SusChEM: Spectro-electrochemical and theoretical study of carbon dioxide up-conversion mechanisms using clathrate hydrates

SusChEM:利用笼形水合物进行二氧化碳上转换机制的光谱电化学和理论研究

基本信息

  • 批准号:
    1665372
  • 负责人:
  • 金额:
    $ 48.5万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Standard Grant
  • 财政年份:
    2017
  • 资助国家:
    美国
  • 起止时间:
    2017-08-15 至 2020-12-31
  • 项目状态:
    已结题

项目摘要

The Chemical Structure, Dynamics, and Mechanism B Program (CSDMB) of the Chemistry Division supports the project by Professor Christoph Rose-Petruck (PI) and Professor Hannes Jónsson (co-PI). Professors Rose-Petruck and Jónsson are faculty members in the Department of Chemistry at Brown University. The research project focuses on the electrochemical conversion of carbon dioxide (CO2) into useful chemicals. Interest in CO2 conversion has increased significantly in recent years, in response to the increasing demand for sustainable products that are not generated from fossil fuels. While much work is being done to advance these efforts, there are still major hurdles to overcome. One of these is the electro-chemical generation of hydrogen gas that constantly competes with the desired CO2 conversion processes. This competing reaction steals the current (flow of electrons) needed for the CO2 conversion and, in so doing, makes the processes inefficient and costly. To solve this problem, the investigator are conducting the electrochemical conversion of CO2 in snow-like water crystals called clathrate hydrates that can store large amounts of CO2. This "snow" is mixed with salts and water to form an electrically conducting "snow-slush". The use of this mixture for the electro-chemical conversion of CO2 dramatically reduces the competing generation of hydrogen gas, leading to greatly improved yields and reaction efficiency. This discovery has the potential to be transformative in terms of how the conversion of CO2 into value added products is conducted. The use of clathrate hydrates in this fashion is very new, and the reaction mechanisms that enable the success of the approach are unknown. Hence, the researchers are seeking a better understanding of how these reactions work and how they can be manipulated to optimize the yield of a particular desired product. The research activities include a collaborative partnership with the Research Instruments Corporation, a Rhode Island based company. This company is a partner for technology transfer from Brown University into the market place. Recruitment and mentoring of historically underrepresented groups is enhanced through the partnership with the Leadership Alliance.The electrochemical reduction of CO2 into carbonaceous products is carried out in clathrate hydrate-loaded electrolytes. These reaction conditions strongly reduce the needed overpotential and change the product spectrum compared to that obtained with non-clathrate electrolytes. A spectrum of products is produced with low reduction potentials. The researchers hypothesize that reactions inside the clathrate hydrate structures are initiated by hydrogen-radical formation from clathrate water molecules as the clathrate crystals contact the working electrode. The experiments are combined with calculations of the reaction mechanisms and rates. These calculations are based on density functional theory of the electronic structure and minimum energy path calculations to estimate energy barriers for the various reaction steps and rate estimates based on harmonic transition state theory. The research investigates CO2 reduction mechanisms in electrolytes that include clathrate hydrates. The study provides a detailed insight into a new class of reaction mechanisms that use clathrates as water-based frameworks for high energy-efficient up-conversion of CO2 and other molecules. The activities include collaborative partners. The Research Instruments Corporation contributes strength in entrepreneurship and a partner for technology transfer from Brown University into the market place. Recruitment and mentoring of historically underrepresented groups is enhanced through the partnership with the Leadership Alliance.
化学系的化学结构,动力学和机制B计划(CSDMB)支持Christoph Rose-Petruck教授(PI)和Hannes Jónsson教授(co-PI)的项目。Rose-Petruck教授和Jónsson教授是布朗大学化学系的教员。该研究项目的重点是将二氧化碳(CO2)电化学转化为有用的化学品。近年来,对二氧化碳转化的兴趣显著增加,以应对对非化石燃料产生的可持续产品的需求日益增加。虽然正在为推动这些努力做大量工作,但仍有重大障碍需要克服。其中之一是电化学产生氢气,它不断与所需的CO2转化过程竞争。这种竞争反应窃取了二氧化碳转化所需的电流(电子流),从而使过程效率低下且成本高昂。为了解决这个问题,研究人员正在进行二氧化碳在雪状水晶体中的电化学转化,这种水晶体称为笼形水合物,可以储存大量的二氧化碳。这种“雪”与盐和水混合,形成导电的“雪泥”。使用这种混合物进行CO2的电化学转化显著减少了氢气的竞争产生,从而大大提高了产率和反应效率。这一发现在如何将二氧化碳转化为增值产品方面具有变革性的潜力。以这种方式使用笼形水合物是非常新的,并且使该方法成功的反应机理是未知的。因此,研究人员正在寻求更好地了解这些反应如何工作,以及如何操纵它们以优化特定所需产物的产率。研究活动包括与罗得岛公司研究仪器公司的合作伙伴关系。这家公司是布朗大学向市场转让技术的合作伙伴。通过与Leadership Alliance的伙伴关系,加强了对历史上代表性不足的群体的招募和指导。二氧化碳电化学还原为碳质产品是在负载包合物水合物的电解质中进行的。与非笼形电解质相比,这些反应条件大大降低了所需的过电位,并改变了产物光谱。生产的一系列产品具有低还原电位。研究人员假设,笼形水合物结构内部的反应是由笼形晶体接触工作电极时笼形水分子形成的氢自由基引发的。实验结果与反应机理和速率的计算相结合。这些计算是基于电子结构的密度泛函理论和最小能量路径计算,以估计各种反应步骤的能量势垒和基于谐波过渡态理论的速率估计。该研究调查了包括笼形水合物在内的电解质中的CO2还原机制。这项研究提供了一个详细的洞察一类新的反应机制,使用包合物作为水基框架的高能效上转换二氧化碳和其他分子。这些活动包括合作伙伴。 研究仪器公司为企业家精神和布朗大学向市场转移技术的合作伙伴做出了贡献。通过与领导力联盟的伙伴关系,加强了对历来代表性不足群体的征聘和辅导。

项目成果

期刊论文数量(2)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Addition to “Assessment of Constant-Potential Implicit Solvation Calculations of Electrochemical Energy Barriers for H 2 Evolution on Pt”
添加到“Pt 上 H 2 演化电化学能垒的恒电位隐式溶剂化计算评估”
  • DOI:
    10.1021/acs.jpcc.9b05026
  • 发表时间:
    2019
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Van den Bossche, Maxime;Skúlason, Egill;Rose-Petruck, Christoph;Jónsson, Hannes
  • 通讯作者:
    Jónsson, Hannes
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Christoph Rose-Petruck其他文献

Christoph Rose-Petruck的其他文献

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{{ truncateString('Christoph Rose-Petruck', 18)}}的其他基金

Ligand substitution dynamics of solvated iron pentacarbonyl measured by ultrafast x-ray absorption spectroscopy
超快 X 射线吸收光谱测量溶剂化五羰基铁的配体取代动力学
  • 批准号:
    0405599
  • 财政年份:
    2004
  • 资助金额:
    $ 48.5万
  • 项目类别:
    Continuing Grant
CAREER: Ultrafast x-ray imaging of molecular dynamics in solution: a research program that enhances students' learning
职业:溶液中分子动力学的超快 X 射线成像:增强学生学习的研究项目
  • 批准号:
    9984890
  • 财政年份:
    2000
  • 资助金额:
    $ 48.5万
  • 项目类别:
    Continuing Grant

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