Interfacial Electrochemistry and Electrocatalysis: Understanding and Directing Electrochemical Phenomena at the Molecular Level

界面电化学和电催化：在分子水平上理解和指导电化学现象

• 批准号: RGPIN-2017-05610
• 负责人: Jerkiewicz, Gregory
• 金额: $ 4.37万
• 依托单位: Queen's University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2020
• 资助国家: 加拿大
• 起止时间: 2020-01-01 至 2021-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=711745
• 关键词: Interfacial; Electrochemistry; Electrocatalysis; Understanding; Directing

Our research in electrochemistry and electrocatalysis consists of three innovative thrusts that will be concurrently pursued to gain molecular-level understanding of electrochemical phenomena, discover new properties of materials, and develop new theories of electrochemical processes. We will synthesize Pd nanoparticles (Pd-NPs) of controlled shape and size, and characterize their structures and compositions using materials science methods (transmission electron microscopy, TEM, X-ray diffraction, XRD, electron tomography, ET). Their H absorbing capacity will be examined using electrochemical techniques (cyclic-voltammetry, CV, chrono-amperometry, CA, and chrono-coulometry, CC). The amount of absorbed H will be related to the size and shape of Pd-NPs to identify parameters that define their absorbing capacity. Absorption isotherms will be prepared to examine thermodynamics of the process and materials science techniques to analyze the structure of Pd-NPs upon H ingress. We will investigate composition-size-structure-reactivity phenomena in electrocatalysis by studying mechanisms and kinetics of the oxygen reduction and evolution reactions (ORR, OER). We will synthesize Pt, PtNi and PtCo nanoparticles and single crystals, and employ them as catalysts for ORR and OER. Their activity will be evaluated using electrochemical techniques (Tafel plots, polarization curves, CV, and CA). Electrochemical and analytical techniques (inductively coupled plasma mass spectrometry, ICPMS) will be used to examine degradation of these materials. Structure and composition of the electrode materials prior to and after electrochemical measurements will be analyzed using TEM, XRD, ET, scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDS). Comparison of results will shed light on composition-size-structure-reactivity phenomena and properties. Mass changes that accompany interfacial electrochemical processes are poorly understood and require examination over a broad temperature range. We will develop and apply variable-temperature electrochemical quartz crystal nanobalance (VT-EQCN) to examine interfacial electrochemical processes, such as catalyst oxidation and degradation. The technique will reveal T-dependent structure-forming and structure-breaking processes. The research program creates an opportunity for breakthroughs and discoveries. It is ambitious and challenging but my well-trained HQP are able to successfully undertake difficult projects. Though the research is fundamental in nature, it will benefit electrochemical technologies by creating new knowledge. Finally, HQP trained as part of this project will acquire knowledge in electrochemistry and electrocatalysis, and will develop a unique set of inter-disciplinary skills, which will enhance their future careers.

我们在电化学和电催化方面的研究包括三个创新主旨，将同时追求获得对电化学现象的分子水平理解、发现材料的新特性以及开发电化学过程的新理论。 我们将合成形状和尺寸受控的钯纳米颗粒（Pd-NP），并使用材料科学方法（透射电子显微镜、TEM、X射线衍射、XRD、电子断层扫描、ET）表征其结构和成分。 将使用电化学技术（循环伏安法，CV，计时电流法，CA 和计时库仑法，CC）检查它们的 H 吸收能力。 吸收的 H 量将与 Pd-NP 的尺寸和形状相关，以确定定义其吸收能力的参数。 将准备吸收等温线来检查过程的热力学和材料科学技术，以分析 H 进入后 Pd-NP 的结构。 我们将通过研究氧还原和析出反应（ORR、OER）的机制和动力学来研究电催化中的组成-尺寸-结构-反应现象。 我们将合成Pt、PtNi和PtCo纳米粒子和单晶，并将它们用作ORR和OER的催化剂。 将使用电化学技术（塔菲尔图、极化曲线、CV 和 CA）评估它们的活性。 电化学和分析技术（电感耦合等离子体质谱法，ICPMS）将用于检查这些材料的降解情况。 将使用 TEM、XRD、ET、扫描电子显微镜 (SEM) 和能量色散 X 射线光谱 (EDS) 分析电化学测量前后电极材料的结构和成分。 结果比较将揭示成分-尺寸-结构-反应现象和性质。 人们对界面电化学过程伴随的质量变化知之甚少，需要在较宽的温度范围内进行检查。 我们将开发并应用变温电化学石英晶体纳米天平（VT-EQCN）来检查界面电化学过程，例如催化剂氧化和降解。 该技术将揭示依赖于 T 的结构形成和结构破坏过程。 该研究计划为突破和发现创造了机会。 这是雄心勃勃且具有挑战性的，但我训练有素的总部能够成功地承担困难的项目。 尽管这项研究本质上是基础性的，但它将通过创造新知识而使电化学技术受益。 最后，作为该项目的一部分接受培训的 HQP 将获得电化学和电催化方面的知识，并将培养一套独特的跨学科技能，这将增强他们未来的职业生涯。