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Nanofluidics: Fundamentals and Applications in Energy Conversion

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Nanofluidics: Fundamentals and Applications in Energy Conversion Nanofluidics: Fundamentals and Applications in Energy Conversion Ling Liu Submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy under the Executive Committee of the Graduate School of Arts and Sciences COLUMBIA UNIVERSITY 2010 © 2010 Ling Liu All Rights Reserved ABSTRACT As a nonwetting liquid is forced to invade the cavities of nanoporous materials, the liquid-solid interfacial tension and the internal friction over the ultra-large specific surface area (usually billions of times larger than that of bulk materials) can lead to a nanoporous energy absorption system (or, composite) of unprecedented performance. Meanwhile, while functional liquids, e.g. electrolytes, are confined inside the nanopores, impressive mechanical-to-electrical and thermal-to-electrical effects have been demonstrated, thus making the nanoporous composite a promising candidate for harvesting/scavenging energy from various environmental energy sources, including low grade heat, vibrations, and human motion. Moreover, by taking advantage of the inverse process of the energy absorption/harvesting, thermally/electrically controllable actuators can be designed with simultaneous volume memory characteristics and large mechanical energy output. In light of all these attractive functionalities, the nanoporous composite becomes a very promising building block for developing the next-generation multifunctional (self-powered, protective and adaptive) structures and systems, with wide potential consumer, military, and national security applications. In essence, all the functionalities of the proposed nanofluidic energy conversion system are governed by nanofluidics, namely, the behavior of liquid molecules and ions when confined in ultra-small nanopores. Nanofluidics is an emerging research frontier where solid mechanics and fluid mechanics meet at the nanoscale. The complex interactions between liquid molecules/ions and solid atoms at the nanointerface, as well as the unique structural, thermal and electrical characteristics of fluids confined in nanocavities collectively represent an outstanding challenge in physical science. A thorough understanding of the science of nanofluids, in particular the detailed molecular mechanisms as well as the roles of various material and system parameters, does not only underpin the development and optimization of the aforementioned nanofluidic energy conversion system, but it also have broad impact on a number of other areas including environmental engineering, chemical engineering, bioengineering, and energy engineering, etc. This dissertation carries out a systematic computational study to explore the fundamental nanofluidic infiltration and transport mechanisms, as well as the thermal and electrical characteristics of the solid-liquid interface. New physical models describing the unique nanofluidic phenomena will be established, where critical parameters, such as the surface tension, contact angle, and viscosity, will be reinvestigated at the nanoscale. The effects of various material and system parameters, such as the solid phase, liquid phase, pore size and pore geometry, as well as the external thermal, electrical and mechanical loads, etc., will be systematically investigated and bridged with the nanofluidic energy conversion processes. The energy conversion efficiencies under various conditions will be evaluated via a synergy between simulation and experiment. Reverse analysis based on the revealed i principles can guide the optimization of the various material and system parameters, which potentially may contribute to the design of highly efficient and sustainable nanofluidic energy conversion devices. Besides the direct impact on the nanofluidic energy conversion, the study is also directly relevant to biological conduction and environmental sustainability, in both of which infiltration and transport play important roles. ii TABLE OF CONTENTS ABSTRACT ................................................................................................................................ I TABLE OF CONTENTS ....................................................................................................... III ACKNOWLEDGEMENTS..................................................................................................VII CHAPTER 1. OVERVIEW AND MOTIVATION..............................................................1 1.1. Grand Challenges of Materials for Enhancing Efficiency of Energy Conversion and Sustainability........................................................................................1 1.2. A New Form of Nanocomposite Combining Nanoporous Materials and Functional Liquids............................................................................................................3 1.2.1. Nanoporous Composite: An Overview..........................................................4 1.2.2. Understanding the Energy Conversion Functionalities ..............................6 1.2.2.1. Energy Absorption................................................................................6 1.2.2.2. Field-responsive Actuation................................................................11 1.2.2.3. Thermal-to-Electrical Energy Harvesting........................................12 1.2.2.4. Mechanical-to-Electrical Energy Harvesting ..................................13 1.2.3. Role of Nanofluidics .......................................................................................14 CHAPTER 2. AN INTRODUCTION TO NANOFLUIDICS..........................................16 2.1. Conventional Fluids vs. Nanofluids .....................................................................17 2.1.1. Conventional Treatment of Capillary Infiltration and Transport............17 2.1.2. Conventional Treatment of Electrical Double Layer..................................17 2.1.3. Uniqueness of Nanofluids..............................................................................18 2.2. Previous Nanofluidic Studies and their Limitations..........................................20 2.2.1. Fluidics in Nanoporous Materials ................................................................20 2.2.2. Fluidics in Nanotubes.....................................................................................21 2.2.3. Fluidics in Biological Channels.....................................................................22 2.2.4. Remaining Issues ............................................................................................22 2.3. Modeling of Nanofluids .........................................................................................23 2.3.1. Empirical Parameters Used in MD Simulation...........................................24 2.3.2. Computational Models and Derivation of Nanofluidic Quantities..........26 2.3.2.1. Infiltration Pressure............................................................................26 2.3.2.2. Static Contact Angle...........................................................................29 2.3.2.3. Shearing Stress.....................................................................................30 2.3.2.4. Interfacial Potential Difference.........................................................32 CHAPTER 3. NANOFLUIDIC INFILTRATION AND TRANSPORT – FUNDAMENTALS AND IMPLICATIONS FOR ENERGY ABSORPTION AND DISSIPATION .........................................................................................................................34 3.1. Nanofluidic Infiltration: Critical Infiltration Pressure and General Size and Geometric Effects............................................................................................................34 3.1.1. Spontaneous Infiltration vs. Pressure-Assisted Infiltration ......................36 3.1.2. General Size and Geometric Effects..............................................................37 3.1.3. Limitations of Laplace-Young Equation......................................................38 iii 3.1.4. Size Effects of Surface Tension and Contact Angle ....................................40 3.1.5. Summary..........................................................................................................41 3.2. Fluidic Infiltration in Molecular-Sized Nanopores ...........................................42 3.2.1. Counterintuitive Cation Size-Dependent Infiltration Pressure................42 3.2.2. Quasi-Periodical Ion Couple Structure........................................................44 3.2.3. Cation Size-Dependent Parameters..............................................................46 3.2.4. Impact of the Unique Ion Couple Structure on Infiltration Pressure......47 3.2.5. Anion Size Effect and Concentration Effect................................................48 3.2.6. Ion Couple Structure: Theoretical Verification ..........................................50 3.2.7. Summary..........................................................................................................52 3.3. Nanofluidic Transport: Viscosity, Shearing Stress and General Size and Loading Rate Effects.......................................................................................................53 3.3.1. Plug-like Flow..................................................................................................53 3.3.2. Shearing Stress: Size and Rate Effects...........................................................55 3.3.3. Nominal Viscosity: Size and Rate Effects.....................................................57
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