Carbon Dioxide and Alkanes as Electron-sink and Source in a Solar Nanocell: towards Tandem Photosynthesis of Carbon Monoxide and Methanol

二氧化碳和烷烃作为太阳能纳米电池中的电子沉和源：一氧化碳和甲醇的串联光合作用

• 批准号: EP/F047878/1
• 负责人: Christopher Pickett
• 金额: $ 85.29万
• 依托单位: University of East Anglia
• 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%2FF047878%2F1
• 关键词: Carbon; Dioxide; Alkanes; Electron; sink

A major solar energy challenge is the goal of artificial synthesis in which sunlight is used to generate fuels or high energy chemicals. Natural photosynthesis uses solar energy to generate dioxygen and carbohydrates from carbon dioxide and water, but the targets of artificial photosynthesis can be more diverse. Our vision is to create a solar nano-device which will drive the coupled photo-conversion of methane and carbon dioxide into methanol and carbon monoxide respectively. This challenging target differs fundamentally from the familiar one of splitting water into hydrogen and oxygen. Our target offers products both on the oxidation and the reduction sides that are significant fuels or feedstocks. The photocatalytic reduction of CO2 and oxidation of alkanes represent long-standing goals of great complexity, but we base our concepts on well-established principles. We break down the goals into individual components, each of which is highly challenging within its own right and delivery of each would constitute a major breakthrough. The challenges will be met by a team of scientists, integrated across the four centres of Manchester, Nottingham, York and Norwich, who lead teams with expertise in photophysics, nanoscience, photochemistry, electrochemistry and synthesis. Thus these researchers will seek to establish the science required to underpin technologies that will allow the conversion of abundant and environmentally damaging feedstocks into products of high economic value by constructing a new class of solar device capable of driving green chemical reactions.

太阳能的一个主要挑战是人工合成的目标，即利用阳光来产生燃料或高能化学品。自然光合作用利用太阳能从二氧化碳和水中产生氧气和碳水化合物，但人工光合作用的目标可以更加多样化。我们的愿景是创造一种太阳能纳米设备，能够驱动甲烷和二氧化碳分别转化为甲醇和一氧化碳的耦合光转化。这个具有挑战性的目标与人们熟悉的将水分解为氢和氧的目标有根本的不同。我们的目标是提供氧化和还原方面的产品，这些产品是重要的燃料或原料。二氧化碳的光催化还原和烷烃的氧化代表着非常复杂的长期目标，但我们的概念建立在既定的原则上。我们将目标分解为单独的组成部分，每个组成部分本身都具有极大的挑战性，实现每个组成部分都将构成一个重大突破。这些挑战将由一个科学家团队应对，该团队整合在曼彻斯特、诺丁汉、约克和诺维奇四个中心，领导着拥有光物理、纳米科学、光化学、电化学和合成专业知识的团队。因此，这些研究人员将寻求建立所需的科学，以支持能够通过构建能够驱动绿色化学反应的新型太阳能设备，将丰富的、对环境有害的原料转化为具有高经济价值的产品的技术。

项目成果

Solar fuels: photoelectrosynthesis of CO from CO2 at p-type Si using Fe porphyrin electrocatalysts.

• DOI: 10.1002/chem.201300764
• 发表时间: 2013-09
• 期刊: Chemistry
• 作者: Khalaf M. Alenezi;S. Ibrahim;Peiyi Li;C. Pickett

Anode modification to improve the performance of a microbial fuel cell volatile fatty acid biosensor

• DOI: 10.1016/j.snb.2014.04.062
• 发表时间: 2014-10-01
• 期刊: SENSORS AND ACTUATORS B-CHEMICAL
• 影响因子: 8.4
• 作者: Kaur, Amandeep;Ibrahim, Saad;Premier, Giuliano C.
• 通讯作者: Premier, Giuliano C.

Electronic Control of the Protonation Rates of Fe-Fe Bonds

• DOI: 10.1021/ja506693m
• 发表时间: 2014-09-17
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Jablonskyte, Ausra;Webster, Lee R.;Pickett, Christopher J.
• 通讯作者: Pickett, Christopher J.

[FeFe] hydrogenase: protonation of {2Fe3S} systems and formation of super-reduced hydride states.

• DOI: 10.1002/anie.201406210
• 发表时间: 2014-09-15
• 期刊: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
• 影响因子: 16.6
• 作者: Jablonskyte, Ausra;Wright, Joseph A.;Fairhurst, Shirley A.;Webster, Lee R.;Pickett, Christopher J.
• 通讯作者: Pickett, Christopher J.

Towards alternatives to anodic water oxidation: basket-handle thiolate Fe(III) porphyrins for electrocatalytic hydrocarbon oxidation.

寻找阳极水氧化的替代品：用于电催化碳氢化合物氧化的篮柄硫醇铁（III）卟啉。

• DOI: 10.1002/cssc.201200572
• 发表时间: 2012
• 期刊: ChemSusChem
• 影响因子: 8.4
• 作者: Li P