SusChEM: Visible Light-Driven Reduction of Carbon Dioxide using Heavy Metal-Free Colloidal Quantum Dots as Sensitizers
SusChEM:使用不含重金属的胶体量子点作为敏化剂进行可见光驱动的二氧化碳还原
基本信息
- 批准号:1664184
- 负责人:
- 金额:$ 40.86万
- 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:2017-06-15 至 2020-05-31
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
The use of sunlight to convert carbon dioxide (CO2) to various small molecules that can be used as fuels is a sustainable way to exploit abundant solar energy for use both during day and night. The chemical reactions involved in this conversion are complicated and multi-step, and typically involve the transfer of electrons from one molecule to another. A "photocatalyst" is a species that lowers the energy barriers for, and thereby facilitates, such complex reactions by using light energy to drive chemical reactions. With funding from the Chemical Catalysis Program of the Chemistry Division, Dr. Emily Weiss of Northwestern University is conducting fundamental studies to identify and optimize photocatalyts for CO2 conversion in catalyst designs that comprise molecules adsorbed to the surfaces of semiconductor nanoparticles made of non-toxic, earth abundant materials. Her studies involve both chemical analysis of these hybrid inorganic-organic complexes and laser spectroscopy to monitor their behaviors on ultrafast timescales after excitation with light energy. Dr. Weiss is actively involved in the mentoring of undergraduate researchers on this project, in the development of a new curriculum for General Chemistry at Northwestern University to increase retention of women and minority students under-represented in STEM fields, and in programs like the Gateway Science Workshop, which offers structured study sessions for students in STEM courses, particularly those students with weaker high school preparation. With funding from the Chemical Catalysis Program of the Chemistry Division, Dr. Emily Weiss of Northwestern University is identifying and optimizing the most important thermodynamic and kinetic parameters in the performance of ternary heavy metal-free colloidal CuInX2 (X = S, Se) quantum dots (QDs) as soluble, multi-site, colloidal sensitizers for photocatalysis of the reduction of CO2 in solution. This work illuminates the mechanisms by which specific and unique properties of a colloidal QD sensitizer enhance the performance of a molecular catalyst with known specificity for CO2 reduction, by addressing several fundamental challenges associated with this task, namely: (i) synthesis and surface functionalization of a QD sensitizer with enough reducing power to donate multiple electrons to the co-catalyst; (ii) control of the local concentration of hydrogen ions; (iii) fast hole extraction from the sensitizer to inhibit recombination and photo-oxidative degradation; and (iv) maximal electronic coupling between the sensitizer and the co-catalyst to provide pathways for fast electron delivery. One and two dimensional nuclear magnetic resonance (NMR) spectroscopy, electron microscopy, electrochemical measurements and steady-state and time resolved optical measurements allow for quantitative characterization of the binding affinity for the QD-catalyst pair, the proton (H+) concentration on the QD surface, the degree of adsorption of the catalytic substrates and intermediates, the rate constants for elementary electron and hole transfer steps, and the efficacy of hole scavenging. These techniques complement the gas and liquid chromatography, NMR, and infrared spectroscopy characterization of product distributions and reaction rates. In addition to the societal impact of finding new pathways to produce carbon- and hydrogen-based fuels from sunlight and CO2 using a non-toxic, earth-abundant colloidal catalyst, this work has broad impact in that undergraduates will be involved both in the proposed research and in ongoing curriculum reform of General Chemistry by Dr. Weiss, in order to increase retention of women and under-represented minority students in STEM fields at Northwestern University.
