skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Advanced Gasification Mercury/Trace Metal Control with Monolith Traps

Abstract

Three potential additives for controlling mercury emissions from syngas at temperatures ranging from 350 to 500 F (177 to 260 C) were developed. Current efforts are being directed at increasing the effective working temperature for these sorbents and also being able to either eliminate any potential mercury desorption or trying to engineer a trace metal removal system that can utilize the observed desorption process to repeatedly regenerate the same sorbent monolith for extended use. Project results also indicate that one of these same sorbents can also successfully be utilized for arsenic removal. Capture of the hydrogen selenide in the passivated tubing at elevated temperatures has resulted in limited results on the effective control of hydrogen selenide with these current sorbents, although lower-temperature results are promising. Preliminary economic analysis suggests that these Corning monoliths potentially could be more cost-effective than the conventional cold-gas (presulfided activated carbon beds) technology currently being utilized. Recent Hg-loading results might suggest that the annualized costs might be as high as 2.5 times the cost of the conventional technology. However, this annualized cost does not take into account the significantly improved thermal efficiency of any plant utilizing the warm-gas monolith technology currently being developed.

Authors:
; ;
Publication Date:
Research Org.:
University Of North Dakota
Sponsoring Org.:
USDOE
OSTI Identifier:
924119
DOE Contract Number:
FC26-05NT42461
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; 54 ENVIRONMENTAL SCIENCES; ADSORBENTS; ACTIVATED CARBON; MATERIALS TESTING; ARSENIC; REGENERATION; ECONOMIC ANALYSIS; COAL GASIFICATION; MERCURY; REMOVAL; SELENIUM HYDRIDES; AIR POLLUTION CONTROL

Citation Formats

Michael L. Swanson, Grant E. Dunham, and Mark A. Musich. Advanced Gasification Mercury/Trace Metal Control with Monolith Traps. United States: N. p., 2007. Web. doi:10.2172/924119.
Michael L. Swanson, Grant E. Dunham, & Mark A. Musich. Advanced Gasification Mercury/Trace Metal Control with Monolith Traps. United States. doi:10.2172/924119.
Michael L. Swanson, Grant E. Dunham, and Mark A. Musich. Thu . "Advanced Gasification Mercury/Trace Metal Control with Monolith Traps". United States. doi:10.2172/924119. https://www.osti.gov/servlets/purl/924119.
@article{osti_924119,
title = {Advanced Gasification Mercury/Trace Metal Control with Monolith Traps},
author = {Michael L. Swanson and Grant E. Dunham and Mark A. Musich},
abstractNote = {Three potential additives for controlling mercury emissions from syngas at temperatures ranging from 350 to 500 F (177 to 260 C) were developed. Current efforts are being directed at increasing the effective working temperature for these sorbents and also being able to either eliminate any potential mercury desorption or trying to engineer a trace metal removal system that can utilize the observed desorption process to repeatedly regenerate the same sorbent monolith for extended use. Project results also indicate that one of these same sorbents can also successfully be utilized for arsenic removal. Capture of the hydrogen selenide in the passivated tubing at elevated temperatures has resulted in limited results on the effective control of hydrogen selenide with these current sorbents, although lower-temperature results are promising. Preliminary economic analysis suggests that these Corning monoliths potentially could be more cost-effective than the conventional cold-gas (presulfided activated carbon beds) technology currently being utilized. Recent Hg-loading results might suggest that the annualized costs might be as high as 2.5 times the cost of the conventional technology. However, this annualized cost does not take into account the significantly improved thermal efficiency of any plant utilizing the warm-gas monolith technology currently being developed.},
doi = {10.2172/924119},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Thu Feb 01 00:00:00 EST 2007},
month = {Thu Feb 01 00:00:00 EST 2007}
}

Technical Report:

