Collaborative Research: Design and Discovery of Entropy-Stabilized Perovskite Halides for Optoelectronics

合作研究：用于光电子学的熵稳定钙钛矿卤化物的设计和发现

• 批准号: 2421149
• 负责人: Liping Yu
• 金额: $ 35万
• 依托单位: The University of Central Florida Board of Trustees
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-03-01 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2421149&HistoricalAwards=false
• 关键词: Collaborative; Research; Design; Discovery; Entropy

PART 1: NON-TECHNICAL SUMMARYPerovskite halides are an exciting family of materials that can be prepared by low-temperature synthesis methods and are promising for a wide variety of optoelectronic applications. With this project, which is jointly funded by the Solid State and Materials Chemistry program in the Division of Materials Research and the Established Program to Stimulate Competitive Research (EPSCoR), a collaborative research team from the University of Maine and the University of Alabama develops, synthesizes, and investigates a new class of perovskite halides for optoelectronics. In this combined theoretical and experimental investigation, the team also evaluates the materials’ stability under ambient environmental conditions. Unlike traditional halides with two to three metal elements, these newly developed perovskite halides consist of five or more principal metal elements in nearly equal concentrations. The workplan features a closed feedback loop between theory and experiment and focuses on materials advancement by performing theoretical predictions, developing synthesis methods, characterizing optoelectronic properties, and evaluating stability under exposure to gases, light, and heat. New perovskite halide materials discovered from this project could lead to a wide variety of optoelectronic applications including solar cells, light-emitting devices, photodetectors and lasers, photoelectrochemical catalysts, radiation detectors, and sensors. This research allows project participants from interdisciplinary programs at these two universities to interact and contribute to technology development within Maine and Alabama. Three Ph.D. graduate students and six undergraduates are trained to acquire skills and competency in the three foundational pillars of computation, experiments, and data analysis which are key attributes for the next-generation workforce. STEM outreach and education activities disseminated to K-12 students, high-school teachers, and the general public within Maine and Alabama are aimed at conveying how collaborative energy-materials design-driven research is relevant to addressing societal challenges. PART 2: TECHNICAL SUMMARYThis project, which is jointly funded by the Solid State and Materials Chemistry program in the Division of Materials Research and the Established Program to Stimulate Competitive Research (EPSCoR), aims to computationally design and experimentally realize a new class of lead-free perovskite halide materials with enhanced thermodynamic and environmental stability along with desired optoelectronic properties. Entropy-stabilized perovskite halides (ESPHs) containing five or more principal metal elements are investigated for enhanced optoelectronic properties and stable environmental performance. The key hypothesis is that the configurational entropy of mixing plays a dominant role in stabilizing a single-phase crystalline ESPH structure. The validation of this hypothesis not only provides a new experimentally controllable pathway to design more stable perovskite halide materials but also yields unique composition-structure-property relationships that are absent when chemical order prevails. Specific objectives are to (i) predict the combinations of metal elements that can give rise to stable ESPHs using high-throughput first-principles calculations, (ii) synthesize the predicted ESPHs using the solid-state solution, hydrothermal, and solvent precipitation methods, (iii) characterize the compositional, structural and optoelectronic properties of the synthesized ESPHs, and (iv) evaluate and analyze the stabilities of experimentally synthesized ESPHs under various laboratory environments including humidity, oxidizing/reducing gases, and heat. New ESPHs from this project are poised to substantially expand the chemical space of perovskite halides, providing more capabilities to tune and tailor materials properties of interest (such as lattice parameter, bandgap, optical absorption strength, and conductivity) and render high potential for a wide variety of optoelectronic applications including solar cells, light-emitting devices, photoelectrochemical catalysts, photodetectors and lasers, radiation detectors, and sensors.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.

第1部分：非技术摘要底石卤化物是一种令人兴奋的材料家族，可以通过低温合成方法制备，并有望用于多种光电应用。借助该项目，该项目由材料研究部的固态和材料化学计划共同资助，以及刺激竞争研究的既定计划（EPSCOR），这是缅因州大学和阿拉巴马大学发展，合成的合作研究团队的合作研究团队，并研究了一种新的perovskite halides for Optoeleclectronics。在这一合并的理论和实验投资中，团队还评估了在环境环境条件下材料的稳定性。与传统的卤化物具有两到三个金属元素不同，这些新开发的钙钛矿卤化物包括五个或更多的主要金属元素，几乎相等。该工作场所具有理论和实验之间的封闭反馈回路，并通过执行理论预测，开发合成方法，表征光电特性以及在暴露于气体，光和热量的情况下评估稳定性来关注材料的发展。从该项目中发现的新钙钛矿卤化物材料可能会导致多种光电应用，包括太阳能电池，发光设备，光电探测器和激光器，光电化学催化剂，辐射探测器和传感器。这项研究使这两所大学跨学科计划的项目参与者可以互动并为缅因州和阿拉巴马州内的技术发展做出贡献。三博士研究生和六名本科生经过培训，可以在计算，实验和数据分析的三个基础支柱中获得技能和能力，这是下一代劳动力的关键属性。 STEM宣传和教育活动传播给K-12学生，高中老师以及缅因州和阿拉巴马州的公众旨在传达协作能源材料设计驱动的研究如何与解决社会挑战有关。第2部分：技术摘要项目是由材料研究部的固态和材料化学计划共同资助的，以及刺激竞争性研究的既定计划（EPSCOR），旨在在计算上设计，并实现了一类新的无铅Perovskite Halide材料，并具有增强的热力学和环境稳定性以及所需的型物质。研究了包含五个或更多主要金属元件的熵稳定的钙钛矿卤化物（ESPHS），以增强光电特性和稳定的环境性能。关键假设是，混合的构型熵在稳定单相晶体ESPH结构中起主要作用。该假设的验证不仅为设计更稳定的钙钛矿卤化物材料提供了新的实验控制的途径，而且还产生了独特的组成结构 - 质体关系，而当化学秩序占据时，这些关系就不存在。特定物体是（i）预测金属元件的组合，这些元素可以使用高通量的第一原理计算产生稳定的ESPH，（ii）使用固态溶液，水热和溶剂的精度和溶剂精度方法（iii）表征组合，结构和光学质量分析的合成属性和合成的质量分析，将预测的ESPH合成预测的ESPH。在各种实验室环境下实验合成的ESPH的稳定性，包括湿度，氧化/还原气体和热量。该项目的新ESPH被中毒以实质性扩大钙钛矿卤化物的化学空间，提供更多的能力来调整和量身定制感兴趣的材料特性（例如晶格参数，bandgap，bandgap，光吸收强度和电导率），并为包括多种选择的光电细胞，光仪，照明器件，照片，摄影机，光仪，摄影师，光仪，光启用器件，光仪，摄影师，光层型，光电孔，光电孔，光层，造型，赋予高潜力。激光，辐射探测器和传感器。该奖项反映了NSF的法定任务，并通过使用基金会的知识分子优点和更广泛的影响审查标准来诚实地通过评估来诚实地支持。