SusChEM: Using theory-driven design to tailor novel nanocomposite oxides for solar fuel production

SusChEM：利用理论驱动设计为太阳能燃料生产定制新型纳米复合氧化物

• 批准号: 1438721
• 负责人: Kimberly Gray
• 金额: $ 55万
• 依托单位: Northwestern University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2014
• 资助国家: 美国
• 起止时间: 2014-09-01 至 2018-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1438721&HistoricalAwards=false
• 关键词: SusChEM; Using; theory; driven; design

Title: SusChEM. The Design of Materials to Harvest and Store Solar Energy in Chemical Bonds: Tailoring nanocomposite catalytic structures for artificial photosynthesis.The basis for this proposed research is the fact that more of the sun's energy hits the face of the earth in two hours than is consumed globally in a year. Yet only minor amounts of sunlight are currently harvested to meet an ever-growing energy demand. The conversion of sunlight to chemical energy is a promising strategy to deliver greater use of solar energy and to provide a variety of possibilities for local, off-the-grid energy storage. The particular focus of this research is the light-driven conversion of CO2 that opens up new strategies for developing closed loop carbon cycles, a key aim of sustainability. To undertake this effort, an award is made to Professors Kimberly Gray, Justin Notestein and Eric Weitz of Northwestern University in line with the SusChEM initiative. An international and interdisciplinary team of catalysis experts has been assembled utilizing the US-Ireland R&D Partnership program. This international R&D Partnership leverages funding from the Irish and UK governments. This team has unparalleled capabilities to carry out theory-driven design, synthesis and testing of multifunctional catalysts that will separate and control the distinct steps of the complex series of reactions around sunlight-driven CO2 conversion. The goal is to improve the fundamental understanding of the mechanisms of CO2 photo-reduction and as a result, the achievement of much higher product yields and energy conversion efficiencies than is currently possible. Researchers on this project will also participate in a Climate Change and Sustainability Professional Development Series that connects middle and high school teachers to cutting-edge academic research and provide STEM enrichment to a racially and economically diverse student population.The photochemical fixation of CO2 to energy rich products, essentially artificial photosynthesis, whether for solar energy storage or the production of potential feedstock chemicals, involves an exceedingly complex system of reactions requiring novel, multifunctional nanoarchitectures that can harvest visible light, stabilize charge separation, reduce the heterogeneity of surface sites, activate CO2, and control the reaction pathway. The overarching hypothesis of the proposed work is that multi-functional nanocomposite metal oxide clusters supported on a semiconductor surface that couple photo- and thermal catalysis can be designed from first principles, and then synthesized and engineered in order to convert CO2 to useful two-electron reduction products selectively and with greatly improved efficiency. The research integrates theory, synthesis, characterization, mechanism interrogation and application and links the efforts of three research teams in a coordinated fashion providing feedback to inform next steps. First principles modeling will be used to design nanostructures tailored to CO2 conversion, followed by sophisticated and controlled synthesis techniques to execute these designs and then, the verification of their efficacy by rigorous structural and functional characterization and scaled-up engineering testing. This is feasible only through a team effort, which will then offer a compelling and potentially transformative strategy to improve fundamentally the efficiency and selectivity of CO2 reduction chemistry and process engineering.

标题：中国农业大学 通过化学键收集和储存太阳能的材料设计：为人工光合作用量身定制纳米复合催化结构。这项研究的基础是这样一个事实，即两小时内照射到地球表面的太阳能比全球一年消耗的太阳能还要多。 然而，目前只有少量的阳光被收集来满足不断增长的能源需求。 将太阳光转化为化学能是一种很有前途的战略，可以更好地利用太阳能，并为当地的离网储能提供各种可能性。 这项研究的重点是光驱动的二氧化碳转化，为开发闭环碳循环开辟了新的战略，这是可持续发展的一个关键目标。 为了开展这项工作，西北大学的Kimberly Gray、Justin Notestein和Eric Weitz教授根据SusChEM倡议获得了一个奖项。利用美国-爱尔兰研发伙伴关系计划，组建了一个国际和跨学科的催化专家团队。这一国际研发伙伴关系利用爱尔兰和英国政府的资金。该团队具有无与伦比的能力，可以进行理论驱动的设计，合成和测试多功能催化剂，这些催化剂将分离和控制围绕阳光驱动的CO2转化的复杂系列反应的不同步骤。目标是提高对CO2光还原机制的基本理解，从而实现比目前可能的更高的产品产量和能量转换效率。该项目的研究人员还将参加气候变化和可持续发展专业发展系列，将初中和高中教师与尖端学术研究联系起来，并为种族和经济多样化的学生群体提供STEM丰富。将CO2光化学固定到能源丰富的产品，本质上是人工光合作用，无论是用于太阳能储存还是生产潜在的原料化学品，涉及一个非常复杂的反应系统，需要新型的多功能纳米结构，可以收集可见光，稳定电荷分离，减少表面位点的异质性，激活CO2，并控制反应途径。所提出的工作的首要假设是，支持在半导体表面上的多功能纳米复合材料金属氧化物簇，可以从第一原理设计光催化和热催化，然后合成和工程化，以将CO2转化为有用的双电子还原产物选择性和大大提高效率。该研究整合了理论，合成，表征，机制询问和应用，并以协调的方式将三个研究团队的努力联系起来，提供反馈，为下一步提供信息。第一原理建模将用于设计针对CO2转化的纳米结构，然后通过复杂和受控的合成技术来执行这些设计，然后通过严格的结构和功能表征以及按比例放大的工程测试来验证其功效。这只有通过团队的努力才是可行的，这将提供一个引人注目的和潜在的变革性战略，从根本上提高二氧化碳还原化学和工艺工程的效率和选择性。