DMREF: INFEWS: Collaborative Research: Photocatalyst by Design: Computational Screening of Reconstructed Perovskite Semiconductor Electrodes for Efficient Solar-to-Fuel Conversion

DMREF：INFEWS：协作研究：光催化剂设计：用于高效太阳能到燃料转换的重构钙钛矿半导体电极的计算筛选

• 批准号: 1729338
• 负责人: Ismaila Dabo
• 金额: $ 71.66万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-10-01 至 2021-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1729338&HistoricalAwards=false
• 关键词: DMREF; INFEWS; Collaborative; Research; Photocatalyst

Non-technical Abstract: The production of hydrogen fuel from sunlight and seawater has the potential to profoundly reshape the food-energy-water (FEW) landscape and to revolutionize the generation of electric power for transportation and residential applications. Hydrogen is a sustainable energy carrier whose catalytic reaction with oxygen generates electrical energy and heat without emitting carbon dioxide; the only byproduct of this reaction is clean water. Solar-to-hydrogen conversion offers the advantage of not requiring agricultural resources to produce synthetic fuels, overcoming one of the major constraints currently imposed on the FEW supply. The goal of this collaborative research is to develop a widely applicable computational protocol, which will be supported by a high-throughput cyberinfrastructure and validated against experimental data, to accelerate the selection of photoactive materials that can efficiently split water (H2O) into hydrogen (H2) and oxygen (O2). At the educational level, this project will promote the emergence of a diverse and well-trained workforce accustomed to collaboration at the frontier of data-driven theory, computation, and experimentation towards solving the outstanding challenges of materials design, which are facing the global FEW system in the twenty-first century.Technical Abstract: To accelerate the design of new photocatalysts, the research team will exploit novel computational capabilities that extend the scope of conventional quantum-mechanical simulations in describing solar-to-hydrogen conversion. An integrated experimental and computational cycle will be followed to validate the theoretical approach and to assess the effectiveness of advanced performance metrics for the successful selection of new classes of photocatalysts. Specifically, the Schottky barrier height, which sets an upper limit for the solar-to-hydrogen turnover number, will be used as an aggregate of the various performance parameters that collectively contribute to photocatalytic activity. Ultimately, this work will deliver a robust high-throughput framework to guide the optimization of novel photocatalysts with an initial focus on oxynitride and oxysulfide perovskites, taking into account realistic synthetic constraints and conditions of operation. Beyond exploring innovative solutions for solar-to-hydrogen production, the team participants have been and will continue to be actively involved in outreach and undergraduate mentoring in an effort to significantly increase the participation of women and underrepresented minorities in science and engineering and build effective collaborations with international institutions.

摘要：从阳光和海水中生产氢燃料有可能深刻地重塑食物-能源-水（FEW）景观，并彻底改变交通和住宅应用的电力生产。氢是一种可持续的能量载体，它与氧催化反应产生电能和热能而不排放二氧化碳；这个反应的唯一副产品是干净的水。太阳能制氢的优势在于不需要农业资源来生产合成燃料，克服了目前对少数几种燃料供应施加的主要限制之一。这项合作研究的目标是开发一种广泛适用的计算协议，该协议将得到高通量网络基础设施的支持，并根据实验数据进行验证，以加速能够有效地将水（H2O）分解为氢（H2）和氧（O2）的光活性材料的选择。在教育层面，该项目将促进多样化和训练有素的劳动力队伍的出现，他们习惯于在数据驱动理论、计算和实验的前沿进行合作，以解决二十一世纪全球FEW系统面临的材料设计的突出挑战。技术摘要：为了加速新型光催化剂的设计，研究团队将开发新的计算能力，扩展传统量子力学模拟的范围，以描述太阳能到氢的转化。综合实验和计算周期将遵循验证理论方法，并评估先进性能指标的有效性，以成功选择新型光催化剂。具体来说，肖特基势垒高度为太阳能转化为氢的数量设定了上限，它将被用作各种性能参数的集合，这些参数共同有助于光催化活性。最终，这项工作将提供一个强大的高通量框架来指导新型光催化剂的优化，最初的重点是氮化氧和硫化氧钙钛矿，考虑到现实的合成限制和操作条件。除了探索太阳能制氢的创新解决方案外，团队参与者一直并将继续积极参与外展和本科生指导，努力显著提高女性和代表性不足的少数民族在科学和工程领域的参与度，并与国际机构建立有效的合作。

项目成果

Colloidal Nanoparticles of a Metastable Copper Selenide Phase with Near-Infrared Plasmon Resonance

• DOI: 10.1021/acs.chemmater.0c04058
• 发表时间: 2020-12
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: Robert W. Lord;J. Fanghanel;Cameron F. Holder;I. Dabo;R. Schaak

Data-driven analysis of the electronic-structure factors controlling the work functions of perovskite oxides

控制钙钛矿氧化物功函数的电子结构因素的数据驱动分析

• DOI: 10.1039/d0cp05595f
• 发表时间: 2021
• 期刊: Physical Chemistry Chemical Physics
• 影响因子: 3.3
• 作者: Xiong, Yihuang;Chen, Weinan;Guo, Wenbo;Wei, Hua;Dabo, Ismaila
• 通讯作者: Dabo, Ismaila

Phase-Selective Solution Synthesis of Perovskite-Related Cesium Cadmium Chloride Nanoparticles

• DOI: 10.1021/acs.inorgchem.0c01574
• 发表时间: 2020-08-17
• 期刊: INORGANIC CHEMISTRY
• 影响因子: 4.6
• 作者: Holder, Cameron F.;Fanghanel, Julian;Schaak, Raymond E.
• 通讯作者: Schaak, Raymond E.

Understanding the Photoelectrochemical Properties of Theoretically Predicted Water‐Splitting Catalysts for Effective Materials Discovery

了解理论预测的水分解催化剂的光电化学性质，以实现有效的材料发现

• DOI: 10.1002/aenm.202201869
• 发表时间: 2022
• 期刊: Advanced Energy Materials
• 影响因子: 27.8
• 作者: Katzbaer, Rowan R.;Theibault, Monica J.;Kirchner‐Hall, Nicole E.;Mao, Zhiqiang;Dabo, Ismaila;Abruña, Héctor D.;Schaak, Raymond E.
• 通讯作者: Schaak, Raymond E.

Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen

• DOI: 10.1039/d0ee02984j
• 发表时间: 2021-03-11
• 期刊: ENERGY & ENVIRONMENTAL SCIENCE
• 影响因子: 32.5
• 作者: Xiong, Yihuang;Campbell, Quinn T.;Dabo, Ismaila
• 通讯作者: Dabo, Ismaila