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Carbon lacks an extended polyanionic chemistry which appears restricted to carbides with C4-, C22-, and C34- moieties. The most common dimeric anion of carbon atoms is C22- with a triple bond between the two carbon atoms. Compounds containing the dicarbide anion can be regarded as salts of acetylene C2H2 (ethyne) and hence are also called acetylides or ethynides. Inspired by the fact that molecular acetylene undergoes pressure induced polymerization to polyacetylene above 3.5 GPa, it is of particular interest to study the effect of pressure on the crystal structures of acetylides as well. In this work, pressure induced polymerization was attempted with two simple metal acetylides, Li2C2 and CaC2. Li2C2 and CaC2 have been synthesized by a direct reaction of the elements at 800ºC and 1200ºC, respectively. Initial high pressure investigations were performed inside Diamond anvil cell (DAC) at room temperature and in situ Raman spectroscopic measurement were carried out up to 30 GPa. Near 15 GPa, Li2C2 undergoes a transition into a high pressure acetylide phase and around 25 GPa this phase turns amorphous. CaC2 is polymorphic at ambient pressure. Monoclinic CaC2-II does not show stability at pressures above 1 GPa. Tetragonal CaC2-I is stable up to at least 12 GPa above which possibly a pressure-induced distortion occurs. At around 18 GPa, CaC2 turns amorphous. In a subsequent series of experiments both Li2C2 and CaC2 were compressed to 10 GPa in a multi anvil (MA) device and heated to temperatures between 300 and 1100oC for Li2C2, and 300°C to 900°C for CaC2. The recovered products were analyzed by PXRD and Raman spectroscopy. It has been observed that reactions at temperature higher than 900°C were very difficult to control and hitherto only short reaction times could be applied. For Li2C2, a new phase, free of starting material was found at 1100°C. Both the PXRD patterns and Raman spectra of products at 1100oC could not be matched to known forms of carbon or carbides. For CaC2 new reflections in PXRD were visible at 900ºC with the starting material phase.
ContributorsKonar, Sumit (Author) / Häussermann, Ulrich (Thesis advisor) / Seo, Dong (Thesis advisor) / Steimle, Timothy (Committee member) / Wolf, George (Committee member) / Arizona State University (Publisher)
Created2012
Description
Carbon nanomaterials have caught tremendous attention in the last few decades due to their unique physical and chemical properties. Tremendous effort has been made to develop new synthesis techniques for carbon nanomaterials and investigate their properties for different applications. In this work, carbon nanospheres (CNSs), carbon foams (CF), and single-walled carbon nanotubes (SWNTs) were studied for various applications, including water treatment, energy storage, actuators, and sensors.
A facile spray pyrolysis synthesis technique was developed to synthesize individual CNSs with specific surface area (SSA) up to 1106 m2/g. The hollow CNSs showed adsorption of up to 300 mg rhodamine B dye per gram carbon, which is more than 15 times higher than that observed for conventional carbon black. They were also evaluated as adsorbents for removal of arsenate and selenate from water and displayed good binding to both species, outperforming commercial activated carbons for arsenate removal in pH > 8. When evaluated as supercapacitor electrode materials, specific capacitances of up to 112 F/g at a current density of 0.1 A/g were observed. When used as Li-ion battery anode materials, the CNSs achieved a discharge capacity of 270 mAh/g at a current density of 372 mA/g (1C), which is 4-fold higher than that of commercial graphite anode.
Carbon foams were synthesized using direct pyrolysis and had SSA up to 2340 m2/g. When used as supercapacitor electrode materials, a specific capacitance up to 280 F/g was achieved at current density of 0.1 A/g and remained as high as 207 F/g, even at a high current density of 10 A/g.
A printed walking robot was made from common plastic films and coatings of SWNTs. The solid-state thermal bimorph actuators were multifunctional energy transducers powered by heat, light, or electricity. The actuators were also investigated for photo/thermal detection. Electrochemical actuators based on MnO2 were also studied for potential underwater applications.
SWNTs were also used to fabricate printable electrodes for trace Cr(VI) detection, which displayed sensitivity up to 500 nA/ppb for Cr(VI). The limit of detection was shown to be as low as 5 ppb. A flow detection system based on CNT/printed electrodes was also demonstrated.
A facile spray pyrolysis synthesis technique was developed to synthesize individual CNSs with specific surface area (SSA) up to 1106 m2/g. The hollow CNSs showed adsorption of up to 300 mg rhodamine B dye per gram carbon, which is more than 15 times higher than that observed for conventional carbon black. They were also evaluated as adsorbents for removal of arsenate and selenate from water and displayed good binding to both species, outperforming commercial activated carbons for arsenate removal in pH > 8. When evaluated as supercapacitor electrode materials, specific capacitances of up to 112 F/g at a current density of 0.1 A/g were observed. When used as Li-ion battery anode materials, the CNSs achieved a discharge capacity of 270 mAh/g at a current density of 372 mA/g (1C), which is 4-fold higher than that of commercial graphite anode.
Carbon foams were synthesized using direct pyrolysis and had SSA up to 2340 m2/g. When used as supercapacitor electrode materials, a specific capacitance up to 280 F/g was achieved at current density of 0.1 A/g and remained as high as 207 F/g, even at a high current density of 10 A/g.
A printed walking robot was made from common plastic films and coatings of SWNTs. The solid-state thermal bimorph actuators were multifunctional energy transducers powered by heat, light, or electricity. The actuators were also investigated for photo/thermal detection. Electrochemical actuators based on MnO2 were also studied for potential underwater applications.
SWNTs were also used to fabricate printable electrodes for trace Cr(VI) detection, which displayed sensitivity up to 500 nA/ppb for Cr(VI). The limit of detection was shown to be as low as 5 ppb. A flow detection system based on CNT/printed electrodes was also demonstrated.
ContributorsWang, Chengwei, Ph.D (Author) / Chan, Candace K. (Thesis advisor) / Tongay, Sefaattin (Committee member) / Wang, Qing Hua (Committee member) / Seo, Dong (Committee member) / Arizona State University (Publisher)
Created2015
Description
High concentrations of carbon monoxide and particulate matter can cause respiratory disease, illness, and death in high doses. Air pollution is a concern in many urban areas of emerging markets that rely on outdated technologies for transportation and electricity generation; rural air quality is also a concern when noting the high prevalence of products of incomplete combustion resulting from open fires for cooking and heating. Monitoring air quality is an essential step to identifying these and other factors that affect air quality, and thereafter informing engineering and policy decisions to improve the quality of air. This study seeks to measure changes in air quality across spatial and temporal domains, with a specific focus on microclimates within an urban area. A prototype, low-cost air quality monitoring device has been developed to measure the concentrations of particulate matter, ozone, and carbon monoxide multiple times per minute. The device communicates data wirelessly via cell towers, and can run off-grid using a solar PV-battery system. The device can be replicated and deployed across urban regions for high-fidelity emissions monitoring to explore the effect of anthropogenic and environmental factors on intra-hour air quality. Hardware and software used in the device is described, and the wireless data communication protocols and capabilities are discussed.
ContributorsReilly, Kyle (Co-author) / Birner, Michael (Co-author) / Johnson, Nathan (Thesis director) / Gary, Kevin (Committee member) / Barrett, The Honors College (Contributor)
Created2015-05