Microphase Photo-Electrochemistry: Light Driven Liquid-Liquid Ion Transfer Processes and Two-Phase Micro-Photovoltaic Systems

微相光电化学：光驱动液-液离子转移过程和两相微光伏系统

• 批准号: EP/G002614/1
• 负责人: Frank Marken
• 金额: $ 11.95万
• 依托单位: University of Bath
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2008
• 资助国家: 英国
• 起止时间: 2008 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FG002614%2F1
• 关键词: Microphase; Photo; Electrochemistry; Light; Driven

Photoelectrochemical processes are ubiquitous in nature and are a fundamental component in light harvesting processes. These processes occur in biological membranes with complex liquid | liquid reaction zones that have evolved to maximise the benefit to the host organism. Recent work on microphase liquid | liquid interfaces has broadened the range of experiments available for the study of electrochemical ion transfer at similarly complex liquid | liquid interfaces. In this proposal we focus on the next step: studying photo-electrochemical processes and tools at microphase liquid | liquid interfaces and within triple phase boundary reaction zones. This reaction zone offers a unique environment where photo-excited intermediates are in close proximity to both the electrode surface and the liquid | liquid interface.The project is exploratory but ambitious in nature and divided into four main, interconnected parts: (A) the study of electrochemically or photo-electrochemically driven ion transfer processes using fluorescent probe anions, (B) the study and screening of simultaneous electron and ion transfer at microphase liquid | liquid interfaces with novel triple phase boundary-based photochemical and photo-electrochemical methods, (C) the investigation of two-phase processes involving electron and ion transfer on TiO2 substrates or within TiO2 hosts, and (D) characterizing the local environment at the liquid | liquid interfaces using fluorescent probe molecules, and understanding how the potential of the interface and flux of ions across the interface affect the local environment.The primary intellectual merit of this project can be identified in (i) the development of new quantitative mechanistic tools for the study of complex electron/ion transfer at liquid | liquid interfaces, (ii) the exploration of the triple phase boundary domain for photo-electrochemical reactivity (the study of microdroplet size effects and reaction zones within microphase systems), and (iii) gaining an understanding of how the molecular scale organization and dynamics of a liquid interface is influenced by electron and/or ion transport across that interface. All of these aspects of the proposal serve to provide a broad understanding of how photoelectrochemical processes operating within microscopic liquid systems can be used to advantage in applications ranging from energy conversion to chemical sensing.The broader impact of the project lies primarily in providing a multinational cohort of globally competitive scientists to the workforce of both the United States and the United Kingdom. This project will facilitate the creation of a bilateral think tank and will foster the free exchange of ideas in a field of research and development that has direct impact on science at the interface between biosystems and energy conversion. We anticipate that the ideas and experiments developed in this collaborative study will help screen and identify new light harvesting processes, possibly mimicking natural processes, and therefore contribute to new energy harvesting/storage/management systems. It is important to note that both PIs have unique and difficult to replicate capabilities. The success of this work hinges on the collaboration between the Marken and Blanchard groups. If either PI were to undertake the proposed work by themselves, the study would be ineffective because neither lab has either the resources or expertise to perform all of the work proposed here.

光电化学过程在自然界中普遍存在，并且是光捕获过程中的基本组成部分。这些过程发生在生物膜与复杂的液体|液体反应区已经发展到最大化对宿主生物体的益处。微相液体研究进展|液体界面拓宽了研究类似复杂液体中电化学离子转移的实验范围|液体界面在本论文中，我们重点研究了微相液体中的光电化学过程和工具|液体界面和三相边界反应区内。该反应区提供了独特的环境，其中光激发的中间体非常接近电极表面和液体|该项目是探索性的，但雄心勃勃的性质，并分为四个主要的，相互关联的部分：（A）使用荧光探针阴离子的电化学或光电化学驱动的离子转移过程的研究，（B）微相液体中同时电子和离子转移的研究和筛选|液体界面与新的三相边界为基础的光化学和光电化学方法，（C）研究两相过程，涉及电子和离子转移的二氧化钛基板上或二氧化钛主机，和（D）表征局部环境的液体|利用荧光探针分子研究液体界面，并了解界面电位和离子穿过界面的通量如何影响局部环境。本项目的主要学术价值在于：（i）开发新的定量机制工具，用于研究液体中复杂的电子/离子转移|液体界面，（ii）光电化学反应性的三相边界域的探索（微滴尺寸效应和微相系统内的反应区的研究），以及（iii）获得对液体界面的分子尺度组织和动力学如何受到电子和/或离子跨该界面传输的影响的理解。所有这些方面的建议，以提供一个广泛的了解如何光电化学过程中运作的微观液体系统可以用来在应用中的优势，从能量转换到化学sensing.The更广泛的影响，该项目主要在于提供一个跨国队列的全球竞争力的科学家的劳动力的美国和英国。该项目将促进建立一个双边智囊团，并将促进在研究和开发领域自由交流想法，这对生物系统和能源转换之间的科学有直接影响。我们预计，在这项合作研究中开发的想法和实验将有助于筛选和识别新的光收集过程，可能模仿自然过程，因此有助于新的能量收集/存储/管理系统。重要的是要注意，这两个PI都具有独特且难以复制的功能。这项工作的成功取决于马尔肯和布兰查德集团之间的合作。如果任何一个PI自行承担拟定的工作，则研究将无效，因为两个实验室都没有资源或专业知识来执行此处拟定的所有工作。

项目成果

Liquid|liquid electrochemical bicarbonate and carbonate capture facilitated by boronic acids.

硼酸促进液体电化学碳酸氢盐和碳酸盐捕获。

• DOI: 10.1039/c1cc15211d
• 发表时间: 2011
• 期刊: Chemical communications (Cambridge, England)
• 作者: Collins AM

Triple phase boundary photovoltammetry: resolving rhodamine B reactivity in 4-(3-phenylpropyl)-pyridine microdroplets.

三相边界光电伏安法：解析 4-(3-苯基丙基)-吡啶微滴中罗丹明 B 的反应性。

• DOI: 10.1002/cphc.200000094
• 发表时间: 2010
• 期刊: a European journal of chemical physics and physical chemistry
• 作者: Collins AM

Spectroelectrochemical Investigation of TPPMn(III/II)-Driven Liquid | Liquid | Electrode Triple Phase Boundary Anion Transfer into 4-(3-Phenylpropyl)-Pyridine: ClO 4 - , CO 3 H - , Cl - , and F -

TPPMn(III/II)驱动液体的光谱电化学研究

• DOI: 10.1002/elan.201100623
• 发表时间: 2012
• 期刊: Electroanalysis
• 影响因子: 3
• 作者: Collins A