物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2010年
2期
350-358
,共9页
杨志彬%张玉文%张云妍%丁伟中%沈培俊%刘勇%周宇鼎%黄少卿
楊誌彬%張玉文%張雲妍%丁偉中%瀋培俊%劉勇%週宇鼎%黃少卿
양지빈%장옥문%장운연%정위중%침배준%류용%주우정%황소경
焦炉煤气%氢%热力学分析%混合导体透氧膜反应器%NiO/MgO固溶体催化剂
焦爐煤氣%氫%熱力學分析%混閤導體透氧膜反應器%NiO/MgO固溶體催化劑
초로매기%경%열역학분석%혼합도체투양막반응기%NiO/MgO고용체최화제
Coke oven gas%Hydrogen%Thermodynamic analysis%Mixed-conducting membrane reactor%NiO/MgO solid solution catalyst
对焦炉煤气甲烷部分氧化重整热力学进行分析,考察反应温度、CH_4/O_2摩尔比及水蒸气加入量等因素对重整性能的影响,并分析焦炉煤气原始氢含量对其部分氧化重整性能的影响.分析结果表明甲烷转化率均随CH_4/O_2摩尔比和水蒸气加入量的增大以及反应温度的升高而增大.在CH_4/O_2摩尔比1.7-2.1,温度825-900℃及压力1.01×10~5 Pa的反应条件下,可得较好重整性能;甲烷转化率,氢及一氧化碳的选择性分别为91.0%-99.9%,87.0%-93.4%和100%-107%,重整后得到的氢量增大到原始氢量的1.95-2.05倍,每摩尔焦炉煤气消耗的热量仅为2.94 J,同时得出在CH_4/O_2摩尔比2,温度825-900℃及1.01×10~5 Pa条件下,往焦炉煤气内添加体积分数为2%-4%的水蒸气时重整性能得到较大提高;重整后甲烷转化率、氢及一氧化碳选择性分别由92.6%、87.2%、104%增大到98.6%、96.4%、107%.并在BaCo_(0.7)Fe_(0.2)Nb_(0.1)O_(3-δ)透氧膜反应器上研究NiO/MgO固溶体催化剂焦炉煤气部分氧化重整陛能.结果表明该重整反应效果较好,于875℃下获得16.3 mL·cm~(-2)·min~(-1)透氧量,95%甲烷转化率及80.5%氢和106%一氧化碳选择性.且所得实验结果与热力学分析结果符合较好,表明NiO/MgO固溶体催化剂有较好的催化重整性能.
對焦爐煤氣甲烷部分氧化重整熱力學進行分析,攷察反應溫度、CH_4/O_2摩爾比及水蒸氣加入量等因素對重整性能的影響,併分析焦爐煤氣原始氫含量對其部分氧化重整性能的影響.分析結果錶明甲烷轉化率均隨CH_4/O_2摩爾比和水蒸氣加入量的增大以及反應溫度的升高而增大.在CH_4/O_2摩爾比1.7-2.1,溫度825-900℃及壓力1.01×10~5 Pa的反應條件下,可得較好重整性能;甲烷轉化率,氫及一氧化碳的選擇性分彆為91.0%-99.9%,87.0%-93.4%和100%-107%,重整後得到的氫量增大到原始氫量的1.95-2.05倍,每摩爾焦爐煤氣消耗的熱量僅為2.94 J,同時得齣在CH_4/O_2摩爾比2,溫度825-900℃及1.01×10~5 Pa條件下,往焦爐煤氣內添加體積分數為2%-4%的水蒸氣時重整性能得到較大提高;重整後甲烷轉化率、氫及一氧化碳選擇性分彆由92.6%、87.2%、104%增大到98.6%、96.4%、107%.併在BaCo_(0.7)Fe_(0.2)Nb_(0.1)O_(3-δ)透氧膜反應器上研究NiO/MgO固溶體催化劑焦爐煤氣部分氧化重整陛能.結果錶明該重整反應效果較好,于875℃下穫得16.3 mL·cm~(-2)·min~(-1)透氧量,95%甲烷轉化率及80.5%氫和106%一氧化碳選擇性.且所得實驗結果與熱力學分析結果符閤較好,錶明NiO/MgO固溶體催化劑有較好的催化重整性能.
대초로매기갑완부분양화중정열역학진행분석,고찰반응온도、CH_4/O_2마이비급수증기가입량등인소대중정성능적영향,병분석초로매기원시경함량대기부분양화중정성능적영향.분석결과표명갑완전화솔균수CH_4/O_2마이비화수증기가입량적증대이급반응온도적승고이증대.재CH_4/O_2마이비1.7-2.1,온도825-900℃급압력1.01×10~5 Pa적반응조건하,가득교호중정성능;갑완전화솔,경급일양화탄적선택성분별위91.0%-99.9%,87.0%-93.4%화100%-107%,중정후득도적경량증대도원시경량적1.95-2.05배,매마이초로매기소모적열량부위2.94 J,동시득출재CH_4/O_2마이비2,온도825-900℃급1.01×10~5 Pa조건하,왕초로매기내첨가체적분수위2%-4%적수증기시중정성능득도교대제고;중정후갑완전화솔、경급일양화탄선택성분별유92.6%、87.2%、104%증대도98.6%、96.4%、107%.병재BaCo_(0.7)Fe_(0.2)Nb_(0.1)O_(3-δ)투양막반응기상연구NiO/MgO고용체최화제초로매기부분양화중정폐능.결과표명해중정반응효과교호,우875℃하획득16.3 mL·cm~(-2)·min~(-1)투양량,95%갑완전화솔급80.5%경화106%일양화탄선택성.차소득실험결과여열역학분석결과부합교호,표명NiO/MgO고용체최화제유교호적최화중정성능.
A thermodynamic analysis of the partial oxidation of methane (POM) in coke oven gas (COG) was carried out. The optimized conditions were CH_4/O_2 molar ratios of 1.7-2.1 and reaction temperatures of 825-900 ℃. We obtained CH_4 conversions of 91.0%-99.9%, H_2 selectivity of 87.0%-93.4%, and CO selectivity of 100%-107% at 1.01×10~5 Pa. The effect of H_2 in the COG on the performance of POM was also investigated between 825 and 900 ℃. The optimized volume ratio of steam addition was 2%-4% and the molar ratio of CH_4/O_2 was 2 at 1.01×10~5 Pa and 825-900 ℃. A maximum conversion rate of 98.6% was achieved for CH_4 using COG, while the maximum selectivities of H_2 and CO were 96.4% and 107%, respectively. The amount of hydrogen obtained after reforming was doubled despite a thermal consumption of only 2.94 J·mol~(-1) for the COG. The performance of a NiO/MgO solid solution catalyst packed on a BaCo_(0.7)Fe_(0.2)Nb_(0.1)O_(3-δ) (BCFNO) membrane reactor was also investigated for the POM in COG. The reforming process was successfully performed. At 875 ℃, 95% CH_4 conversion, 80.5% H_2 selectivity, and 106% CO selectivity at an oxygen permeation flux of 16.3 mL·cm~(-2)·min~(-1) were achieved. The results for POM reforming in COG on the membrane reactor were consistent with the thermodynamic analysis. The NiO/MgO solid solution catalyst, therefore, has good activity and is suitable for application in hydrogen production.