Save / Share:
  • Two Corning monoliths and a non-carbon-based material have been identified as potential additives for mercury capture in syngas at temperatures above 400°F and pressure of 600 psig. A new Corning monolith formulation, GR-F1-2189, described as an active sample appeared to be the best monolith tested to date. The Corning SR Liquid monolith concept continues to be a strong candidate for mercury capture. Both monolith types allowed mercury reduction to below 5-μg/m{sup 3} (~5 ppb), a current U.S. Department of Energy (DOE) goal for trace metal control. Preparation methods for formulating the SR Liquid monolith impacted the ability of the monolithmore » to capture mercury. The Energy & Environmental Research Center (EERC)-prepared Noncarbon Sorbents 1 and 2 appeared to offer potential for sustained and significant reduction of mercury concentration in the simulated fuel gas. The Noncarbon Sorbent 1 allowed sustained mercury reduction to below 5-μg/m{sup 3} (~5 ppb). The non-carbon-based sorbent appeared to offer the potential for regeneration, that is, desorption of mercury by temperature swing (using nitrogen and steam at temperatures above where adsorption takes place). A Corning cordierite monolith treated with a Group IB metal offered limited potential as a mercury sorbent. However, a Corning carbon-based monolith containing prereduced metallic species similar to those found on the noncarbon sorbents did not exhibit significant or sustained mercury reduction. EERC sorbents prepared with Group IB and IIB selenide appeared to have some promise for mercury capture. Unfortunately, these sorbents also released Se, as was evidenced by the measurement of H2Se in the effluent gas. All sorbents tested with arsine or hydrogen selenide, including Corning monoliths and the Group IB and IIB metal-based materials, showed an ability to capture arsine or hydrogen selenide at 400°F and 600 psig. Based on current testing, the noncarbon metal-based sorbents appear to be the most effective arsine and hydrogen selenide sorbents. The noncarbon sorbent was able to reduce the concentration to 0 ppb from a starting concentration of 120 ppb. This compares to the target value of 5 ppb (~17μg/m{sup 3}). The EERC-prepared metal-based pellet and coprecipitate sorbents exhibited arsine reductions of 90% or greater, being below 10 ppb. Corning SR Liquid monoliths exhibited brief periods (<1 hour) of attaining 90% arsine reduction but were able to achieve greater than 80% reduction for several hours. With respect to hydrogen selenide, all Group IB and IIB metal-based sorbents tested exhibited 100% reduction from an inlet concentration of approximately 400 ppb. Corning SR Liquid monoliths exhibited an 82% reduction when two monoliths were tested simultaneously in series.« less
  • Two Corning monoliths and a non-carbon-based material have been identified as potential additives for mercury capture in syngas at temperatures above 400°F and pressure of 600 psig. A new Corning monolith formulation, GR-F1-2189, described as an active sample appeared to be the best monolith tested to date. The Corning SR Liquid monolith concept continues to be a strong candidate for mercury capture. Both monolith types allowed mercury reduction to below 5-μg/m3 (~5 ppb), a current U.S. Department of Energy (DOE) goal for trace metal control. Preparation methods for formulating the SR Liquid monolith impacted the ability of the monolith tomore » capture mercury. The Energy & Environmental Research Center (EERC)-prepared Noncarbon Sorbents 1 and 2 appeared to offer potential for sustained and significant reduction of mercury concentration in the simulated fuel gas. The Noncarbon Sorbent 1 allowed sustained mercury reduction to below 5-μg/m3 (~5 ppb). The non-carbon-based sorbent appeared to offer the potential for regeneration, that is, desorption of mercury by temperature swing (using nitrogen and steam at temperatures above where adsorption takes place). A Corning cordierite monolith treated with a Group IB metal offered limited potential as a mercury sorbent. However, a Corning carbon-based monolith containing prereduced metallic species similar to those found on the noncarbon sorbents did not exhibit significant or sustained mercury reduction. EERC sorbents prepared with Group IB and IIB selenide appeared to have some promise for mercury capture. Unfortunately, these sorbents also released Se, as was evidenced by the measurement of H2Se in the effluent gas. All sorbents tested with arsine or hydrogen selenide, including Corning monoliths and the Group IB and IIB metal-based materials, showed an ability to capture arsine or hydrogen selenide at 400°F and 600 psig. Based on current testing, the noncarbon metal-based sorbents appear to be the most effective arsine and hydrogen selenide sorbents. The noncarbon sorbent was able to reduce the concentration to 0 ppb from a starting concentration of 120 ppb. This compares to the target value of 5 ppb (~17μg/m3). The EERC-prepared metal-based pellet and coprecipitate sorbents exhibited arsine reductions of 90% or greater, being below 10 ppb. Corning SR Liquid monoliths exhibited brief periods (<1 hour) of attaining 90% arsine reduction but were able to achieve greater than 80% reduction for several hours. With respect to hydrogen selenide, all Group IB and IIB metal-based sorbents tested exhibited 100% reduction from an inlet concentration of approximately 400 ppb. Corning SR Liquid monoliths exhibited an 82% reduction when two monoliths were tested simultaneously in series.« less
