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Title: Development and Evaluation of Nanoscale Sorbents for Mercury Capture from Warm Fuel Gas. Evaluation of Binary Metal Oxides for Mercury Capture

Abstract

Gas Technology Institute (GTI), in collaboration with Nanoscale Materials, Inc. (NanoScale), is developing and evaluating several nanocrystalline sorbents for capture of mercury from coal gasifier (such as IGCC) warm fuel gas. The focus of this study is on the understanding of fundamental mechanism of interaction between mercury and nanocrystalline sorbents over a range of fuel gas conditions. Detailed chemical and structural analysis of the sorbents will be carried out using an array of techniques, such as XPS, SEM, XRD, N{sub 2}-adsorption, to understand the mechanism of interaction between the sorbent and mercury. The proposed nanoscale oxides have significantly higher reactivities as compared to their bulk counterparts, which is a result of high surface area, pore volume, and nanocrystalline structure. These metal oxides/sulfides will be evaluated for their mercury-sorption potential in an experimental setup equipped with state-of-the-art analyzers. Initial screening tests will be carried out in N{sub 2} atmosphere, and two selected sorbents will be evaluated in simulated fuel gas containing H{sub 2}, H{sub 2}S, Hg and other gases. The focus will be on development of sorbents suitable for higher temperature (420-640 K) applications. In this Task, several formulations of binary metal oxide-based sorbents were prepared and evaluated for capture ofmore » mercury (Hg) in simulated fuel gas (SFG) atmosphere at temperatures in the range 423-533 K. The binary metal oxides with high surface area were found to be more effective, confirming the role of sorbent surface in mercury capture. These binary sorbents were found to be effective in capturing Hg at 473 and 533 K, with Hg capture decreasing at higher temperature. Based on the desorption studies, physical adsorption was found to be the dominant capture mechanism with lower temperatures favoring capture of Hg.« less

Authors:
;
Publication Date:
Research Org.:
Gas Technology Institute
Sponsoring Org.:
USDOE
OSTI Identifier:
881998
DOE Contract Number:
FC26-04NT42312
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; ADSORPTION; COAL; DESORPTION; EVALUATION; FUEL GAS; GASES; MERCURY; OXIDES; SURFACE AREA; X-RAY DIFFRACTION; X-RAY PHOTOELECTRON SPECTROSCOPY

Citation Formats

Raja A. Jadhav, and Howard Meyer. Development and Evaluation of Nanoscale Sorbents for Mercury Capture from Warm Fuel Gas. Evaluation of Binary Metal Oxides for Mercury Capture. United States: N. p., 2006. Web. doi:10.2172/881998.
Raja A. Jadhav, & Howard Meyer. Development and Evaluation of Nanoscale Sorbents for Mercury Capture from Warm Fuel Gas. Evaluation of Binary Metal Oxides for Mercury Capture. United States. doi:10.2172/881998.
Raja A. Jadhav, and Howard Meyer. Sat . "Development and Evaluation of Nanoscale Sorbents for Mercury Capture from Warm Fuel Gas. Evaluation of Binary Metal Oxides for Mercury Capture". United States. doi:10.2172/881998. https://www.osti.gov/servlets/purl/881998.
@article{osti_881998,
title = {Development and Evaluation of Nanoscale Sorbents for Mercury Capture from Warm Fuel Gas. Evaluation of Binary Metal Oxides for Mercury Capture},
author = {Raja A. Jadhav and Howard Meyer},
abstractNote = {Gas Technology Institute (GTI), in collaboration with Nanoscale Materials, Inc. (NanoScale), is developing and evaluating several nanocrystalline sorbents for capture of mercury from coal gasifier (such as IGCC) warm fuel gas. The focus of this study is on the understanding of fundamental mechanism of interaction between mercury and nanocrystalline sorbents over a range of fuel gas conditions. Detailed chemical and structural analysis of the sorbents will be carried out using an array of techniques, such as XPS, SEM, XRD, N{sub 2}-adsorption, to understand the mechanism of interaction between the sorbent and mercury. The proposed nanoscale oxides have significantly higher reactivities as compared to their bulk counterparts, which is a result of high surface area, pore volume, and nanocrystalline structure. These metal oxides/sulfides will be evaluated for their mercury-sorption potential in an experimental setup equipped with state-of-the-art analyzers. Initial screening tests will be carried out in N{sub 2} atmosphere, and two selected sorbents will be evaluated in simulated fuel gas containing H{sub 2}, H{sub 2}S, Hg and other gases. The focus will be on development of sorbents suitable for higher temperature (420-640 K) applications. In this Task, several formulations of binary metal oxide-based sorbents were prepared and evaluated for capture of mercury (Hg) in simulated fuel gas (SFG) atmosphere at temperatures in the range 423-533 K. The binary metal oxides with high surface area were found to be more effective, confirming the role of sorbent surface in mercury capture. These binary sorbents were found to be effective in capturing Hg at 473 and 533 K, with Hg capture decreasing at higher temperature. Based on the desorption studies, physical adsorption was found to be the dominant capture mechanism with lower temperatures favoring capture of Hg.},
doi = {10.2172/881998},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Sat Apr 01 00:00:00 EST 2006},
month = {Sat Apr 01 00:00:00 EST 2006}
}

Technical Report:

