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

标题：SusChEM。以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做纳米复合催化结构。这项拟议的研究的基础是这样一个事实，即两小时内到达地球表面的太阳能量比全球一年消耗的能量还多。然而，目前只有少量的阳光被收集来满足日益增长的能源需求。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，这为开发闭合循环碳循环开辟了新的战略，这是可持续发展的关键目标。为了开展这项工作，根据SusChEM倡议，向西北大学的金伯利·格雷、贾斯汀·诺特斯坦和埃里克·韦茨教授颁发了一个奖项。利用美国-爱尔兰研发伙伴计划，已经组建了一支由催化专家组成的国际和跨学科团队。这一国际研发伙伴关系利用了来自爱尔兰和英国政府的资金。该团队拥有无与伦比的能力，可以进行理论驱动的多功能催化剂的设计、合成和测试，这些催化剂将分离和控制围绕阳光驱动的二氧化碳转化的复杂系列反应的不同步骤。其目标是提高对二氧化碳光还原机理的基本了解，从而实现比目前可能实现的更高的产品产量和能源转换效率。该项目的研究人员还将参与气候变化和可持续发展专业发展系列，该系列将中学和高中教师与尖端学术研究联系起来，并为不同种族和经济背景的学生群体提供STEM浓缩。二氧化碳与能量丰富的产品的光化学固定，基本上是人工光合作用，无论是用于太阳能储存还是生产潜在的原料化学品，涉及一个极其复杂的反应系统，需要新颖、多功能的纳米结构，可以获取可见光，稳定电荷分离，减少表面位置的异质性，激活二氧化碳，并控制反应路径。这项工作的总体假设是，负载在半导体表面的耦合光催化和热催化的多功能纳米复合金属氧化物团簇可以从第一原理设计，然后合成和工程设计，以便选择性地将二氧化碳转化为有用的两电子还原产物，并大大提高效率。这项研究集理论、综合、表征、机制询问和应用于一体，并以协调的方式将三个研究团队的努力联系在一起，提供反馈，为下一步提供信息。首先将使用原理建模来设计针对二氧化碳转化量身定做的纳米结构，然后使用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放大的工程测试来验证其有效性。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、潜在的变革性战略，从根本上提高二氧化碳减排化学和工艺工程的效率和选择性。

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.