CAREER: Controlling two-dimensional heterointerface in layered oxides for electrodes with advanced electrochemical properties

职业：控制具有先进电化学性能的电极层状氧化物中的二维异质界面

• 批准号: 1752623
• 负责人: Ekaterina Pomerantseva
• 金额: $ 50万
• 依托单位: Drexel University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-07-01 至 2024-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1752623&HistoricalAwards=false
• 关键词: CAREER; Controlling; two; dimensional; heterointerface

NON-TECHNICAL DESCRIPTION: This CAREER project aims to create a completely new class of ceramic oxide materials with advanced charge storage capabilities, opening a door to next-generation batteries with higher energy density, faster charging and a much longer lifetime. These new materials are two-dimensional (2D) oxide-based structures that are built by alternating oxide layers and electronically conductive layers, such as graphene-based compounds or transition metal carbides (MXenes). The resulting structures exhibit characteristics important for battery electrodes: space that allows ion movement, and conductive layers that enable fast transport of electrons. Combining layered metal oxides and carbon-based compounds in high quality layer-by-layer architecture offers an opportunity to discover and investigate new phenomena occurring at interfaces. This fundamental understanding is important for the creation of batteries with improved energy and power capabilities. The materials and methods developed in this work are relevant to a wider range of applications, including energy storage, electrochromics (responsible for reversible changes of colour), sensing, actuation (or control of movement), and water treatment. The interdisciplinary nature of this project attracts diverse undergraduate and graduate students to research. The project integrates synthesis and properties of 2D structures into the engineering curriculum at the PI's institution and enriches outreach programs through the creation of educational videos on synthesis and electrochemical properties of materials. A variation on the gameshow Family Feud focused on electrochemistry is being used to attract more students to STEM fields.TECHNICAL DETAILS: This research is focused on understanding how face-to-face heterostructured interfaces can be created and controlled in layered materials. The aim is to produce 2D oxide-based heterostructures with high electron and ion transport leading to improved energy storage capabilities in Li-ion, Na-ion and K-ion batteries. Layered transition metal oxides show high redox activity in intercalation reactions and relatively high working potentials, making them especially attractive for use as cathodes in energy storage devices. However, the low electronic conductivity of most oxides limits their performance. To overcome this limitation, layered oxides are combined in unique heterostructured architectures with electronically conductive 2D compounds by controllably alternating atomically thick layers of different individual materials. The 2D heterostructure electrodes are constructed using a sol-gel assisted transition metal oxide synthesis process through (1) chemical pre-intercalation of organic molecules followed by pyrolysis, or (2) addition of solid nanoflakes of conducting phases (graphene or MXene) during the sol-gel process. The improved understanding of the transport of ions and electrons and charge storage mechanisms in layered heterostructured materials achieved in this work is expected to lead to better electrodes and open exciting new research directions. The tailored 2D heterointerfaces make it possible to design new ceramic materials with tunable structures and compositions that exhibit high ion storage capability, rapid electron and ion transport, and enhanced electrochemical stability.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.

非技术描述：这个CAREER项目旨在创造一种全新的具有先进电荷存储能力的陶瓷氧化物材料，为具有更高能量密度、更快充电速度和更长寿命的下一代电池打开大门。这些新材料是二维（2D）氧化物基结构，通过交替氧化物层和电子导电层（如石墨烯基化合物或过渡金属碳化物（MXenes））构建。由此产生的结构表现出对电池电极重要的特性：允许离子移动的空间，以及能够快速传输电子的导电层。将层状金属氧化物和碳基化合物结合在高质量的逐层结构中，为发现和研究界面处发生的新现象提供了机会。这种基本的理解对于创造具有改进的能量和功率能力的电池是重要的。在这项工作中开发的材料和方法与更广泛的应用有关，包括能量存储，电致变色（负责颜色的可逆变化），传感，驱动（或运动控制）和水处理。该项目的跨学科性质吸引了不同的本科生和研究生进行研究。该项目将2D结构的合成和性能整合到PI机构的工程课程中，并通过创建有关材料合成和电化学性能的教育视频丰富了推广计划。一个以电化学为重点的游戏节目Family Feud的变体正在被用来吸引更多的学生进入STEM领域。技术支持：这项研究的重点是了解如何在层状材料中创建和控制面对面的异质结构界面。目的是生产具有高电子和离子传输的2D氧化物基异质结构，从而提高锂离子、钠离子和钾离子电池的储能能力。层状过渡金属氧化物在插层反应中显示出高的氧化还原活性和相对高的工作电位，使得它们特别有吸引力地用作储能装置中的阴极。然而，大多数氧化物的低电子电导率限制了它们的性能。为了克服这一限制，层状氧化物通过可控地交替不同单个材料的原子厚度层而在独特的异质结构架构中与电子导电2D化合物组合。二维异质结构电极是使用溶胶-凝胶辅助过渡金属氧化物合成工艺构建的，通过（1）化学预嵌入有机分子，然后热解，或（2）在溶胶-凝胶过程中添加导电相（石墨烯或MXene）的固体纳米片。在这项工作中实现的层状异质结构材料中离子和电子的传输以及电荷存储机制的改进理解有望导致更好的电极并开辟令人兴奋的新研究方向。定制的2D异质界面使设计具有可调结构和成分的新型陶瓷材料成为可能，这些材料具有高离子存储能力、快速电子和离子传输以及增强的电化学稳定性。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Chemical preintercalation synthesis approach for the formation of new layered tungsten oxides

用于形成新型层状氧化钨的化学预插层合成方法

• DOI: 10.1007/s10853-022-07190-z
• 发表时间: 2022
• 期刊: Journal of Materials Science
• 影响因子: 4.5
• 作者: Clites, Mallory;Blickley, Adam;Cullen, David A.;Pomerantseva, Ekaterina
• 通讯作者: Pomerantseva, Ekaterina

Phase transformation and electrochemical charge storage properties of vanadium oxide/carbon composite electrodes synthesized via integration with dopamine

与多巴胺结合合成的氧化钒/碳复合电极的相变和电化学电荷存储性能

• DOI: 10.1111/jace.18502
• 发表时间: 2022
• 期刊: Journal of the American Ceramic Society
• 影响因子: 3.9
• 作者: Andris, Ryan;Averianov, Timofey;Pomerantseva, Ekaterina
• 通讯作者: Pomerantseva, Ekaterina

Improving Electronic Conductivity of Layered Oxides through the Formation of Two-Dimensional Heterointerface for Intercalation Batteries

• DOI: 10.1021/acsaem.0c00274
• 发表时间: 2020-03
• 作者: Mallory Clites;R. Andris;D. Cullen;K. More;E. Pomerantseva

Composite Li-ion battery cathodes formed via integration of carbon nanotubes or graphene nanoplatelets into chemical preintercalation synthesis of bilayered vanadium oxides

• DOI: 10.1016/j.jallcom.2022.163929
• 发表时间: 2022-01
• 期刊: Journal of Alloys and Compounds
• 影响因子: 6.2
• 作者: T. Averianov;E. Pomerantseva

MXene-Derived Bilayered Vanadium Oxides with Enhanced Stability in Li-Ion Batteries

• DOI: 10.1021/acsaem.0c01906
• 发表时间: 2020-10
• 作者: P. Ridley;Cyra Gallano;R. Andris;C. Shuck;Y. Gogotsi;E. Pomerantseva