CAREER: Large-scale quantum-continuum simulation of layered metal oxide semiconductor photoelectrodes under finite-temperature electrochemical conditions

职业：有限温度电化学条件下层状金属氧化物半导体光电极的大规模量子连续模拟

• 批准号: 1654625
• 负责人: Ismaila Dabo
• 金额: $ 56.29万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-02-01 至 2022-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1654625&HistoricalAwards=false
• 关键词: CAREER; Large; scale; quantum; continuum

NON-TECHNICAL SUMMARYThe Division of Materials Research and the Division of Chemistry provide funding for this CAREER award, which supports computational research tightly integrated with educational and outreach activities aimed at broadening the palette of currently available photocatalytic materials.Solar energy is the most abundant energy source available to humankind, but this energy cannot be harnessed on demand due to the variability of sunlight. This CAREER award supports research and education in the specific area of artificial photosynthesis, which emulates natural photosynthesis, the sunlight-driven process used by plants to transform the carbon dioxide absorbed by their leaves and the water pumped by their roots into organic nutrients for supporting their survival and growth. Using artificial photosynthesis, carbon-neutral fuels can be produced.By developing accurate computer models to predict the chemical transformations that underlie artificial photosynthesis, the PI and his research team aim at answering critical questions that surround the fuel-production ability of a promising family of materials that have been shown to absorb a much larger portion of the solar spectrum than previously used materials. The outcome of this research will be to expand the palette of materials that can efficiently operate under sunlight, and develop new software for understanding how small variations in the composition of a given material can affect its ultimate fuel-production performance. The new software will be disseminated to the community through an open-source distribution.This CAREER award also supports a comprehensive educational and outreach plan to increase the participation of women and underrepresented groups in science and engineering with an emphasis on exposing them to the universe of computer programming and simulation, on developing effective teaching materials to train a computationally literate generation of young scientists and engineers, and on accelerating the emergence of a diverse and well-trained workforce in the area of materials modeling in an effort to reduce the time and cost involved in the industrial development of new energy materials.TECHNICAL SUMMARYThe Division of Materials Research and the Division of Chemistry provide funding for this CAREER award, which supports computational research tightly integrated with educational and outreach activities aimed at broadening the palette of currently available photocatalytic materials. Solar energy is the most abundant energy source available to humankind, but this energy cannot be harnessed on demand due to the variability of sunlight. Artificial photosynthesis provides a sustainable way to overcome that variability through the direct photocatalytic storage of solar power into chemical fuels; however, most of the stable photocatalysts in use today rely on metal oxide semiconductors whose bandgap does not match the solar spectrum, which greatly limits their overall performance.By developing accurate molecular and submolecular models of electrochemical reactions at the interface between a semiconductor and an electrolyte under realistic environmental conditions, the PI and his research team aim to understand, predict, and control the surface mechanisms that underlie the operation of photochemical reactors towards maximizing their fuel-production performance. This CAREER project is specifically focused on studying layered metal oxide photocatalysts that can operate optimally under sunlight. In order to predict the properties of promising layered semiconductors, the PI will exploit and further develop a newly released quantum-continuum model to perform large-scale simulations of semiconductor-solution interfaces at finite temperature, taking into account the adsorption of ions and the response of explicit water layers under applied voltage. New software will be created in the open-source Quantum-Espresso distribution to provide the computational community with a widely applicable and highly transferable modeling framework for future studies of photocatalytic mechanisms at electrified photoelectrodes. This CAREER award also supports a comprehensive educational and outreach plan to increase the participation of women and underrepresented groups in science and engineering with an emphasis on exposing them to the universe of computer programming and simulation, on developing effective teaching materials to train a computationally literate generation of young scientists and engineers, and on accelerating the emergence of a diverse and well-trained workforce in the area of materials modeling in an effort to reduce the time and cost involved in the industrial development of new energy materials.

