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Design of Carbonaceous Mercury Adsorbents from Waste Materials Open Access

Descriptions

Other title
Subject/Keyword
Leach
Mercury emission
Activated carbon
Mercury
Sulfur
Mechanism
Biomass
Bromine
Type of item
Thesis
Degree grantor
University of Alberta
Author or creator
Bisson, Teresa M
Supervisor and department
Xu, Zhenghe (Department of Chemical and Materials Engineering)
Examining committee member and department
Wendt, Jost (Department of Chemical Engineering, University of Utah)
Gupta, Rajender (Department of Chemical and Materials Engineering)
Yu, Tong (Department of Civil and Environmental Engineering)
Xu, Zhenghe (Department of Chemical and Materials Engineering)
de Klerk, Arno (Department of Chemical and Materials Engineering)
Department
Department of Chemical and Materials Engineering
Specialization
Chemical Engineering
Date accepted
2014-09-29T11:10:24Z
Graduation date
2014-11
Degree
Doctor of Philosophy
Degree level
Doctoral
Abstract
Mercury is an air pollutant emitted from coal fired power plants. Once released into the environment, mercury undergoes conversion to organomercury compounds, which cause health concerns for both humans and animals. Many studies have been completed with the goal of reducing mercury emissions from flue gases of coal fired power plants using various types of sorbent and catalytic technologies. Mercury removal has most commonly been accomplished in full scale applications through injecting powdered activated carbon-based sorbents into flue gas streams, including several commercial operations in North America. In particular, brominated activated carbon has been proven to be effective at improving the mercury removal efficiency. In order to reduce the cost associated with activated carbon injection, the research of this thesis studied an alternative carbon source, biomass ash waste, which is a by-product from combustion of waste wood for power generation. A chemical-mechanical bromination procedure was used to impregnate the wood ash with bromine (Br-Ash). The mercury capture performance of Br-Ash was found to be comparable to that of a commercial brominated activated carbon (Br-AC). Both Br-Ash and Br-AC captured mercury up to 390oC. Bromine was found to be stable on the Br-Ash up to high temperatures, but leached considerably when exposed to water at all pH values and liquid to solid mass ratios. The mercury concentration in the leachate was very low at neutral pH and high liquid to solid mass ratios. However, at low or high pH values, the mercury concentration in the leachate was above the amount set by the Environmental Protection Agency (EPA) for classifying hazardous waste. Decreasing the liquid to solid mass ratio in the leach tests (from 20:1 to 2:1) further increased the concentration of mercury in the leachate. The high mercury concentration in this case was due to increased bromine concentration in the leachate. Based on these results, it was recommended to consider landfill conditions before disposal of the spent sorbent. In order to reduce environmental impact, the sorbent was re-designed to minimize the amount of Br required for mercury capture. The design of the new sorbent was based on studying the mercury removal mechanisms for Br-Ash compared to Br-AC using x-ray absorption spectroscopy (XAS). The mechanism of mercury capture by Br-Ash was proposed to involve oxidation of the mercury by the surface of the sorbent followed by binding to carbon near Br on the surface. In the case of Br-AC, the mercury was bound to sulfide groups that were not present on the Br-Ash. Understanding the mechanism of mercury capture led to the design of an optimal sorbent containing both Br and sulfide groups. Elemental sulfur was used to impregnate the wood ash, followed by bromination with a lower amount of Br (2 drops). Compared with sorbents containing only 2 drops Br (2D-Br-Ash) or sulfur (S-Ash), the combination of Br and sulfur (2D Br-S-Ash) significantly improved mercury capture. Optimum sulfur loading was achieved at a sulfur:carbon mass ratio of 1:20. The mercury capture mechanism of the 2D Br-S-Ash sorbent was also studied by XAS and was proposed to involve surface enhanced oxidation of mercury, followed by binding of the oxidized mercury to S, Br, or C on the surface of the sorbent. In addition, leach tests on the 2D Br-S-Ash sorbent showed a significant reduction of Hg and Br in the leachate at low liquid to solid ratios. Overall, a new type of carbon based sorbent containing both Br and S was designed with high mercury capture efficiency based on a study of mercury removal mechanisms.
Language
English
DOI
doi:10.7939/R3CR5NM6K
Rights
Permission is hereby granted to the University of Alberta Libraries to reproduce single copies of this thesis and to lend or sell such copies for private, scholarly or scientific research purposes only. Where the thesis is converted to, or otherwise made available in digital form, the University of Alberta will advise potential users of the thesis of these terms. The author reserves all other publication and other rights in association with the copyright in the thesis and, except as herein before provided, neither the thesis nor any substantial portion thereof may be printed or otherwise reproduced in any material form whatsoever without the author's prior written permission.
Citation for previous publication
Bisson, T. M.; MacLean, L. C. W.; Hu, Y.; Xu, Z. Characterization of mercury binding onto a novel brominated biomass ash sorbent by x‑ray absorption spectroscopy. Environ. Sci. Technol. 2012, 46, 12186−12193.Bisson, T. M.; Xu, Z.; Gupta, R.; Maham, Y.; Liu, Y.; Yang, H.; Clark, M.; Patel, M. Chemical-mechanical bromination of biomass ash for mercury removal from flue gases. Fuel. 2013, 108, 54-59.

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