CAREER: Electronic transport and interfacial effects on electrochemical hydrogen evolution reaction for transition metal dichalcogenides

职业：过渡金属二硫属化物电化学析氢反应的电子传输和界面效应

• 批准号: 1749742
• 负责人: Judy Cha
• 金额: $ 58万
• 依托单位: Yale University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-03-15 至 2022-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1749742&HistoricalAwards=false
• 关键词: CAREER; Electronic; transport; interfacial; effects

Electrochemical catalysis can be used to generate hydrogen from water, thereby offering a sustainable alternative to conventional processes that generate hydrogen from natural gas or petroleum. In recent years, a class of low-cost chemical materials, known as transition metal dichalcogenides (TMDCs), have been identified as promising materials for water-based hydrogen production to power fuel cells and as a raw material for the manufacture of chemicals. Despite their promise, additional scientific understanding and engineering design will be needed to maximize the performance of the dichalcogenide materials to levels rivaling more expensive state-of-the-art platinum-based catalysts. To that end, the project will explore fundamental aspects of the dichalcogenide materials and their effectiveness for hydrogen generation utilizing a unique reactor system. The research will help pave the path to a sustainable energy and chemicals future while also laying ground work for long-term competitiveness of the U.S. in the fuels and chemical manufacturing sectors. The research will be integrated with educational and outreach activities emphasizing participation by under-represented groups. The project seeks answers to the extent that electronic transport properties and interfacial effects (rather than the free energy of hydrogen adsorption) limit the overall rate of the hydrogen evolution reaction (HER) on TMDCs. A single-crystalline flake nanodevice will be employed as a HER micro-reactor, which allows precise control of the density and types of catalytic sites, and accurate measurements of charge transport within the catalyst, as well as the Schottky barrier at the catalyst/current collector interface. Three aims are proposed to study how the TMDC electrical properties, interfacial Schottky barrier, and the hydrogen adsorption free energy change as a function of 1) the phase transition from the semiconducting 2H to the semi-metallic 1T' phase of TMDCs, 2) strain engineering of TMDCs, and 3) different current collectors. The changes in the various properties will be correlated with the measured HER activities using a standard three-electrode cell coupled to the individual TMDC nanodevices in sulfuric acid electrolyte solution. Semiconducting MoS2 and WS2, and semi-metallic MoTe2 and WTe2 nanoflakes will be used for the proposed research, grown by chemical vapor deposition or exfoliated mechanically from bulk crystals grown by chemical vapor transport. Beyond optimization of TMDC materials for HER, the nanodevice platform can be applied to other electro- and photo-catalysts to correlate their catalytic properties to critical parameters such as energetics of catalytic sites, equilibrium electrical properties, interfacial effects, and excited states induced by photons. The project will link the research to education and outreach activities via three outreach programs targeting, respectively, the general public (a weekend Energy symposium at Yale West Campus), under-represented undergraduate students (a monthly seminar series given by minority faculty members), and local high school students (a demonstration HER kit and workbook based on TMDC thin films).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.

电化学催化可用于从水中产生氢，从而为传统工艺提供可持续的替代方法，该过程可从天然气或石油产生氢。近年来，一类低成本的化学材料（称为过渡金属二甲化物（TMDC））已被确定为有前途的水基氢生产材料，以供电燃料电池，也是制造化学物质的原材料。 尽管他们有希望，但仍需要额外的科学理解和工程设计，以最大程度地提高二分法材料的性能，从而使基于铂金的最昂贵的催化剂与更昂贵的最昂贵的催化剂媲美。为此，该项目将探索二甲基元化材料的基本方面及其利用独特的反应器系统的氢生成有效性。这项研究将帮助铺平通往可持续能源和化学物质未来的道路，同时还为美国在燃料和化学制造业的长期竞争力奠定了地面工作。 这项研究将与教育和外展活动集成，该活动强调代表性不足的群体的参与。 该项目寻求答案的程度，即电子传输特性和界面效应（而不是氢吸附的自由能）限制了TMDC上氢进化反应（HER）的总体速率。 单晶薄片纳米涂片将被用作她的微反应器，可以精确控制催化位点的密度和类型，并准确地测量催化剂内电荷传输以及催化剂/电流收集器界面的Schottky屏障。提出了三个目标来研究TMDC电气性能，界面肖特基屏障和氢吸附自由能的变化如何随着1）的函数的函数1）从半导体2H到半金属1T到TMDC的阶段的相变，2）TMDCS的过滤量，以及TMDC的过滤量。各种特性的变化将与硫酸电解质溶液中偶联的标准三电极细胞与单个TMDC纳米电视耦合的标准三电极细胞相关。半导体MOS2和WS2，以及半金属MOTE2和WTE2纳米片将用于拟议的研究，该研究是通过化学蒸气沉积而生长的，或者是通过化学蒸气运输生长的散装晶体而机械地剥落的。 除了对她的TMDC材料进行优化外，纳米式维斯平台还可以应用于其他电催化剂和光催化剂，以将其催化特性与关键参数相关联，例如催化位点的能量，平衡电特性，界面效应以及受光子刺激的态度的激发液。该项目将通过针对公众（Yale West Campus举行的周末能源研讨会），将研究与教育和外展活动联系起来，这是代表性不足的本科生（由少数派教职员工的每月研讨会系列）和当地的高中生（基于TMDC the tem and tem and seals and and the seals and and and the seals and and and the and and sefors and and the and the and and the sepors and and the and the sepors and and the and te e n esse ne sefors ers and the sepors and the seals。值得通过基金会的智力优点和更广泛的影响审查标准来通过评估来支持。

项目成果

Revisiting Intercalation‐Induced Phase Transitions in 2D Group VI Transition Metal Dichalcogenides

• DOI: 10.1002/aesr.202100027
• 发表时间: 2021-05
• 期刊: Advanced Energy and Sustainability Research
• 作者: Mengjing Wang;Shiyu Xu;J. Cha

A Highly Efficient All‐Solid‐State Lithium/Electrolyte Interface Induced by an Energetic Reaction

• DOI: 10.1002/anie.202004477
• 发表时间: 2020-06
• 期刊: Angewandte Chemie International Edition
• 作者: Y. Zhong;Yujun Xie;Sooyeon Hwang;Qian Wang;Judy J. Cha;Dong Su;Hailiang Wang

Recent progress on in situ characterizations of electrochemically intercalated transition metal dichalcogenides

• DOI: 10.1007/s12274-019-2408-6
• 发表时间: 2019-09
• 期刊: Nano Research
• 影响因子: 9.9
• 作者: Sajad Yazdani;Milad Yarali;J. Cha

The development of 2D materials for electrochemical energy applications: A mechanistic approach

• DOI: 10.1063/1.5085187
• 发表时间: 2019-03
• 期刊: APL Materials
• 影响因子: 6.1
• 作者: D. Hynek;Joshua V. Pondick;J. Cha

The Effect of Mechanical Strain on Lithium Staging in Graphene

• DOI: 10.1002/aelm.202000981
• 发表时间: 2020-08
• 期刊: Advanced Electronic Materials
• 影响因子: 6.2
• 作者: Joshua V. Pondick;Sajad Yazdani;Milad Yarali;Serrae N. Reed;D. Hynek;J. Cha