间。预计这项研究将导致在一系列明确定义的活性站点上发展结构功能关系的发展，然后将其作为更大的异质催化界的指南。此外，这些研究有可能发现具有高催化性能的新型材料，特别需要对传统的异构催化剂（例如选择性跨耦合）进行挑战。该奖项反映了NSF的法定任务，并通过使用该基金会的知识优点和广泛影响来评估NSF的法定任务，并被认为是值得的支持。