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The process of surface modification allows us to combine the structural advantages of materials with the chemical functionality of organic compounds. Attachment of functional organic molecules to surfaces of high surface area substrates yields materials having dense chemical functionality. Materials with meso- and nanoscale features are often used as support substrates because their small-scale features provide very high surface area. Mesoporous silica is one of the most chemically accessible mesoscale materials, and the well-established chemistries of its production and modification lead to controlled pore structure and rapid kinetics. Such materials have seen use as sorbents for environmental remediation of contaminated water. For this application, their high degree of functionality and high-affinity surface chemistries permit a relatively small amount of material to effectively treat a large volume of water. The many advantages of these highly engineered materials come at a relatively high economic cost. The high-affinity chemical functionalities that provide these materials with unprecedented efficiencies also make them correspondingly more difficult to recycle. One-time utilization of these materials makes the cost-per-use high which consequently limits their economically viable applications. The goal of this work has been to explore surface chemistries that will allow high performance, regenerable or recyclable sorbent materials. Shifting from a single-use material to a regenerable platform in which the mesoscale supports are recycled may lower the environmental and economic costs of the material while retaining the advantageous properties of the meso- and nanostructured materials. We chose to approach this goal by developing non-covalent, supramolecular surface modification techniques as alternatives to current surface modification techniques which, almost without exception, are based on covalent modification motifs. Non-covalent attachment of organic molecules to surfaces allows us to avoid the necessity of optimizing the attachment for each class of organic molecule as well as avoid protection and de-protection procedures necessary to attach delicate or reactive functional groups to surfaces. In this way, supramolecular modification processes reduce the cost of material research and development in addition to the costs of material production and use. The process of surface modification allows us to combine the structural advantages of materials with the chemical functionality of organic compounds. Attachment of functional organic molecules to surfaces of high surface area substrates yields materials having dense chemical functionality. Materials with meso- and nanoscale features are often used as support substrates because their small-scale features provide very high surface area. Mesoporous silica is one of the most chemically accessible mesoscale materials, and the well-established chemistries of its production and modification lead to controlled pore structure and rapid kinetics. Such materials have seen use as sorbents for environmental remediation of contaminated water. For this application, their high degree of functionality and high-affinity surface chemistries permit a relatively small amount of material to effectively treat a large volume of water. The many advantages of these highly engineered materials come at a relatively high economic cost. The high-affinity chemical functionalities that provide these materials with unprecedented efficiencies also make them correspondingly more difficult to recycle. One-time utilization of these materials makes the cost-per-use high which consequently limits their economically viable applications. The goal of this work has been to explore surface chemistries that will allow high performance, regenerable or recyclable sorbent materials. Shifting from a single-use material to a regenerable platform in which the mesoscale supports are recycled may lower the environmental and economic costs of the material while retaining the advantageous properties of the meso- and nanostructured materials. We chose to approach this goal by developing non-covalent, supramolecular surface modification techniques as alternatives to current surface modification techniques which, almost without exception, are based on covalent modification motifs. Non-covalent attachment of organic molecules to surfaces allows us to avoid the necessity of optimizing the attachment for each class of organic molecule as well as avoid protection and de-protection procedures necessary to attach delicate or reactive functional groups to surfaces. In this way, supramolecular modification processes reduce the cost of material research and development in addition to the costs of material production and use. This dissertation contains previously published and unpublished co-authored material.

