CAS: Achieving Long Lived Charge Separated States in Donor-Bridge-Acceptor Dyads Based on 3d Alkynyls – a Synthetic Approach

CAS:基于 3d 炔基在供体-桥-受体二元组中实现长寿命电荷分离态 — 一种合成方法

基本信息

  • 批准号:
    2102049
  • 负责人:
  • 金额:
    $ 53.8万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Standard Grant
  • 财政年份:
    2021
  • 资助国家:
    美国
  • 起止时间:
    2021-08-01 至 2024-07-31
  • 项目状态:
    已结题

项目摘要

With funding from the Chemical Synthesis program in the Division of Chemistry, Professor Tong Ren at Purdue University will prepare conjugated metal complexes of interesting photo-activity based on earth abundant metals. Chemists and material scientists have made great stride in molecular photovoltaics using so called dye-sensitized solar cells. The key molecules for the initial capture of solar energy are all based on rare precious metals such as Ru and Ir. Hence, it is highly desirable to develop molecules of similar capturing capability but based on earth abundant metals such as Cr, Fe and Co. However, most of compounds based on earth abundant metals lose the captured solar energy (so called excited state) before converting it into electricity. Professor Ren and his coworkers will extend the lifetime of excited states by using a new family of macrocycles to support Fe and Co containing molecules, and hence improve the conversion efficiency of solar energy to electricity. Professor Ren will work with a group of graduate and undergraduate students from diverse backgrounds. Through Purdue Science Express, he and his students will strive to improve the high school STEM education in the rural areas in Indiana through sharing laboratory equipment sets and designing new laboratory curriculum.The chemistry of metal alkynyls is a vibrant and evolving field, on which important technological advances including photovoltaics, photo-catalysis and molecular electronic devices have been achieved. This project will seek to develop unsymmetric bis-alkynyl complexes with long lived charge separated excited states based on the combination of earth abundant 3d metals and unsaturated [14]-tetraene-N4 macrocycles. The initial effort will be directed at the identification/preparation of suitable M([14]-tetraene-N4) starting materials, where M is Co(III) or Fe(III) and L is one of the three [14]-tetraene-N4 macrocycles, HMTI, TIM and TMTI. The ensuing effort will be focused on both the development of high yield preparation of the D-B-A dyads, and the understanding of donor/acceptor properties through voltammetry, steady state emission spectroscopy and ground state DFT calculations. The later phase of the project will be focused on the dynamics of the excited states. Through collaborations, significant aspects include the temporal and spatial evolution of the MLCT states in [M(II)( [14]-tetraene-N4)] complexes will be studied using fs M-edge XANES technique and companion high level CASSCF/CASPT2 analysis; and the dynamics of photo-induced electron transfer with the D-B-A dyad using both pump-probe and time-resolved IR techniques.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.
通过化学合成计划的资金,普渡大学的Tong Ren教授将根据地球丰富的金属制备有趣的光活性金属配合物。化学家和物质科学家使用所谓的染料敏化太阳能电池在分子光伏方面取得了长足的进步。最初捕获太阳能的关键分子都是基于RU和IR等稀有贵金属的。因此,高度希望开发具有相似捕获能力的分子,但基于CR,FE和Co等地球丰富的金属。但是,基于地球丰富金属的大多数化合物在将其转化为电力之前会失去捕获的太阳能(所谓的激发态)。 Ren教授和他的同事将通过使用新的大环基来支持FE和CO含有分子的寿命,从而提高太阳能对电力的转化效率。 Ren教授将与来自不同背景的一群研究生和本科生合作。通过Purdue Science Express,他和他的学生将努力通过共享实验室设备套装和设计新的实验室课程来改善印第安纳州农村地区的高中STEM教育。金属Alkynyls的化学是一个充满活力且不断发展的领域,在该领域上,重要的技术进步在其中,包括光伏,光电含量,光电含量,图形分析和分子电子设备在内的重要技术进步。该项目将寻求基于地球丰富的3D金属和不饱和的[14] - tetraene-N4宏环的组合,开发具有长期电荷的激发状态的不对称的双卵巢复合物。最初的努力将针对合适的M([14] -Tetraene-n4)起始材料的鉴定/制备,其中M是CO(III)或Fe(III),L是三个[14] -Tetraene-N4宏观环,HMTI,HMTI,TIM和TMTI之一。随后的努力将集中在D-B-A二元组的高产量制备以及通过伏安法,稳态发射光谱和基态DFT计算的理解。该项目的后期将集中在激发态的动态上。通过合作,将使用FS M-EDGE XANES技术和高级CASSCF/CASPT2分析进行协作,包括[M(ii)([14] -Tetraene-n4)中MLCT状态的时间和空间演变];以及使用Pump-probe和时间分辨的IR技术,通过D-B-A DYAD进行光诱导的电子传输的动力学。该奖项反映了NSF的法定任务,并被认为是通过基金会的智力优点和更广泛影响的审查标准通过评估来通过评估来获得支持的。

