Collaborative Research: Experimental and Computational Studies on CO2 Photoreduction to Fuels by Nanostructured Catalysts

机构：威斯康星大学密尔沃基分校/亚利桑那州立大学标题：合作研究：纳米结构催化剂将二氧化碳光还原为燃料的实验和计算研究知识产权来自大气的二氧化碳（CO2）是生产可再生燃料的潜在可持续碳来源。 将CO2和水光催化转化为碳氢化合物是一种特别有吸引力的途径，因为它使用太阳能作为还原电子的来源来驱动这一转化过程。 然而，由于CO2稳定的热力学性质，CO2的光催化还原是一项极具挑战性的任务。CO2转化率低要求更有效的光催化剂，但高效的光催化剂的发展需要了解CO2？催化剂的相互作用和电子转移途径推导出的计算研究在分子水平上。拟议研究的总体目标是通过操纵催化剂成分和纳米结构，利用太阳辐射以高转化效率将CO2光催化还原为燃料（CO，甲烷，甲醇和其他碳氢化合物）。为此，拟议的研究有三个目标。 第一个目标是制造纳米结构的光催化剂，特别是板钛矿含混合相二氧化钛纳米粒子与控制相含量，如晶格掺杂的碘和表面铜簇，以实现可见光响应性和促进电荷分离。 第二个目的是发展对混合相催化剂性质和电荷分离机理的基本理解（例如，锐钛矿-板钛矿）纳米晶界面。 第三个目的是优化催化剂组合物和纳米结构（例如，TiO 2相组成、晶体尺寸、表面结构、掺杂剂浓度等）以协同提高CO2光还原效率。 在这方面，拟议的研究将整合实验和计算方法，以评估板钛矿基催化剂对CO2光还原的活性，并将推进材料科学，表面化学，纳米技术和纳米技术等多学科领域的基本理解。更广泛的影响将CO2和水光还原为碳氢化合物燃料的过程解决了温室气体管理和可再生燃料生产同时面临的挑战。 教育和外联活动将在拟议研究的范围内进行。与二氧化碳减排和太阳能燃料相关的主题将被纳入亚利桑那州立大学（ASU）和威斯康星大学密尔沃基分校（UWM）的太阳能工程，化学反应器设计和空气质量工程课程。 亚利桑那州立大学通过伊拉协会赞助的外联活动。富尔顿工程学院（IAFSE）将为来自代表性不足群体的学生以及当地教师提供太阳能燃料方面的实践经验。 还将制作一个关于阳光转化二氧化碳的动画教育模块，以吸引学生和公众的参与。这一单元将张贴在主要调查员的网站以及亚利桑那州立大学国际农林科学和环境学院外联网站上。 UWM的免费推广活动将通过威斯康星州密尔沃基的城市生态中心（UEC）进行协调，该中心与44所市中心的小学和高中建立了伙伴关系，并提供？户外教室？在城市青年的科学教育中。

Institution: University of Wisconsin-Milwaukee / Arizona State UniversityTitle: Collaborative Research: Experimental and Computational Studies on CO2 Photoreduction to Fuels by Nanostructured CatalystsIntellectual MeritCarbon dioxide (CO2) from the atmosphere is a potentially sustainable source of carbon for the production of renewable fuels. The photocatalytic conversion of CO2 and water to hydrocarbons is a particularly attractive route, as it uses solar energy as the source of reducing electrons to drive this conversion process. However, the photocatalytic reduction of CO2 is an extremely challenging task due to the stable thermodynamic properties of CO2. The low yield of CO2 conversion calls for more efficient photocatalysts, but the development of efficient photocatalysts requires understanding of CO2?catalyst interactions and electron transfer pathways deduced from computational studies at the molecular level. The overall objective of the proposed research is to use solar radiation to photocatalytically reduce CO2 to fuels (CO, methane, methanol, and other hydrocarbons) at high conversion efficiency through manipulation of catalyst composition and nanostructure. Toward this end, the proposed research has three objectives. The first objective is to fabricate nanostructured photocatalysts, specifically brookite-containing mixed-phase TiO2 nanoparticles with controlled phase contents such as lattice-doped iodine and surface Cu clusters, to achieve visible light responsiveness and facilitate charge separation. The second objective is to develop a fundamental understanding of the catalyst properties and charge separation mechanism at the mixed-phase (e.g., anatase-brookite) nanocrystalline interfaces through closely coupled experiments and computational chemistry (density functional theory) modeling. The third objective is to optimize catalyst composition and nanostructure (e.g., TiO2 phase composition, crystal size, surface structures, dopant concentration, etc.) to synergistically improve CO2 photoreduction efficiency. In this regard, the proposed research will integrate experimental and computational approaches to evaluate brookite-based catalyst activity toward CO2 photoreduction, and will advance fundamental understanding in the multidisciplinary areas of material science, surface chemistry, photocatalysis, and nanotechnology. Broader ImpactsProcesses for photoreduction of CO2 and water to hydrocarbon fuels tackle the simultaneous challenges of greenhouse gas management and renewable fuels production. The educational and outreach activities will be in the context of the proposed research. Topics related to CO2 reduction and solar fuels will be incorporated into solar engineering, chemical reactor design, and air quality engineering courses at Arizona State University (ASU) and the University of Wisconsin-Milwaukee (UWM). Outreach activities at ASU sponsored though the Ira A. Fulton Schools of Engineering (IAFSE) will provide hands-on experiences in solar fuels to students from underrepresented groups as well as local teachers. An animated educational module on CO2 conversion by sunlight will also be created to engage students and the general public. This module will be posted on the websites of the principal investigators as well as on the ASU IAFSE outreach website. Complimentary outreach activities at UWM will be coordinated through the Urban Ecology Center (UEC) in Milwaukee, Wisconsin, who has partnerships with forty-four inner-city elementary and high schools and provides ?outdoor classrooms? in science education for urban youth.