Synthesis and Electrochemical Studies of Intercalated and Framework Substituted Silicon Clathrates

插层和骨架取代的硅包合物的合成和电化学研究

基本信息

批准号：
1206795
负责人：
Candace Chan
金额：
$ 39万
依托单位：
Arizona State University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2012
资助国家：
美国
起止时间：
2012-09-01 至 2016-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1206795&HistoricalAwards=false
关键词：
Synthesis Electrochemical Studies Intercalated Framework

项目摘要

TECHNICAL SUMMARY:With the support of the Solid State and Materials Chemistry program, this project will undertake a detailed structural and electrochemical investigation of silicon clathrates. These materials consist of silicon covalently bonded in cage structures comprised of face-sharing Si20, Si24, and/or Si28 clusters that can be doped by the incorporation of alkali or alkaline guest ions inside the cages. Framework substituted clathrates involve replacing silicon atoms with other metals such as Al and Cu. Key objectives of this project are to understand the electrochemical properties of these materials and how their structure affects those properties, as well as how the structure of the silicon clathrates changes upon electrochemical insertion of guest ions. Direct synthesis methods such as thermal and arc melting will be utilized to make framework substituted silicon clathrates, followed by electrochemical methods to insert and remove guest ions. The project aims are the synthesis and both structural and electrochemical characterization of Li, Na, and Mg intercalated silicon clathrates. Potential outcomes are: (1) the synthesis of new clathrates doped with Li and Mg, (2) the creation of fundamental knowledge regarding the electrochemistry of guest atom insertion and removal in silicon clathrate structures, and (3) the correlation of redox processes with structural changes in silicon clathrates. These outcomes have implications for the development of new anodes for Li, Na, and Mg-ion based rechargeable batteries. In addition, the new knowledge gained related to the synthesis of novel silicon clathrates (such as Li and Mg intercalated clathrate) may be of interest to researchers who study silicon clathrates for other applications such as thermoelectric, superconducting, magnetic, and hard materials. ON-TECHNICAL SUMMARY:Electrochemical energy storage is increasingly becoming an important component of technology and society, with widespread use in portable electronics and soon to be larger roles in electric vehicles and photovoltaic-grid applications. The search for new electrode materials with higher energy and power densities is necessary in order for the future energy storage demands to be realized. Silicon clathrate materials have cage-like structures that can naturally hold guest ions, a feature that may be exploited in energy storage applications. This project seeks to establish fundamental understanding on how the structures of silicon clathrates affect the type and number of guest ions that can be electrochemically inserted and removed, key properties that can lead to the development of new battery electrode materials with improved charge storage capabilities, mechanical integrity, and cycle life. This project will also provide broad training in materials chemistry and electrochemistry for students at the graduate and undergraduate level through the experimental and computational techniques involved. While batteries are used on a daily basis by the general public, most people do not understand the intimate details of these devices. Therefore, the importance and impact of basic materials research as it relates to energy storage devices will be disseminated through teaching at the undergraduate and graduate level, as well as through outreach programs to target K-12 students and the general population. The broad dissemination of the results of this project will enhance scientific understanding in the general public of how ubiquitous energy storage devices work and may also stimulate further research in the scientific community on the application of silicon clathrate materials in other energy and electronic applications.

技术摘要：在固态和材料化学计划的支持下，该项目将对硅外生物进行详细的结构和电化学研究。这些材料由在笼子结构中共价键合的硅组成，这些芯子由面部共享SI20，SI24和/或SI28簇组成，可以通过将碱或碱性离子掺入笼子内的掺入。框架取代的杂质涉及用其他金属（例如Al和Cu）代替硅原子。该项目的关键目标是了解这些材料的电化学特性及其结构如何影响这些特性，以及硅外层的结构在电化学插入来宾离子时如何变化。直接的合成方法（例如热和电弧熔化）将用于使框架取代硅离子物，然后采用电化学方法来插入和去除客体离子。该项目的目的是LI，NA和MG插入硅的合成以及结构和电化学表征。潜在结果是：（1）与Li和Mg掺杂的新覆盖物的合成，（2）建立有关客座原子插入和硅层层结构中的基本知识的基本知识，以及（3）Redox过程的相关性与硅离子层的结构变化的相关性。这些结果对基于LI，NA和MG-ION的可充电电池的新阳极的开发具有影响。此外，研究人员可能会感兴趣的新知识（例如LI和MG插入式覆盖物）与研究硅外层有关其他应用，例如热电，超导，磁性和硬材料等其他应用的研究人员可能感兴趣。现有技术摘要：电化学能源储存越来越成为技术和社会的重要组成部分，在便携式电子产品中广泛使用，并且很快在电动汽车和光伏电网应用中发挥了更大的作用。为了实现未来的储能需求，需要搜索具有较高能量和功率密度的新电极材料。硅离子材料具有类似笼子的结构，可以自然容纳客人离子，这是一种在储能应用中可以利用的功能。该项目旨在建立对硅外层结构如何影响可以在电化学上插入和去除的来宾离子的类型和数量的基本理解，这可以导致具有改善电荷存储能力，机械完整性和周期寿命的新电池电极材料开发新的电池电极材料。该项目还将通过涉及的实验和计算技术为研究生和本科级别的学生提供材料化学和电化学的广泛培训。尽管公众每天使用电池，但大多数人不了解这些设备的私密细节。因此，与储能设备相关的基本材料研究的重要性和影响将通过在本科和研究生层面的教学以及针对K-12学生和一般人群的外展计划来传播。该项目结果的广泛传播将增强公众对无处不在的能源存储设备如何运作的科学理解，并可能激发科学界在其他能源和电子应用中应用硅外层材料应用的进一步研究。

项目成果

期刊论文数量（11）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Electrochemical Cycling of Sodium-Filled Silicon Clathrate

钠填充硅笼形物的电化学循环

DOI：
10.1002/celc.201300104
发表时间：
2014
期刊：
ChemElectroChem
影响因子：
4
作者：
Wagner, Nicholas A.;Raghavan, Rahul;Zhao, Ran;Wei, Qun;Peng, Xihong;Chan, Candace K.
通讯作者：
Chan, Candace K.

Synthesis and Characterization of Empty Silicon Clathrates for Anode Applications in Li-ion Batteries

DOI：
10.1557/adv.2016.434
发表时间：
2016-01-01
期刊：
MRS ADVANCES
影响因子：
0.8
作者：
Chan, Kwai S.;Miller, Michael A.;Chan, Candace K.
通讯作者：
Chan, Candace K.

Surface Properties of Battery Materials Elucidated Using Scanning Electrochemical Microscopy: The Case of Type I Silicon Clathrate

使用扫描电化学显微镜阐明电池材料的表面特性：以 I 型硅包合物为例

DOI：
10.1002/celc.201901688
发表时间：
2019
期刊：
ChemElectroChem
影响因子：
4
作者：
Tarnev, Tsvetan;Wilde, Patrick;Dopilka, Andrew;Schuhmann, Wolfgang;Chan, Candace K.;Ventosa, Edgar
通讯作者：
Ventosa, Edgar

First-Principles Studies of the Lithiation and Delithiation Paths in Si Anodes in Li-Ion Batteries