CHAR CRYSTALLINE TRANSFORMATIONS DURING COAL COMBUSTION AND THEIR IMPLICATIONS FOR CARBON BURNOUT
Recent work at Sandia National Laboratories, Imperial College, and the U.K. utility PowerGen, has identified an important mechanism believed to have a large influence on unburned carbon levels from pulverized coal-fired boilers. That mechanism is char carbon crystalline rearrangements on subsecond times scales at temperatures of 1800 - 2500 K, which lead to char deactivation in the flame zones of furnaces. The so-called thermal annealing of carbons is a well known phenomenon, but its key role in carbon burnout has only recently been appreciated, and there is a lack of quantitative data in this time/temperature range. In addition, a new fundamental tool has recently become available to study crystalline transformations, namely high resolution transmission electron microscopy (HRTEM) fringe imaging, which provides a wealth of information on the nature and degree of crystallinity in carbon materials such as coal chars. Motivated by these new developments, this University Coal Research project has been initiated with the following two goals: to determine transient, high-temperature, thermal deactivation kinetics as a function of parent coal and temperature history. to characterize the effect of this thermal treatment on carbon crystalline structure through high-resolution transmission electron microscopy and specialized, quantitative image analysis. Work is currently underway on the following three tasks: Task 1 Experimental technique development. The goal of this task is to develop and demonstrate an apparatus and procedure for measuring transient, high-temperature, thermal deactivation of coal chars. While peak gas temperatures in boilers are often in the range 1800 - 2000 K, peak particle temperatures can be much higher due to high rates of heat release at the particle surface due to exothermic carbon oxidation. The prototype transient heat treatment apparatus is based on an inert-gas purged graphite-rod sample holder that is subjected to rapid Joule heating to temperatures approaching 3000 o C. For the measurement of temperature histories an optical diagnostic is being developed that offers sufficient spatial resolution to distinguish the sample temperature from the substrate temperature. The optical diagnostic is based on a CID camera, a high-power lens, and movable mirrors to projecting multiple, filtered images onto a single chip. Oxidation kinetics are measured on the heat treated samples by a nonisothermal TGA technique. Task 2 Thermal deactivation kinetics. The goal of this task is to quantify thermal char deactivation as a function of temperature history and parent coal, with an emphasis on inert environments at temperatures and times found in combustion systems. The results are to be cast in the form of deactivation kinetics useful for incorporation in combustion models. Task 3 Crystal structure characterization. Crystal structure characterization provides important insight into the mechanisms of thermal char deactivation, and the degree of crystalline transformations has shown a strong correlation with reactivity changes in recent combustion studies [Davis et al., 1992, Beeley et al., 1996]. This task seeks to improve our understanding of char carbon crystalline transformations under combustion conditions by analyzing a large set of HRTEM fringe images for a series of flame-generated chars whose reactivities have been previously reported [Hurt et al., 1995, Beeley et al., 1996]. As a first step, a new technique is being developed for the quantitative analysis of fringe images, extending previous work to allow measurement of a complete set of crystal structure parameters including mean layer size, mean stacking height, interlayer spacing, layer curvature, amorphous fraction, and degree of anisotropy. The resulting database will revealing, at a very fundamental level, the basic differences in char crystal structure due to parent coal rank and to temperature history in the range of interest to combustion systems.
- Research Organization:
- Federal Energy Technology Center (FETC), Morgantown, WV, and Pittsburgh, PA
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- FG22-95PC95205
- OSTI ID:
- 7551
- Report Number(s):
- DE-FG22-95PC95205-05; ON: DE00007551
- Country of Publication:
- United States
- Language:
- English
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