摘 要

論文題目(中文)﹕高壓丙烷火焰預分解雷射激發螢光之氫氧基定量量測
論文題目(英文)﹕QUANTITATIVE MEASUREMENT OF OH
CONCENTRATION WITH LASER-INDUCED PREDISSOCIATIVE
FLUORESCENCE IN HIGH-PRESSURE PROPANE FLAMES

研究生﹕張智銘
指導教授﹕袁曉峰

燃燒是一快速之化學反應，過程會釋放出燃燒熱而所伴隨的卻是一些對環境以及人體健康皆有傷害的污染物質。一般相信丙烷是分子結構較簡單卻又具有常用燃油燃燒反應特徵的燃料。以反應機構模擬而言，一個經過實驗分析及驗證的丙烷燃燒反應機構必定會對更複雜的相關燃油燃燒反應分析具有莫大的幫助，然而燃燒實驗觀測數據的缺乏卻是個不爭的事實；因此本研究即對丙烷平板火焰於油氣當量比介於0.7到1.3之範圍，針對一、三及五大氣壓環境下進行火焰溫度與氫氧基之量測，所提供之定量實驗結果將可進行丙烷燃燒反應機構的驗證及分析。

火焰溫度分佈於反應機構模擬分析上扮演著極重要的角色，尤其對侷限於平焰爐面附近的燃燒反應區計算模擬而言更形關鍵。本實驗利用R-type的熱電偶搭配上輔助定位的光學觀測系統，而能將觀測點延伸至平焰爐面，並以代表反應區的最高溫處為依據進行高空間解析度的量測。此量測結果利用初步的火焰模擬進行Nu參數的估計以進行熱輻射效應之修正，其總體的溫度量測不確定性小於±12 K。

另外，本論文利用高壓丙烷/空氣預混平板火焰，進行火焰中預分解雷射激發螢光之氫氧基(OH-LIPF)定量分析研究。氫氧基分子經由氟化氪準分子雷射從X2Π(v" = 0)激發至A2Σ+(v' = 3)，觀察(3,2)的螢光光譜。在後焰區域中以氫氧基螢光強度對火焰模擬計算的氫氧基濃度做校正，而火焰模擬計算結果是利用美國Sandia國家實驗室的火焰程式(flame code)，配合GRI 3.0反應機構而得。經由對冷卻速率與Voigt profile的嚴謹計算，並且對室內空氣中之N2 Raman訊號做校正，氫氧基的濃度與螢光訊號之間的關係式可用下述方程式表示：
[OH]=[(1.120±0.263)E+16].Sf.
(A+Q+P)/(RN2.A.B.fB.Gv)

OH-LIPF量測而得的校正曲線可以正確的描述出氫氧基的濃度變化，其最大誤差不超過±25%，此結果與目前文獻上有限的研究作比較具有相當好的一致性。

本研究依據GRI 3.0反應機構為基礎，由文獻上廣泛的收集而建立一含碳數達C6的嘗試反應機構，以用於模擬分析火焰中氫氧基之分佈；此反應機構初步驗證發現，對於偏離貧油狀態(phi>=0.9)亦即是後焰區其計算模擬結果皆未能再現實驗的量測，而藉由所建立的嘗試反應機構進行測試分析，於富油環境下發現其主要原因是在一些所產生的大分子具有相當明顯之熱化學資料不確定性所導致。

此論文提出一具有廣泛化的OH-LIPF校正常數，同時透過實驗量測進行丙烷火焰燃燒中OH濃度及溫度分佈曲線之定量分析，另外所建立之嘗試反應機構則提供丙烷或更高碳燃油燃燒研究之重要依據。

Abstract

QUANTITATIVE MEASUREMENT OF OH CONCENTRATION WITH LASER-INDUCED PREDISSOCIATIVE FLUORESCENCE
IN HIGH-PRESSURE PROPANE FLAMES

Student : Chih-Ming Chang
Advisor : Hsiao-Feng T. Yuan

ABSTRACT

Combustion is a fast chemical reaction that liberates heat and some relevant pollutants. It is generally accepted that propane is the simplest hydrocarbon fuel that has reaction characteristics representative of many technical fuels. Therefore, from a modelling perspective, a propane combustion mechanism that has been verified against experimental data would be a valuable tool for analyzing and interpreting the combustion phenomena involving typical hydrocarbon fuels. However, the lack of precision measurements of propane flame is still an imperative need in the development of a combustion mechanism. In this work, we provide quantitative measurements of hydroxyl radicals (OH) and temperatures in premixed propane/air flat flames at equivalence ratios from 0.7 to 1.3 and pressures of 1, 3 and 5 bars.

The accuracy and the spatial resolution of the measured temperatures is an important factor to the precision of the corresponding flame simulations, especially in the reaction zone near the burner surface. In this work, a carefully constructed thermocouple (R-type, 50 mm) assisted by an optical positioning system was used to identify the temperatures above the burner surface. These measured temperatures were corrected with the radiation heat loss in which the Nusellt (Nu) number was estimated by the preliminary flame simulations. The uncertainties of the final corrected temperatures were estimated to within ±12 K.

A quantitative analysis of OH-LIPF in high-pressure (1 ~ 5 bars) premixed propane flames (phi = 0.7 ~ 1.3) was performed in this thesis research. OH molecules in the flames were excited from v" = 0 to v' = 3 in the A2Σ+<---X2Π system using a tunable KrF excimer laser where the fluorescence of OH (3, 2) band was observed. The OH fluorescence intensities in the post flame zone were calibrated against the OH concentrations calculated by the lean (phi = 0.7, 0.8) flame simulation using the Sandia flame code in conjunction with the GRI 3.0 mechanism. With careful evaluations of quenching rates and Voigt profiles, and after normalizing the OH fluorescence against N2 Raman signal, a linear relation was derived to be
[OH]=[(1.120±0.263)E+16].Sf.
(A+Q+P)/(RN2.A.B.fB.Gv)
The uncertainty of this semi-theoretical correlation between the OH number density (#/cm3) and the fluorescence intensities was ±25%. These calibration results were compared to the limited data in the literature and showed good consistency.

A comprehensive trial mechanism based on the GRI 3.0 mechanism and up to C6 oxidation reactions as found in the literature was carefully composed and tested against the measured OH distributions. Flame simulations were performed and showed that the mechanism still failed to predict the OH concentrations, even in the post flame zone for slightly richer propane flames (phi>= 0.9). An analysis determined that the major cause of the inadequacy of the flame simulations was the inaccuracy of the thermochemical data of the large molecules involved in rich flame oxidation reactions.

In this work, a universal OH-LIPF calibration correlation was deduced, the quantitative OH concentration profiles as well as the temperature profiles of premixed propane/air flat flames were analyzed, and a trial mechanism up to C6 oxidation reactions was composed, the results of which can serve as important information for further studies of the chemical kinetics and the mechanisms of propane or higher hydrocarbon fuels combustion.

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