项目成果

期刊论文数量(11)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Phenylene as an efficient mediator for intermetallic electronic coupling
亚苯基作为金属间电子耦合的有效介体
  • DOI:
    10.1039/d2cc00949h
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    4.9
  • 作者:
    Miller-Clark, Lyndsy A.;Raghavan, Adharsh;Clendening, Reese A.;Ren, Tong
  • 通讯作者:
    Ren, Tong
Further Studies of Co III (TIM) Mono‐Alkynyl and Bis‐Alkynyl Complexes
Co III (TIM) 单炔基和双炔基配合物的进一步研究
  • DOI:
    10.1002/ejic.202200641
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    2.3
  • 作者:
    Rodriguez Segura, Leobardo;Cox, Kenneth E.;Samayoa‐Oviedo, Hugo Y.;Ren, Tong
  • 通讯作者:
    Ren, Tong
A Series of Mono- and Bis-Alkynyl Co(III) Complexes Supported by a Tetra-imine Macrocyclic Ligand (TIM)
  • DOI:
    10.1021/acs.organomet.1c00423
  • 发表时间:
    2021-09
  • 期刊:
  • 影响因子:
    2.8
  • 作者:
    Leobardo Rodriguez Segura;Seul Ah Lee;Brandon L Mash;Ashley J. Schuman;T. Ren
  • 通讯作者:
    Leobardo Rodriguez Segura;Seul Ah Lee;Brandon L Mash;Ashley J. Schuman;T. Ren
Mono‐ and Bis‐Alkynyl Iron Complexes Supported by a “Softened” Tetraaza Macrocycle
“软化”四氮杂大环支持的单炔基铁配合物和双炔基铁配合物
Nanosecond Metal-to-Ligand Charge-Transfer State in an Fe(II) Chromophore: Lifetime Enhancement via Nested Potentials
Fe(II) 发色团中的纳秒金属到配体的电荷转移状态:通过嵌套电势延长寿命
  • DOI:
    10.1021/jacs.2c13532
  • 发表时间:
    2023
  • 期刊:
  • 影响因子:
    15
  • 作者:
    Malme, Justin T.;Clendening, Reese A.;Ash, Ryan;Curry, Taylor;Ren, Tong;Vura-Weis, Josh
  • 通讯作者:
    Vura-Weis, Josh
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Tong Ren其他文献

An Analysis of First-Party Cookie Exfiltration due to CNAME Redirections
CNAME重定向导致的第一方Cookie泄露分析
Impact of Malnutrition on Length of Stay for Hospitalized CAR T Therapy Patients in the United States (2020)
  • DOI:
    10.1182/blood-2024-193980
  • 发表时间:
    2024-11-05
  • 期刊:
  • 影响因子:
  • 作者:
    Tong Ren;Daniel Kerr;Oyesanmi Olu;Salman Muddassir
  • 通讯作者:
    Salman Muddassir
The developments and applications of brain-like computing chips
类脑计算芯片的发展与应用
  • DOI:
    10.1117/12.2636417
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Yuzhou Nie;Tong Ren;Zhe Shi
  • 通讯作者:
    Zhe Shi
Anomalous peak effect in (Ba,A)Fe2As2 (A: Rb, K) single crystals with splayed columnar defects
具有张开柱状缺陷的 (Ba,A)Fe2As2 (A: Rb, K) 单晶的反常峰效应
  • DOI:
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Yuhang Zu;Tong Ren;Sunseng Pyon;Satoru Okayasu;and Tsuyoshi Tamegai
  • 通讯作者:
    and Tsuyoshi Tamegai
Nanopore detection of guanine derivatives based on vacancy G-quadruplex DNA
  • DOI:
    10.1016/j.microc.2024.112366
  • 发表时间:
    2025-01-01
  • 期刊:
  • 影响因子:
  • 作者:
    Tong Ren;Zhen Feng;Fang Jiang;Xingtong Liu;Tingting Chen;Yanli Guo;Lei Tian;Xiao-Feng Kang;Fujun Yao
  • 通讯作者:
    Fujun Yao

Tong Ren的其他文献

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{{ truncateString('Tong Ren', 18)}}的其他基金

Developing A Sustainable Metal Alkynyl Chemistry
开发可持续的金属炔基化学
  • 批准号:
    1764347
  • 财政年份:
    2018
  • 资助金额:
    $ 53.8万
  • 项目类别:
    Standard Grant
SusChEM: New Ni Macrocyclic Catalysts for Solar Driven Carbon Dioxide Reduction
SusChEM:用于太阳能驱动二氧化碳减排的新型镍大环催化剂
  • 批准号:
    1609151
  • 财政年份:
    2016
  • 资助金额:
    $ 53.8万
  • 项目类别:
    Standard Grant
MRI: Acquisition of an X-ray Diffractometer at Purdue University
MRI:在普渡大学购买 X 射线衍射仪
  • 批准号:
    1625543
  • 财政年份:
    2016
  • 资助金额:
    $ 53.8万
  • 项目类别:
    Standard Grant
Cross-conjugated 3d and 4d Metal-alkynyl Frameworks: Synthesis and Properties
交叉共轭 3d 和 4d 金属-炔基框架:合成和性能
  • 批准号:
    1362214
  • 财政年份:
    2014
  • 资助金额:
    $ 53.8万
  • 项目类别:
    Standard Grant
Novel Carbon Rich Organometallics based on iso-Triacetylene: Effects of Cross Conjugation
基于异三乙炔的新型富碳有机金属化合物:交叉共轭的影响
  • 批准号:
    1057621
  • 财政年份:
    2011
  • 资助金额:
    $ 53.8万
  • 项目类别:
    Continuing Grant
Conjugated Diruthenium Metallaynes: Monomers, Dimers and Oligomers
共轭二钌金属系化合物:单体、二聚体和低聚物
  • 批准号:
    0553564
  • 财政年份:
    2005
  • 资助金额:
    $ 53.8万
  • 项目类别:
    Continuing Grant
Conjugated Diruthenium Metallaynes: Monomers, Dimers and Oligomers
共轭二钌金属系化合物:单体、二聚体和低聚物
  • 批准号:
    0242623
  • 财政年份:
    2003
  • 资助金额:
    $ 53.8万
  • 项目类别:
    Continuing Grant

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在阿片类药物治疗患者中实现戒烟里程碑:直接观察和长期伐尼克兰的随机 2 x 2 析因试验
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