SusChEM: Rational design of aqueous interfaces of Earth abundant and nontoxic transition metal sulfides for photocatalytic conversion of CO2 to fuels

SusChEM：地球丰富且无毒的过渡金属硫化物的水界面的合理设计，用于二氧化碳光催化转化为燃料

• 批准号: 1336845
• 负责人: Ponisseril Somasundaran
• 金额: $ 45.71万
• 依托单位: Columbia University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-08-01 至 2018-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1336845&HistoricalAwards=false
• 关键词: SusChEM; Rational; design; aqueous; interfaces

PI: Somasundaran, PonisserilProposal Number: 1336845Institution: Columbia UniversityTitle: SusChEM: Rational design of aqueous interfaces of Earth abundant and nontoxic transition metal sulfides for photocatalytic conversion of CO2 to fuelsThis project focuses on understanding aqueous interfaces of Earth abundant and nontoxic transition metal sulfides to engineer a cost-effective photo-electrocatalytic CO2 reduction system. The biggest roadblock to making scalable the sun-light powered synthesis of carbonaceous fuels from CO2 and water is the lack of a catalysts which is simultaneously efficient, cheap, and environmentally benign. The development of such a catalyst is hindered by the infancy of the mechanistic understanding of the proton-coupled multiple electron transfers involved into the CO2 reduction beyond CO and formate. The proposed interdisciplinary research will bridge this knowledge gap by systematically studying for the first time copper and iron sulfide minerals as novel and cheap photocatalytic materials. A novel molecular cocatalytic approach is suggested to overcome the thermodynamic and kinetic limitations of CO2 reduction towards energy-dense fuels. The objective is to determine the mechanisms of the reaction dependence on molecular cocatalysts at the interfaces and in bulk electrolyte, with the ultimate goal to develop more sustainable and efficient photosynthetic systems. Towards this ambitious goal, a team from Columbia University will study for the first time the multiscale physics and chemistry driving artificial photosynthesis of carbonaceous fuels by iron and copper sulfides, using advanced operando FTIR and Raman spectro-electrochemical, (photo)electrochemical, and theoretical (e.g., Density Fuction Theory) methods. The new more efficient photosynthetic systems based on copper and iron sulfides developed during the research will be a practical step towards scaling up renewable energy. It will lead to novel scalable strategies for the rational design of the interfaces of metal sulfides with water. Apart from artificial photosynthesis, this outcome can find application in immobilizing radionuclides in environmental remediation, as well as in mineral processing (selective separation) of sulfide minerals, in the design of greener chemicals. In addition, this knowledge will broaden our understanding of biogeochemical process including processes in acid-mine drainage, cycling of iron and cupper in deep oceans, and eventually the origin of life. The general results of the research and the new methodology will be included in the PI's undergraduate/graduate level courses.

主要研究者：Somasundaran，Ponisseril提案编号：1336845机构：哥伦比亚大学标题：SusChEM：合理设计地球丰富和无毒过渡金属硫化物的水界面，用于光催化转化CO2为燃料本项目的重点是了解地球丰富和无毒过渡金属硫化物的水界面，以设计具有成本效益的光电催化CO2还原系统。使由二氧化碳和水合成碳质燃料的太阳光动力合成可扩展的最大障碍是缺乏同时有效，廉价和环境友好的催化剂。这种催化剂的发展是阻碍了婴儿期的机械理解的质子耦合多电子转移参与到CO和甲酸以外的CO2还原。拟议的跨学科研究将通过首次系统地研究铜和铁硫化物矿物作为新型廉价的光催化材料来弥合这一知识差距。提出了一种新的分子共催化方法，以克服热力学和动力学的限制，CO2减少能源密集型燃料。其目的是确定在界面和散装电解质的分子助催化剂的反应依赖的机制，最终目标是开发更可持续和有效的光合系统。为了实现这一雄心勃勃的目标，来自哥伦比亚大学的一个团队将首次研究多尺度物理和化学驱动铁和铜硫化物对碳质燃料的人工光合作用，使用先进的操作FTIR和拉曼光谱电化学，（光）电化学和理论（例如，密度泛函理论）方法。在研究过程中开发的基于铜和铁硫化物的新的更有效的光合系统将是扩大可再生能源规模的实际步骤。这将导致新的可扩展的策略，合理设计的金属硫化物与水的界面。除了人工光合作用，这一成果可以在环境修复中固定放射性核素，以及在硫化物矿物的矿物加工（选择性分离）中，在绿色化学品的设计中找到应用。此外，这些知识将扩大我们对海洋地球化学过程的理解，包括酸性矿山排水过程，深海铁和铜的循环，以及最终生命的起源。研究的一般结果和新的方法将包括在PI的本科/研究生课程。