SusChEM: Understanding and controlling photoinduced self-exchange reactions across sensitized mesoporous thin films to drive multiple-electron-transfer catalysis
SusChEM:理解和控制敏化介孔薄膜上的光诱导自交换反应以驱动多电子转移催化
基本信息
- 批准号:1566160
- 负责人:
- 金额:$ 38.5万
- 依托单位:
- 依托单位国家:美国
- 项目类别:Continuing Grant
- 财政年份:2016
- 资助国家:美国
- 起止时间:2016-08-15 至 2020-07-31
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
Professor Shane Ardo of the University of California-Irvine is supported by the Chemical Catalysis program in the Division of Chemistry to investigate dye-sensitized solar cells (DSSCs). DSSCs are an inexpensive alternative to commercial solar cells but have exhibited low solar-energy-conversion efficiencies that hamper their commercialization. This project is investigating an alternative reaction to dramatically increase the efficiency of iodide-containing DSSCs, from their current world-record efficiency of ~12% to over 20%. The project promotes the progress of science and facilitates environmental stewardship. Outreach workshops accompany this research program with the aim of increasing the participation and interest of female middle-school students in research related to solar energy conversion.The research is motivated by a new mechanism of operation for DSSCs and dye-sensitized functional assemblies for solar fuels where multiple-electron-transfer redox-shuttle chemistry is driven at molecular electrocatalysts co-anchored to dye-sensitized nanocrystalline TiO2. Fundamental studies include (i) surface-confined electrocatalysis of multiple-electron-transfer redox-shuttle oxidation, (ii) self-exchange electron transfer between molecules anchored to the TiO2 surface, and (iii) (slow) recombination of electrons in TiO2 with oxidized surface-anchored molecules. Several series of polymeric materials and Pt and Pd organometallic coordination compounds are synthesized and investigated for their ability to facilitate inner-sphere iodide oxidation electrocatalysis. The molecular structure of dyes is varied to identify those with the most rapid self-exchange electron transfer and slowest recombination. TiO2-bound electrocatalysts and dyes are studied simultaneously in order to interrogate the effects of several interacting functions and with the aim of realizing efficient light-driven iodide electrocatalysis. The electrocatalysis work is performed using a rotating ring-disk electrode setup and/or cyclic voltammetry to assess the catalytic competency of the molecules. Dye phenomena are interrogated using spectroelectrochemistry and nanosecond pump-probe transient-absorption and time-resolved photoluminescence (polarization) spectroscopies. In addition to spectrally modeling transient spectra and polarization kinetics, numerical models and Monte Carlo simulations helps clarify what controls the rate of (desired) self-exchange electron transfer and (undesired) recombination.