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  • The Mercury Testing Experimental System available in GTI's Hot Gas Cleanup laboratory was prepared for the project. As part of the shakedown testing, the system was checked for possible gas leaks and fixed. In addition, the mass flow controller was calibrated for diluent N{sub 2} stream. A major part of the shakedown testing was the calibration of the semi-continuous mercury analyzer and the verification of the permeation rate of the mercury permeation tube. It was found that the analyzer's mercury concentration measurements were much lower than expected from the permeation tube rate calculations. Vendors of the analyzer and the permeationmore » tube are contacted to find out the reason for this discrepancy.« less
  • Several nanocrystalline sorbents were synthesized by GTI's subcontractor NanoScale Materials, Inc. (NanoScale) and submitted to GTI for evaluation. A total of seventeen sorbent formulations were synthesized and characterized by NanoScale, including four existing sorbent formulations (NanoActive{trademark} TiO{sub 2}, NanoActive CeO{sub 2}, NanoActive ZnO, and NanoActive CuO), three developmental nanocrystalline metal oxides (MnO{sub 2}, MoO{sub 3}, and Cr{sub 2}O{sub 3}), and ten supported forms of metal oxides. These sorbents were characterized for physical and chemical properties using a variety of analytical equipments, which confirmed their nanocrystalline structure.
  • Gas Technology Institute (GTI), in collaboration with Nanoscale Materials, Inc. (NanoScale), is developing and evaluating several nanocrystalline sorbents for capture of mercury from coal gasifier (such as IGCC) warm fuel gas. The focus of this study is on the understanding of fundamental mechanism of interaction between mercury and nanocrystalline sorbents over a range of fuel gas conditions. Detailed chemical and structural analysis of the sorbents will be carried out using an array of techniques, such as XPS, SEM, XRD, N{sub 2}-adsorption, to understand the mechanism of interaction between the sorbent and mercury. The proposed nanoscale oxides have significantly higher reactivitiesmore » as compared to their bulk counterparts, which is a result of high surface area, pore volume, and nanocrystalline structure. These metal oxides/sulfides will be evaluated for their mercury-sorption potential in an experimental setup equipped with state-of-the-art analyzers. Initial screening tests will be carried out in N{sub 2} atmosphere, and two selected sorbents will be evaluated in simulated fuel gas containing H{sub 2}, H{sub 2}S, Hg and other gases. The focus will be on development of sorbents suitable for higher temperature (420-640 K) applications. As part of this Task, several metal oxide (MeO)-based sorbents were evaluated for capture of mercury (Hg) in simulated fuel gas (SFG) atmosphere at temperatures in the range 423-533 K. Nanocrystalline sorbents prepared by NanoScale Materials, Inc. (NanoScale) as well as in-house (GTI) sorbents were evaluated. These supported sorbents were found to be effective in capturing Hg at 423 and 473 K. Based on the desorption studies, physical adsorption was found to be the dominant capture mechanism with lower temperatures favoring capture of Hg. A nanocrystalline sorbent formulation captured 100% of Hg at 423 K with a 4-hr Hg-sorption capacity of 2 mg/g (0.2 wt%) in SFG. The high capacity of the nanocrystalline sorbent is believed to be the result of its high surface area and small crystallite size.« less
  • Several different types of nanocrystalline metal oxide sorbents were synthesized and evaluated for capture of mercury (Hg) from coal-gasifier warm fuel gas. Detailed experimental studies were carried out to understand the fundamental mechanism of interaction between mercury and nanocrystalline sorbents over a range of fuel gas conditions. The metal oxide sorbents evaluated in this work included those prepared by GTI's subcontractor NanoScale Materials, Inc. (NanoScale) as well as those prepared in-house. These sorbents were evaluated for mercury capture in GTI's Mercury Sorbent Testing System. Initial experiments were focused on sorbent evaluation for mercury capture in N{sub 2} stream over themore » temperature range 423-533 K. These exploratory studies demonstrated that NanoActive Cr{sub 2}O{sub 3} along with its supported form was the most active of the sorbent evaluated. The capture of Hg decreased with temperature, which suggested that physical adsorption was the dominant mechanism of Hg capture. Desorption studies on spent sorbents indicated that a major portion of Hg was attached to the sorbent by strong bonds, which suggested that Hg was oxidized by the O atoms of the metal oxides, thus forming a strong Hg-O bond with the oxide. Initial screening studies also indicated that sulfided form of CuO/alumina was the most active for Hg capture, therefore was selected for detailed evaluation in simulated fuel gas (SFG). It was found that such supported CuO sorbents had high Hg-sorption capacity in the presence of H{sub 2}, provided the gas also contained H{sub 2}S. Exposure of supported CuO sorbent to H{sub 2}S results in the formation of CuS, which is an active sorbent for Hg capture. Sulfur atom in CuS forms a bond with Hg that results into its capture. Although thermodynamically CuS is predicted to form unreactive Cu{sub 2}S form when exposed to H{sub 2}, it is hypothesized that Cu atoms in such supported sorbents are in ''dispersed'' form, with two Cu atoms separated by a distance longer than required to form a Cu{sub 2}S molecule. Thus CuS remains in the stable reactive form as long as H{sub 2}S is present in the gas phase. It was also found that the captured Hg on such supported sorbents could be easily released when the spent sorbent is exposed to a H2-containing stream that is free of Hg and H{sub 2}S. Based on this mechanism, a novel regenerative process has been proposed to remove Hg from fuel gas at high temperature. Limited multicyclic studies carried out on the supported Cu sorbents showed their potential to capture Hg from SFG in a regenerative manner. This study has demonstrated that supported nanocrystalline Cu-based sorbents have potential to capture mercury from coal syngas over multiple absorption/regeneration cycles. Further studies are recommended to evaluate their potential to remove arsenic and selenium from coal fuel gas.« less