利用阳光将二氧化碳(CO2)转化为可用作燃料的各种小分子,是一种可持续的方式,可以利用丰富的太阳能在白天和夜晚使用。这种转化所涉及的化学反应是复杂和多步骤的,并且通常涉及电子从一个分子转移到另一个分子。“光催化剂”是一种物质,其通过使用光能驱动化学反应来降低这种复杂反应的能量势垒,从而促进这种复杂反应。在化学部化学催化项目的资助下,西北大学的艾米丽韦斯博士正在进行基础研究,以确定和优化催化剂设计中用于CO2转化的光催化剂,该催化剂设计包括吸附到由无毒、地球丰富的材料制成的半导体纳米颗粒表面的分子。 她的研究涉及这些混合无机-有机复合物的化学分析和激光光谱学,以监测它们在光能激发后在超快时间尺度上的行为。韦斯博士积极参与指导本科研究人员在这个项目上,在西北大学普通化学的新课程的开发,以提高妇女和少数民族学生在STEM领域的代表性不足的保留,并在像网关科学研讨会,它提供了结构化的学习课程,为学生在STEM课程,特别是那些学生与较弱的高中准备方案。 在化学部化学催化项目的资助下,西北大学的艾米丽韦斯博士正在确定和优化三元重金属胶体CuInX 2(X = S,Se)量子点(QD)作为可溶性,多位点,胶体敏化剂的性能中最重要的热力学和动力学参数,用于减少溶液中的CO2。这项工作阐明了胶体QD敏化剂的特定和独特性质增强具有已知的CO2还原特异性的分子催化剂的性能的机制,通过解决与该任务相关的几个基本挑战,即:(i)具有足够还原能力以向助催化剂提供多个电子的QD敏化剂的合成和表面官能化;(ii)控制氢离子的局部浓度;(iii)从光敏剂中快速提取空穴,以抑制复合和光氧化降解;以及(iv)光敏剂和助催化剂之间的最大电子耦合,为快速电子传递提供途径。一维和二维核磁共振(NMR)光谱、电子显微镜、电化学测量以及稳态和时间分辨光学测量允许定量表征QD-催化剂对的结合亲和力、QD表面上的质子(H+)浓度、催化底物和中间体的吸附程度、基本电子和空穴转移步骤的速率常数、以及空穴清除的功效。这些技术补充了产物分布和反应速率的气相和液相色谱、核磁共振和红外光谱表征。除了寻找新的途径,以生产碳和氢为基础的燃料,从阳光和二氧化碳使用无毒,地球丰富的胶体催化剂的社会影响,这项工作具有广泛的影响,本科生将参与拟议的研究和正在进行的课程改革一般化学博士韦斯,以增加妇女和代表性不足的少数民族学生在西北大学STEM领域的保留。
项目成果
期刊论文数量(7)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
pH-Dependent structure of water-exposed surfaces of CdSe quantum dots.
CdSe 量子点暴露于水的表面的 pH 依赖性结构。
- DOI:10.1039/c9cc01339c
- 发表时间:2019
- 期刊:
- 影响因子:0
- 作者:Westmoreland,DanaE;Nap,RikkertJ;Arcudi,Francesca;Szleifer,Igal;Weiss,EmilyA
- 通讯作者:Weiss,EmilyA
Oxidation of a Molecule by the Biexcitonic State of a CdS Quantum Dot
- DOI:10.1021/acs.jpcc.9b00210
- 发表时间:2019-02
- 期刊:
- 影响因子:0
- 作者:Shichen Lian;Joseph A. Christensen;Mohamad S. Kodaimati;Cameron R. Rogers;M. Wasielewski;E. Weiss
- 通讯作者:Shichen Lian;Joseph A. Christensen;Mohamad S. Kodaimati;Cameron R. Rogers;M. Wasielewski;E. Weiss
Quantum Dot‐Catalyzed Photoreductive Removal of Sulfonyl‐Based Protecting Groups
量子点催化光还原去除磺酰基保护基团
- DOI:10.1002/ange.202005074
- 发表时间:2020
- 期刊:
- 影响因子:0
- 作者:Perez, Kaitlyn A.;Rogers, Cameron R.;Weiss, Emily A.
- 通讯作者:Weiss, Emily A.
Viewpoint: Challenges in Colloidal Photocatalysis and Some Strategies for Addressing Them
- DOI:10.1021/acs.inorgchem.7b03182
- 发表时间:2018-04-02
- 期刊:
- 影响因子:4.6
- 作者:Kodaimati, Mohamad S.;McClelland, Kevin P.;Weiss, Emily A.
- 通讯作者:Weiss, Emily A.
Systematic control of the rate of singlet fission within 6,13-diphenylpentacene aggregates with PbS quantum dot templates
使用 PbS 量子点模板系统控制 6,13-二苯基并五苯聚集体中的单线态裂变速率
- DOI:10.1039/c8fd00157j
- 发表时间:2019
- 期刊:
- 影响因子:3.4
- 作者:Wang, Chen;Kodaimati, Mohamad S.;Lian, Shichen;Weiss, Emily A.