加州大学欧文分校的 Shane Ardo 教授在化学系化学催化项目的支持下研究染料敏化太阳能电池 (DSSC)。 DSSC 是商业太阳能电池的廉价替代品,但太阳能转换效率较低,阻碍了其商业化。该项目正在研究一种替代反应,以显着提高含碘化物 DSSC 的效率,从目前约 12% 的世界纪录效率提高到 20% 以上。 该项目促进科学进步并促进环境管理。 该研究项目还举办了外展研讨会,旨在提高女中学生对太阳能转换相关研究的参与度和兴趣。该研究的动机是 DSSC 和太阳能燃料染料敏化功能组件的新操作机制其中多电子转移氧化还原穿梭化学是由与染料敏化纳米晶 TiO2 共同锚定的分子电催化剂驱动的。基础研究包括 (i) 多电子转移氧化还原-穿梭氧化的表面限制电催化,(ii) 固定在 TiO2 表面的分子之间的自交换电子转移,以及 (iii) TiO2 中的电子与氧化的表面锚定分子。合成了几个系列的聚合物材料以及 Pt 和 Pd 有机金属配位化合物,并研究了它们促进内球碘化物氧化电催化的能力。染料的分子结构各不相同,以识别那些具有最快自交换电子转移和最慢重组的染料。同时研究 TiO2 结合电催化剂和染料,以探讨几种相互作用功能的影响,并实现高效的光驱动碘化物电催化。使用旋转环盘电极装置和/或循环伏安法进行电催化工作,以评估分子的催化能力。使用光谱电化学、纳秒泵浦探针瞬态吸收和时间分辨光致发光(偏振)光谱来研究染料现象。除了对瞬态光谱和极化动力学进行光谱建模之外,数值模型和蒙特卡罗模拟还有助于阐明控制(所需的)自交换电子转移和(不需要的)复合速率的因素。
项目成果
期刊论文数量(0)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
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Shane Ardo其他文献
Probing the active sites of oxide encapsulated electrocatalysts with controllable oxygen evolution selectivity
- DOI:
10.1039/d4ey00074a - 发表时间:
2024-04 - 期刊:
- 影响因子:0
- 作者:
William D. H. Stinson;Robert S. Stinson;Jingjing Jin;Zejie Chen;Mingjie Xu;Fikret Aydin;Yinxian Wang;Marcos F. Calegari Andrade;Xiaoqing Pan;Tuan Anh Pham;Katherine E. Hurst;Tadashi Ogitsu;Shane Ardo;Daniel V. Esposito - 通讯作者:
Daniel V. Esposito
BOWLING GREEN STATE 1
保龄球馆 州 1
- DOI:
- 发表时间:
2008 - 期刊:
- 影响因子:0
- 作者:
N. Ruiz Castellano;A. Seymour;F. Guo;K. Ogawa;Young‐gi kim;F. Castellano;J. Reynolds;E. Suchocki;A. Brecher;A. Rachford;F. Castella;Michael Y. Ogawa;R. Ziessel;Martin H Coggin;R. M. Srapionian;Elena A. Glik;L. Kate;I. Sazanovich;J. Weinstein;S. Murrey;K. Gray;Aaron J. Staniszewski;Shane Ardo;Yali Sun;Felix N. Cas;Tanya N. Singh;Alexandre Haefelé;Manuel A. Palacios;Zhuo Wang;Victor A. Montes;V. Zyryanov;Bethany J Hausch;K. Jursíková;S. Goeb;J. Richard - 通讯作者:
J. Richard
Modellierung, Simulation und Implementierung von Zellen für die solargetriebene Wasserspaltung
Zellen 的太阳能热水器建模、模拟和实施
- DOI:
10.1002/ange.201510463 - 发表时间:
2016-10-10 - 期刊:
- 影响因子:0
- 作者:
Chen Xiang;Adam Weber;Shane Ardo;A. Berger;Yikai Chen;Robert H. Coridan;Katherine T. Fountaine;Sophia Haussener;Shuyun Hu;Ruoyang Liu;Nathan S. Lewis;Miguel A. Modestino;Matthew Shaner;Meenesh R. Singh;John C. Stevens;K. Sun;Karl Walczak - 通讯作者:
Karl Walczak
Direct observation of the local microenvironment in inhomogeneous CO2reduction gas diffusion electrodesviaversatile pOH imaging
- DOI:
10.1039/d2ee02607d - 发表时间:
2023-02 - 期刊:
- 影响因子:32.5
- 作者:
Annette Böhme;Justin C. Bui;Aidan Q. Fenwick;Rohit Bhide;Cassidy N. Feltenberger;Alexandra J. Welch;Alex J. King;Alexis T. Bell;Adam Z. Weber;Shane Ardo;Harry A. Atwater - 通讯作者:
Harry A. Atwater
Particle suspension reactors and materials for solar-driven water splitting
- DOI:
10.1039/c5ee01434d - 发表时间:
2015-07 - 期刊:
- 影响因子:32.5
- 作者:
David M. Fabian;Shu Hu;Nirala Singh;Frances A. Houle;Takashi Hisatomi;Kazunari Domen;Frank E. Osterloh;Shane Ardo - 通讯作者:
Shane Ardo
Shane Ardo的其他文献
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{{ truncateString('Shane Ardo', 18)}}的其他基金
CAS: Assessing the Applicability of Marcus Theory to Excited-state Proton Transfer and Protonic Photochemical Energy Conversion
CAS:评估马库斯理论在激发态质子转移和质子光化学能量转换中的适用性
- 批准号:
2102665 - 财政年份:2021
- 资助金额:
$ 38.5万 - 项目类别:
Standard Grant
CAS: Assessing the Applicability of Marcus Theory to Excited-state Proton Transfer and Protonic Photochemical Energy Conversion
CAS:评估马库斯理论在激发态质子转移和质子光化学能量转换中的适用性
- 批准号:
2102665 - 财政年份:2021
- 资助金额:
$ 38.5万 - 项目类别:
Standard Grant
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