  • The Center for Air Toxic Metals® (CATM®) Program at the Energy & Environmental Research Center (EERC) continues to focus on vital basic and applied research related to the fate, behavior, measurement, and control of trace metals, especially mercury, and the impact that these trace metals have on human health and the environment. For years, the CATM Program has maintained an international perspective, performing research and providing results that apply to both domestic and international audiences, with reports distributed in the United States and abroad. In addition to trace metals, CATM’s research focuses on other related emissions and issues that impactmore » trace metal releases to the environment, such as SO x, NO x, CO 2, ash, and wastewater streams. Of paramount interest and focus has been performing research that continues to enable the power and industrial sectors to operate in an environmentally responsible manner to meet regulatory standards. The research funded by the U.S. Department of Energy’s (DOE’s) National Energy Technology Laboratory (NETL) through CATM has allowed significant strides to be made to gain a better understanding of trace metals and other emissions, improve sampling and measurement techniques, fill data gaps, address emerging technical issues, and develop/test control technologies that allow industry to cost-effectively meet regulatory standards. The DOE NETL–CATM research specifically focused on the fate and control of mercury and trace elements in power systems that use CO 2 control technologies, such as oxycombustion and gasification systems, which are expected to be among those technologies that will be used to address climate change issues. In addition, research addressed data gaps for systems that use conventional and multipollutant control technologies, such as electrostatic precipitators, selective catalytic reduction units, flue gas desulfurization systems, and flue gas-conditioning methods, to understand mercury interactions, develop better control strategies and, in some cases, prevent mercury from being reemitted. This research also addressed stakeholder concerns and questions related to sampling and analytical methods for mercury, especially for continuous mercury monitors and sorbent trap methods for future compliance. Advancements were made toward the development of a much simpler dry-based method for measurement of halogens and trace metals. Finally, this research resulted in significant outcomes related to mercury and selenium concentrations in freshwater fish and how it is associated with other elements, thereby potentially impacting health; this has greatly enhanced the understanding of the second-order mechanism of mercury toxicity. The outcomes of this research have been shared with stakeholders in various domestic and international forums, working groups, conferences, educational settings, and published documents, with information available and accessible to those most impacted or interested in timely and current results on toxic metals. This subtask was funded through the EERC–DOE Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FC26-08NT43291.« less
  • The Energy and Environmental Research Center (EERC) is carrying out an investigation that will provide methods to predict the fate of selected trace elements in integrated gasification combined cycle (IGCC) and integrated gasification fuel cell (IGFC) systems to aid in the development of methods to control the emission of trace elements determined to be air toxics. The goal of this project is to identify the effects of critical chemical and physical transformations associated with trace element behavior in IGCC and IGFC systems. The trace elements included in this project are arsenic, chromium, cadmium, mercury, nickel, selenium, and lead. The researchmore » seeks to identify and fill, experimentally and/or theoretically, data gaps that currently exist on the fate and composition of trace elements. The specific objectives are to (1) review the existing literature to identify the type and quantity of trace elements from coal gasification systems; (2) perform laboratory-scale experimentation and computer modeling to enable prediction of trace element emissions; and (3) identify methods to control trace element emissions. Results are presented and discussed on the partitioning of trace metals and the model design for predicting trace metals behavior.« less