非技术总结材料研究部和化学部为该职业奖提供资金，该奖项支持与教育和推广活动紧密结合的计算研究，旨在扩大现有光催化材料的范围。太阳能是人类可用的最丰富的能源，但由于阳光的多变性，这种能源无法按需利用。该职业奖支持人工光合作用特定领域的研究和教育，人工光合作用模仿自然光合作用，植物利用阳光驱动的过程将叶子吸收的二氧化碳和根部泵出的水转化为有机营养素，以支持其生存和生长。通过开发精确的计算机模型来预测人工光合作用背后的化学转化，PI和他的研究团队旨在回答围绕一种有前途的材料家族的燃料生产能力的关键问题，这些材料已被证明比以前使用的材料吸收更大部分的太阳光谱。这项研究的结果将是扩大可以在阳光下有效运行的材料的调色板，并开发新的软件来了解给定材料成分的微小变化如何影响其最终的燃料生产性能。新的软件将通过开放源代码分发到社区。这个职业奖还支持一个全面的教育和推广计划，以增加妇女和代表性不足的群体在科学和工程领域的参与，重点是让她们接触计算机编程和模拟的世界，开发有效的教学材料，以培养一代懂计算的年轻科学家和工程师，以及加速材料建模领域多样化和训练有素的劳动力的出现，以减少新能源材料工业开发的时间和成本。技术总结材料研究部和化学部为该职业奖提供资金，它支持与教育和推广活动紧密结合的计算研究，旨在扩大目前可用的光催化材料的调色板。太阳能是人类可利用的最丰富的能源，但由于阳光的可变性，这种能源不能按需利用。人工光合作用通过将太阳能直接光催化储存为化学燃料，提供了一种克服这种可变性的可持续方法;然而，目前使用的大多数稳定的光催化剂依赖于其带隙与太阳光谱不匹配的金属氧化物半导体，通过开发半导体和半导体之间界面处电化学反应的精确分子和亚分子模型，PI和他的研究团队的目标是了解，预测和控制光化学反应器操作的表面机制，以最大限度地提高其燃料生产性能。这个CAREER项目特别专注于研究可以在阳光下最佳运行的层状金属氧化物光催化剂。为了预测有前途的层状半导体的性质，PI将利用并进一步开发新发布的量子连续模型，在有限温度下对半导体-溶液界面进行大规模模拟，同时考虑到离子的吸附和外加电压下显式水层的响应。新软件将在开源Quantum-Espresso发行版中创建，为计算社区提供广泛适用且高度可转移的建模框架，用于未来研究带电光电极的光催化机制。该职业奖还支持一项全面的教育和推广计划，以增加妇女和代表性不足的群体在科学和工程领域的参与，重点是使她们接触计算机编程和模拟的世界，开发有效的教材，以培训具有计算能力的一代年轻科学家和工程师，以及加速材料建模领域多样化和训练有素的劳动力的出现，以努力减少新能源材料工业开发所涉及的时间和成本。

项目成果

BaZrSe 3: Ab initio study of anion substitution for bandgap tuning in a chalcogenide material

BaZrSe 3：硫族化物材料中用于带隙调节的阴离子取代的从头算研究

• DOI: 10.1063/1.5097940
• 发表时间: 2019
• 期刊: Journal of Applied Physics
• 影响因子: 3.2
• 作者: Ong, Marc;Guzman, David M.;Campbell, Quinn;Dabo, Ismaila;Jishi, Radi A.
• 通讯作者: Jishi, Radi A.

First-principles investigation of BiVO3 for thermochemical water splitting

• DOI: 10.1016/j.ijhydene.2018.11.125
• 发表时间: 2019-01-15
• 期刊: INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
• 影响因子: 7.2
• 作者: Ong, Marc;Campbell, Quinn;Jishi, Radi A.
• 通讯作者: Jishi, Radi A.

Quantum-continuum calculation of the surface states and electrical response of silicon in solution

• DOI: 10.1103/physrevb.95.205308
• 发表时间: 2017-01
• 期刊: Physical Review B
• 影响因子: 3.7
• 作者: Q. Campbell;I. Dabo

Voltage-dependent cluster expansion for electrified solid-liquid interfaces: Application to the electrochemical deposition of transition metals

• DOI: 10.1103/physrevb.96.205134
• 发表时间: 2017-08
• 期刊: Physical Review B
• 影响因子: 3.7
• 作者: Stephen E. Weitzner;I. Dabo

Electrochemical stability and light-harvesting ability of silicon photoelectrodes in aqueous environments

水环境中硅光电极的电化学稳定性和光捕获能力

• DOI: 10.1063/1.5093810
• 发表时间: 2019
• 期刊: The Journal of Chemical Physics
• 作者: Campbell, Quinn;Dabo, Ismaila
• 通讯作者: Dabo, Ismaila