Collaborative Research: In Situ Surface Spectroscopy of 2D Material-based Electrocatalysis and Photoelectrocatalysis

合作研究：二维材料电催化和光电催化的原位表面光谱

• 批准号: 2012845
• 负责人: Stephen Cronin
• 金额: $ 30万
• 依托单位: University of Southern California
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-08-01 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2012845&HistoricalAwards=false
• 关键词: Collaborative; Research; Situ; Surface; Spectroscopy

Electrochemical and photoelectrochemical processes are important to a wide range of energy-related and environmental applications, including solar energy storage and carbon remediation. Photoelectrochemical hydrogen production is especially exciting for its potential to convert solar energy into carbon-free chemical fuels. The project will enable increased efficiency of photoelectrocatalytic reactions through study of the fundamental physical and chemical processes occurring in a class of ultrathin catalytic materials important for the sustainable production of fuels and chemicals.The study will investigate electrocatalysis (EC) and photoeletrocatalysis (PEC) in two-dimensional dichalcogenide materials using various forms of in situ linear, nonlinear, and ultrafast spectroscopy to characterize three critical factors in EC/PEC reactions: interfacial electrostatics (local (i.e., surface) electrostatic fields), interfacial dynamics and electrostatics (photoexcited charge carrier dynamics), and interfacial molecular structures (surface bound intermediate species) produced during the EC and PEC processes. Sum frequency generation (SFG), second harmonic generation (SHG), vibrational Stark Shift (VSS) spectroscopy, and transient absorption spectroscopy (TAS) will be employed to reveal key mechanistic information regarding the EC and PEC processes primarily for the reduction of CO2 to methanol and carbon monoxide. Spectroscopic data will be acquired in situ as a function of the electrochemical potential and electrolyte composition, and correlated with product yield and selectivity. The project includes educational and outreach activities that build upon the research to promote engagement of students in science, technology, engineering and mathematics (STEM) disciplines. These activities, which include workshop for high school science teachers, are directed at improving the education of promising high school students and encouraging their interest in STEM careers.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.

电化学和光电化学过程对于广泛的能源相关和环境应用非常重要，包括太阳能存储和碳修复。光电化学制氢因其将太阳能转化为无碳化学燃料的潜力而特别令人兴奋。该项目将通过研究一类对燃料和化学品可持续生产非常重要的超薄催化材料中发生的基本物理和化学过程来提高光电催化反应的效率。该研究将研究光电催化（EC）和光电催化（PEC）在二维二硫族化物材料使用各种形式的原位线性、非线性和超快光谱来表征 EC/PEC 反应中的三个关键因素：界面静电（局部（即，表面）静电场）、界面动力学和静电（光激发电荷载流子动力学）以及 EC 和 PEC 过程中产生的界面分子结构（表面结合中间物质）。将采用和频发生 (SFG)、二次谐波发生 (SHG)、振动斯塔克频移 (VSS) 光谱和瞬态吸收光谱 (TAS) 来揭示有关 EC 和 PEC 过程的关键机械信息，主要用于将 CO2 还原为甲醇和一氧化碳。 光谱数据将在原位获得，作为电化学势和电解质组成的函数，并与产物产率和选择性相关。 该项目包括以研究为基础的教育和外展活动，以促进学生对科学、技术、工程和数学 (STEM) 学科的参与。这些活动包括针对高中科学教师的研讨会，旨在改善有前途的高中生的教育并鼓励他们对 STEM 职业的兴趣。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力评估进行评估，认为值得支持。优点和更广泛的影响审查标准。

项目成果

Harvesting Planck radiation for free-space optical communications in the long-wave infrared band

收集长波红外波段自由空间光通信的普朗克辐射

• DOI: 10.1364/ol.476394
• 发表时间: 2022-11
• 期刊: Optics Letters
• 影响因子: 3.6
• 作者: Weinstein, Haley A.;Cai, Zhi;Cronin, Stephen B.;Habif, Jonathan L.
• 通讯作者: Habif, Jonathan L.

Gate-tunable modulation of the optical properties of multilayer graphene by the reversible intercalation of ionic liquid anions

通过离子液体阴离子的可逆嵌入对多层石墨烯的光学性质进行门可调调制

• DOI: 10.1063/5.0093651
• 发表时间: 2022-09-07
• 期刊: Journal of Applied Physics
• 影响因子: 3.2
• 作者: Zhi Cai;Indu Aravind;Haley Weinstein;Ruoxi Li;Jiangbin Wu;Han Wang;J. Habif;S. Cronin
• 通讯作者: S. Cronin

SERS Detection of Charge Transfer at Electrochemical Interfaces Using Surface-Bound Ferrocene

使用表面结合二茂铁检测电化学界面的电荷转移的 SERS

• DOI: 10.1021/acs.jpcc.3c01973
• 发表时间: 2023-07-13
• 期刊: The Journal of Physical Chemistry C
• 作者: Ruoxi Li;Imran Chaudhry;Cindy Tseng;Sizhe Weng;Y. Wang;Bofan Zhao;Indu Aravind;Zhi Cai;J. Dawlaty;L. Jensen;S. Cronin
• 通讯作者: S. Cronin

Field-Dependent Orientation and Free Energy of D 2 O at an Electrode Surface Observed via SFG Spectroscopy

通过 SFG 光谱观察电极表面 D 2 O 的场相关取向和自由能

• DOI: 10.1021/acs.jpcc.2c06063
• 发表时间: 2022-12
• 期刊: The Journal of Physical Chemistry C
• 作者: Montenegro, Angelo;Vaughn, Ariel E.;Mammetkuliyev, Muhammet;Zhao, Bofan;Zhang, Boxin;Shi, Haotian;Bhattacharyya, Dhritiman;Benderskii, Alexander V.;Cronin, Stephen B.
• 通讯作者: Cronin, Stephen B.

Monitoring Reaction Intermediates in Plasma-Driven SO 2 , NO, and NO 2 Remediation Chemistry Using In Situ SERS Spectroscopy

使用原位 SERS 光谱监测等离子体驱动的 SO 2 、NO 和 NO 2 修复化学中的反应中间体

• DOI: 10.1021/acs.analchem.0c05413
• 发表时间: 2021-04
• 期刊: Analytical Chemistry
• 影响因子: 7.4
• 作者: Li, Shujin;Zhao, Bofan;Aguirre, Alejo;Wang, Yu;Li, Ruoxi;Yang, Sisi;Aravind, Indu;Cai, Zhi;Chen, Ran;Jensen, Lasse;et al
• 通讯作者: et al