Arsenic is a naturally occurring contaminant in ground water. The link between human exposure to elevated levels of arsenic and the increase in cancerous and non-cancerous diseases is well documented. Consequently, arsenic removal from drinking water has been thoroughly investigated.Lowering the maximum contaminant limit of arsenic (from 50 to 10 ppb) will burden small water utilities, who either lack the financial or technical ability to comply. Adsorption onto solid media has been one of the most attractive options for small water utilities (EPA, 2001), but this process generates huge amounts of arsenic bearing solid residuals (ABSRs) complicating further this matter.Numerous studies have suggested that the Toxicity Characteristics Leaching Procedure (TCLP) does not properly reflect the actual leaching behavior of ASBRs under landfills (Ghosh et al., 2004). This work focuses on testing different arsenic iron- oxide and non- iron- based sorbents, likely to be used for arsenic removal, and assessing the long term behavior of these sorbents under landfill conditions. Our results indicate that microbial processes play a major role in the mobilization of As from granular ferric hydroxide (GFH). Long term operation of GFH sorbent showed that Fe (III) was reduced to Fe(II) and As(V) was reduced to As(III) under anaerobic/reducing conditions. Under semi batch landfill simulation experiments, our results show that non iron based media leached arsenic above the Toxicity Characteristics limit (TC) and it was observed that sorbate (As) might leach at a faster rate than the sorbent itself. It is thought that arsenic mobilization from iron-based sorbent occurs mostly due to iron reduction and its subsequent dissolution. However, measured arsenic leaching rates from the sorbents used in this study are comparable with that of the ferric hydroxide media, which indicates that the mechanism of arsenic mobilization might be independent of the possible dissolution of the sorbent. Despite the fact that non- iron based media may have a higher arsenic adsorption capacity, they leach arsenic at a higher rate than iron based media under our simulated landfill conditions.

Process water is used for cooling and for transporting material in all kinds of industries. To clean the water for reuse, various types of filters can be used. Many conventional process water treatment plants incorporate sand filters, which readily clean the water from suspended matters. However, at some circumstances the sand filters do not remove high enough concentrations of metals. This master thesis compares the water treatment abilities of activated cork, produced by Spikes & Cogs AB, to those of the sand filters used at steel making company Ovako Hofors AB in Hofors. As an on-site pilot study, the thesis investigates the cleaning capacity of three types of activated cork filters: Fats, Oils and Solvents (FOSS) filter, Fast Acting Digesting Enzymes (FADE) filter, and Metal Adsorption and Concentration (MAAC) filter. The cork filters were compared to the sand filters during normal operation and, because of previous problems with the stability of the sand filter performance, during stress tests. The results show that the cleaning capacity of the sand filters is higher than the cleaning capacity of the cork filters at normal operation. At the conditions of the stress tests, at which the sand filters do not function, the cleaning capacity of the cork filters was somewhat lowered but was still well within acceptable limits. An important result from the experiments is that the cork filters neutralize the pH. The sand filters are sensitive to changes in the pH, meaning that the cork filters could function as a buffering unit prior to the sand filters.

Water scarcity has caused severe impact on the entire ecosphere while the climate change is resulting in high frequency of extreme weather conditions, especially extended period of drought. Due to the even increasing world’s population and the continued societal modernization, water scarcity is now one of the leading global challenges towards the development of human society. On the other hand, atmospheric water, accounting for 6 times the water in all rivers on Earth, is emerging as an alternative water resource. This dissertation thoroughly investigated the fully solar energy driven atmospheric water harvesting (AWH) process in a broad scientific and application context. The light-to-heat conversion process of solar photothermal materials was investigated first with a rationally designed droplet-laser system, which in combination with the calculation of heat of absorption of water vapor for various application scenarios, formed a theoretical basis of this dissertation research. As a result, a series of commonly used hydrated salts and their anhydrous counterparts were judiciously selected and successfully proven to be low-cost AWH materials to generate clean fresh water for arid regions. A hydrogel-deliquescent salt composite was further developed as AWH material with a significantly enhanced fresh water production capacity. A new design of nano-capsule encapsulated deliquescent salt was further put forward to enhance water vapor sorption/desorption kinetics, which enabled, for the first time, multiple sorption/desorption cycles within one day and thus multiplied water production capacity. The first-ever continuous AWH device, as opposed to batch-type one, was rationally designed, fabricated, and successfully tested in field conditions outdoors. At last, the dissertation pioneered a novel concept of atmospheric water sorption and desorption cycle for photovoltaic (PV) panel cooling. This dissertation shines significant light on sorption based atmospheric water harvesting and inspires more research efforts on this important research topic.

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