- 通讯作者:Weiss, Emily A.
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Emily Weiss其他文献
Examination of the COVID-19 Pandemic’s Impact on Mental Health From Three Perspectives: Global, Social, and Individual
从全球、社会和个人三个角度审视 COVID-19 大流行对心理健康的影响
- DOI:
- 发表时间:
2022 - 期刊:
- 影响因子:12.6
- 作者:
Lauren E Thomas;Abigail Emich;Emily Weiss;Corina R Zisman;Katherine Foray;D. Roberts;Emily Page;M. Ernst - 通讯作者:
M. Ernst
Farming, Foreign Holidays, and Vitamin D in Orkney
奥克尼群岛的农业、国外假期和维生素 D
- DOI:
- 发表时间:
2016 - 期刊:
- 影响因子:3.7
- 作者:
Emily Weiss;L. Zgaga;S. Read;S. Wild;M. Dunlop;H. Campbell;R. McQuillan;James F. Wilson - 通讯作者:
James F. Wilson
Service dog selection tests: Effectiveness for dogs from animal shelters
服务犬选择测试:对动物收容所的狗的有效性
- DOI:
10.1016/s0168-1591(96)01176-8 - 发表时间:
1997 - 期刊:
- 影响因子:2.3
- 作者:
Emily Weiss;G. Greenberg - 通讯作者:
G. Greenberg
Health Management for Quality of Life of Multiple Sclerosis Patients
- DOI:
10.1093/cdn/nzaa040_086 - 发表时间:
2020-06-01 - 期刊:
- 影响因子:
- 作者:
Emily Weiss;Hyun Kim - 通讯作者:
Hyun Kim
406. Associations Between Kappa Opioid Receptor Availability and Hoarding Behaviors: Preliminary Evidence Using [11C]EKAP Positron Emission Tomography
406. κ阿片受体可利用性与囤积行为之间的关联:使用[11C]EKAP正电子发射断层扫描的初步证据
- DOI:
10.1016/j.biopsych.2025.02.644 - 发表时间:
2025-05-01 - 期刊:
- 影响因子:9.000
- 作者:
Emily Weiss;Victoria Hart-Derrick;Dayna Freeman;Christopher Pittenger;David Matuskey;Nabeel Nabulsi;Margaret Davis - 通讯作者:
Margaret Davis
Emily Weiss的其他文献
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{{ truncateString('Emily Weiss', 18)}}的其他基金
REU Site: Research Experience for Undergraduates in Nanoscale Science and Engineering
REU网站:纳米科学与工程本科生的研究经验
- 批准号:
1757618 - 财政年份:2019
- 资助金额:
$ 40.86万 - 项目类别:
Standard Grant
A Partnership to Adapt, Implement and Study a Professional Learning Model and Build District Capacity to Improve Science Instruction and Student Understanding
建立伙伴关系,以适应、实施和研究专业学习模式并建设学区能力,以改善科学教学和学生理解
- 批准号:
1720894 - 财政年份:2017
- 资助金额:
$ 40.86万 - 项目类别:
Continuing Grant
Transforming College Teaching: Statewide Implementation of the Faculty Learning Program to Improve STEM Undergraduate Teaching and Learning
转变大学教学:在全州范围内实施教师学习计划,以改善 STEM 本科教学
- 批准号:
1626624 - 财政年份:2016
- 资助金额:
$ 40.86万 - 项目类别:
Standard Grant
Charge Transfer as a Probe of the Permeability of Organic Adlayers on Colloidal Semiconductor Quantum Dots
电荷转移作为胶体半导体量子点上有机吸附层渗透性的探针
- 批准号:
1400596 - 财政年份:2014
- 资助金额:
$ 40.86万 - 项目类别:
Standard Grant
2014 Colloidal Semiconductor Nanocrystals Gordon Research Conference, July 20-25, 2014
2014胶体半导体纳米晶体戈登研究会议,2014年7月20-25日
- 批准号:
1401045 - 财政年份:2014
- 资助金额:
$ 40.86万 - 项目类别:
Standard Grant
REU Site: Research Experience for Undergraduates in Nanoscale Science & Engineering
REU 网站:纳米科学本科生的研究经验
- 批准号:
1359004 - 财政年份:2014
- 资助金额:
$ 40.86万 - 项目类别:
Standard Grant
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