Fuel-rich methane oxidation in a high-pressure flow reactor studied by optical-fiber laser-induced fluorescence, multi-species sampling profile measurements and detailed kinetic simulations
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- 作者：Heiner Schwarz<sup>asup> ; Michael Geske<sup>bsup> ; C. Franklin Goldsmith<sup>csup> ; Robert Schlö ; gl<sup>asup> ; Raimund Horn<sup>dsup><sup> ; sup><sup>horn@tuhh.de" class="auth_mailsup>
- 关键词：Oxidative coupling of methane (OCM) ; Profile reactor ; Laser-induced fluorescence (LIF) ; Detailed kinetics ; Reactor modeling ; Computational fluid dynamics (CFD)
- 刊名：Combustion and Flame
- 出版年：July 2014
- 年：2014
- 卷：161
- 期：7
- 页码：1688-1700
- 全文大小：1275 K
文摘
A versatile flow-reactor design is presented that permits multi-species profile measurements under industrially relevant temperatures and pressures. The reactor combines a capillary sampling technique with a novel fiber-optic Laser-Induced Fluorescence (LIF) method. The gas sampling provides quantitative analysis of stable species by means of gas chromatography (i.e. <span id="mmlsi51" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si51.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=bde0847bae63546fe3784f986a2b61c0" title="Click to view the MathML source">CH<sub>4sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span>, <span id="mmlsi52" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si52.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=d7718fe98f3e5d8a53dc2b8778d9c79f" title="Click to view the MathML source">O<sub>2sub>,CO,CO<sub>2sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span>, <span id="mmlsi53" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si53.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=5906b0f62e237f828c0fa13131f37481" title="Click to view the MathML source">H<sub>2sub>O,H<sub>2sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span>, <span id="mmlsi54" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si54.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=479ec47eae2a0cf92debf906079ac7b6" title="Click to view the MathML source">C<sub>2sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span><span id="mmlsi55" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si55.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=ff1e30cb00f2302841de6021e0b02643" title="Click to view the MathML source">H<sub>6sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span>, <span id="mmlsi56" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si56.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=70d03de29a87fce688958394a4a3cebc" title="Click to view the MathML source">C<sub>2sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span><span id="mmlsi57" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si57.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=11febb60d456323956cb4e8411f02090" title="Click to view the MathML source">H<sub>4sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span>), and the fiber-optic probe enables in situ detection of transient LIF-active species, demonstrated here for C<span id="mmlsi58" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si58.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=19e67bcdb44e0b611b4b546a10d99e27" title="Click to view the MathML source">H<sub>2sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span>O. A thorough analysis of the LIF correction terms for the temperature-dependent Boltzmann fraction and collisional quenching are presented. The laminar flow reactor is modeled by solving the two-dimensional Navier–Stokes equations in conjunction with a detailed kinetic mechanism. Experimental and simulated profiles are compared. The experimental profiles provide much needed data for the continued validation of the kinetic mechanism with respect to <span id="mmlsi59" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si59.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=076a9bd3687ed83579d6f0671d102c78" title="Click to view the MathML source">C<sub>1sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span> and <span id="mmlsi60" class="mathmlsrc"><span class="formulatext stixSupport mathImg" data-mathURL="/science?_ob=MathURL&_method=retrieve&_eid=1-s2.0-S0010218014000121&_mathId=si60.gif&_user=111111111&_pii=S0010218014000121&_rdoc=1&_issn=00102180&md5=08623bbcffc25eb7f4823d6c052fbf18" title="Click to view the MathML source">C<sub>2sub>span><span class="mathContainer hidden"><span class="mathCode">span>span>span> chemistry; additionally, the results provide mechanistic insight into the reaction network of fuel-rich gas-phase methane oxidation, thus allowing optimization of the industrial process.