Collaborative Research: Integrated Design of Ultrahigh Surface Area Conductive Materials

合作研究：超高比表面积导电材料集成设计

• 批准号: 1634448
• 负责人: Peter Kroll
• 金额: $ 27.43万
• 依托单位: University of Texas at Arlington
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-07-15 至 2020-02-29
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1634448&HistoricalAwards=false
• 关键词: Collaborative; Research; Integrated; Design; Ultrahigh

Porous materials have great potential in a number of applications, but many challenges exist in the synthesis and manufacturing of high surface-area porous materials that can operate at high temperatures and conduct electricity. This award supports research aiming to integrate theory, experiment, and computational simulations to understand and enable a new class of high temperature stable and ultrahigh surface area porous materials known as silicon oxycarbides (SiOC). Such porous materials have exciting applications in catalysis, gas separation, sensing, electrodes, molecular sieves, thermal insulation, and micro-reactors. Their high thermal stability will enable new applications under harsh conditions where traditional materials have failed. The program integrates multi-layered education and outreach activities and will provide training to multiple graduate and undergraduate students, in materials experimental and simulation research and across two university campuses. This project is aimed at understanding the relationship between the composition and structure of SiOC materials, and the potential for synthesizing materials with high surface area, high temperature stability, and high electrical conductivity. The team will create nanosized pores and domains by tailoring polymer precursors, as well as tailoring crosslinking and pyrolysis conditions. By selective removal of phase-separated species, the approach will provide ultrahigh surface area and high temperature stable materials with 5 nm pores and much desired electrical conductivity. Multi-scale atomistic modeling (ab-initio and large-scale molecular dynamics) will couple to experiment and provide insight in bonding characteristics at interfaces between different phases, driving forces for phase segregation, the evolution of the graphitic substructure, as well as macroscopic properties governed at the nanoscale. A coarse-grain model will combine experimental and computational data and provide an unprecedented and unique platform to model and design the polymer-to-ceramic transformation and post-pyrolysis treatment. This research will establish a new paradigm in molecular design and processing of ultrahigh surface area, high temperature materials with electrical conductivity beyond SiOC, such as SiCN, SiOCN, SiBCN, SiOBC, SiAlCN, and SiAlOC.

多孔材料在许多应用领域具有巨大的潜力，但在合成和制造具有高温和导电性能的高表面积多孔材料方面存在许多挑战。该奖项支持旨在整合理论、实验和计算模拟的研究，以理解和实现一类新的高温稳定和超高表面积的多孔材料，即氧化硅（SiOC）。这种多孔材料在催化、气体分离、传感、电极、分子筛、隔热和微反应器等方面有着令人兴奋的应用。它们的高热稳定性将在传统材料失效的恶劣条件下实现新的应用。该项目整合了多层次的教育和推广活动，并将为多个研究生和本科生提供培训，在材料实验和模拟研究方面，跨越两个大学校园。本项目旨在了解SiOC材料的组成和结构之间的关系，以及合成具有高表面积，高温稳定性和高导电性的材料的潜力。该团队将通过定制聚合物前体，以及定制交联和热解条件来创建纳米级孔隙和结构域。通过选择性去除相分离物质，该方法将提供具有5纳米孔隙和理想导电性的超高表面积和高温稳定材料。多尺度原子模型（从头算和大尺度分子动力学）将与实验相结合，并提供不同相之间界面的键合特征，相分离的驱动力，石墨亚结构的演变以及纳米尺度下的宏观性质。粗粒模型将实验和计算数据相结合，为模拟和设计聚合物到陶瓷的转化和热解后处理提供了前所未有的独特平台。本研究将为SiCN、SiOCN、SiBCN、SiOBC、SiAlCN、SiAlOC等具有超SiOC导电性的超高表面积高温材料的分子设计和加工建立新的范式。

项目成果

Reactive Force Field for Simulations of the Pyrolysis of Polysiloxanes into Silicon Oxycarbide Ceramics

• DOI: 10.1021/acs.jpcc.9b03810
• 发表时间: 2019-06
• 期刊: The Journal of Physical Chemistry C
• 作者: I. Ponomarev;A. V. van Duin;P. Kroll

Impact of Transition Metal Cations on the 29 Si NMR Signal in Metal Oxide Glasses: A DFT Case Study of Hafnia Silica Glass

过渡金属阳离子对金属氧化物玻璃中 29 Si NMR 信号的影响：氧化铪二氧化硅玻璃的 DFT 案例研究

• DOI: 10.1021/acs.jpcc.7b06094
• 发表时间: 2017
• 期刊: The Journal of Physical Chemistry C
• 作者: Ponomarev, Ilia;Kroll, Peter
• 通讯作者: Kroll, Peter

Simulation of Vacuum Ultraviolet Absorption Spectra: Paraffin, Isoparaffin, Olefin, Naphthene, and Aromatic Hydrocarbon Class Compounds

真空紫外吸收光谱的模拟：石蜡、异链烷烃、烯烃、环烷烃和芳香烃类化合物

• DOI: 10.1177/0003702819875132
• 发表时间: 2020
• 期刊: Applied Spectroscopy
• 影响因子: 3.5
• 作者: Mao, James X.;Walsh, Phillip;Kroll, Peter;Schug, Kevin A.
• 通讯作者: Schug, Kevin A.

Paving the way for cristobalite TiO2 and GeO2 attainable under moderate tensile stress: A DFT study of transformation paths and activation barriers in cristobalite-rutile transformations of MO2 (M = Si, Ge, Ti)

为在中等拉伸应力下获得方英石 TiO2 和 GeO2 铺平道路：MO2 (M-=-Si、Ge、Ti) 方英石-金红石转化过程中转化路径和活化势垒的 DFT 研究

• DOI: 10.1016/j.commatsci.2019.109170
• 发表时间: 2019
• 期刊: Computational Materials Science
• 影响因子: 3.3
• 作者: Haseen, Shariq;Kroll, Peter
• 通讯作者: Kroll, Peter

Novel Sulfur‐Containing Cross‐Linking Agent for Si‐Based Preceramic Polymers

新型含硫硅基陶瓷预聚物交联剂

• DOI: 10.1002/macp.201900380
• 发表时间: 2019
• 期刊: Macromolecular Chemistry and Physics
• 影响因子: 2.5
• 作者: Taheri, Poroshat;Bokka, Apparao;Asgari, Parham;Jeon, Junha;Lang, John C.;Campostrini, Renzo;Sorarù, Gian Domenico;Kroll, Peter
• 通讯作者: Kroll, Peter