CH4-CO2 reforming by combination of plasma and catalysts
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摘要: 考察了热等离子体与催化剂协同作用于重整反应过程。实验采用三种不同的模式进行:等离子体单独作用、等离子体与催化剂协同作用、等离子体与催化剂协同作用且部分原料气引入等离子体放电区。结果表明,在模式三下,当原料气的总流量为5 m3/h、CH4/CO2物质的量比为4/6、等离子体的输入功率为14.4 kW时,CH4-CO2重整过程可获得最佳结果,CH4转化率为77.00%、CO2转化率为62.40%、H2选择性为96.70%、CO选择性为88.60%、反应比能为193 kJ/mol、过程的能量转化率为66.4%,该结果已十分接近CH4-H2O(g)重整的技术指标。最佳结果主要得益于模式三下的三种不同的反应路径,放电反应、热化学反应与催化反应。Abstract: To reduce the energy consumption of CO2 reforming of CH4, the synergies of thermal plasma and catalysts in the reforming process was studied in three elaborate modes: plasma only, combination of plasma and catalysts (CPC), and CPC with part of feed gases introduced into plasma discharge region. The optimal specific energy of 193 kJ/mol and energy conversion efficiency of 66.4% were achieved under the conditions of CH4/CO2 of 4/6, input power at 14.4 kW, feed gases of 5 m3/h in mode 3, when the conversions of CH4 and CO2 were 77.00% and 62.40%, and the selectivities of H2 and CO were 88.60% and 96.70%, respectively. These results were closed to that of CH4-H2O(g) reforming process. The excellent performance of the present process benefits from three different reaction courses: discharge reaction, thermochemical reaction and catalytic reaction.
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Key words:
- CH4 /
- CO2 /
- synergies /
- catalysts /
- thermal plasma
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WENDER I. Reactions of synthesis gas[J]. Fuel Process Technol, 1996, 48(3): 189-297. ROSTRUP-NIELSEN J R. New aspects of syngas production and use[J]. Catal Today, 2000, 63(2/4): 159-164. ASHCROFT A T, CHEETHAM A K, GREEN M L H, VERNON P D F. Partial oxidation of methane to synthesis gas-using carbon-dioxide[J]. Nature, 1991, 352(6332): 225-226. WILHELM D J, SIMBECK D R, KARP A D, DICKENSON R L. Syngas production for gas-to-liquids applications: Technologies, issues and outlook[J]. Fuel Process Technol, 2001, 71(1/3): 139-148. TAO X, BAI M, LI X, LONG H, SHANG S, YIN Y, DAI X. CH4-CO2 reforming by plasma-challenges and opportunities[J]. Prog Energy Combust Sci, 2011, 37(2): 113-124. LI M-W, LIU C-P, TIAN Y-L, XU G-H, ZHANG F-C, WANG Y-Q. Effects of catalysts in carbon dioxide reforming of methane via corona plasma reactions[J]. Energy Fuels, 2006, 20(3): 1033-1038. LI M-W, TIAN Y-L, XU G-H. Characteristics of carbon dioxide reforming of methane via alternating current (AC) corona plasma reactions[J]. Energy Fuels, 2007, 21(4): 2335-2339. GOUJARD V, TATIBOUET J-M, BATIOT-DUPEYRAT C. Use of a non-thermal plasma for the production of synthesis gas from biogas[J]. Appl Catal A, 2009, 353(2): 228-235. WANG Q, YAN B-H, JIN Y, CHENG Y. Dry reforming of methane in a dielectric barrier discharge reactor with Ni/Al2O3 catalyst: Interaction of catalyst and plasma[J]. Energy Fuels, 2009, 23(8): 4196-4201. BO Z, YAN J, LI X, CHI Y, CEN K. Plasma assisted dry methane reforming using gliding arc gas discharge: Effect of feed gases proportion[J]. Int J Hydrogen Energy, 2008, 33(20): 5545-5553. RUEANGJITT N, AKARAWITOO C, CHAVADEJ S. Production of hydrogen-rich syngas from biogas reforming with partial oxidation using a multi-stage AC gliding arc system[J]. Plasma Chem Plasma Process, 2012, 32(3): 583-596. 张军旗, 杨永进, 张劲松, 刘强. 常压、脉冲微波强化丝光等离子体作用下甲烷与二氧化碳的反应研究[J].化学学报, 2002, 60(11): 1973-1980. (ZHANG Jun-qi, YANG Yong-jin, ZHANG Jin-song, LIU Qiang. Study on the conversion of CH4 and CO2 using a pulsed microwave plasma under atmospheric pressure[J]. Acta Chimica Sinica, 2002, 60(11): 1973-1980.) FIDALGO B, DOMINGUEZ A, PIS J J, MENENDEZ J A. Microwave-assisted dry reforming of methane[J]. Int J Hydrogen Energy, 2008, 33(16): 4337-4344. GHORBANZADEH A M, MODARRESI H. Carbon dioxide reforming of methane by pulsed glow discharge at atmospheric pressure: The effect of pulse compression[J]. J Appl Phys, 2007, 101(12):123303-123312. LONG H, SHANG S, TAO X, YIN Y, DAI X. CO2 reforming of CH4 by combination of cold plasma jet and Ni/gamma-Al2O3 catalyst[J]. Int J Hydrogen Energy, 2008, 33(20): 5510-5515. GHORBANZADEH A M, LOTFALIPOUR R, REZAEI S. Carbon dioxide reforming of methane at near room temperature in low energy pulsed plasma[J]. Int J Hydrogen Energy, 2009, 34(1): 293-298. LI D, LI X, BAI M, TAO X, SHANG S, DAI X, YIN Y. CO2 reforming of CH4 by atmospheric pressure glow discharge plasma: A high conversion ability[J]. Int J Hydrogen Energy, 2009, 34(1): 308-313. LI X-S, ZHU B, SHI C, XU Y, ZHU A-M. Carbon dioxide reforming of methane in kilohertz spark-discharge plasma at atmospheric pressure[J]. AIChE J, 2011, 57(10): 2854-2860. ZHU B, LI X-S, SHI C, LIU J-L, ZHAO T-L, ZHU A-M. Pressurization effect on dry reforming of biogas in kilohertz spark-discharge plasma[J]. Int J Hydrogen Energy, 2012, 37(6): 4945-4954. TAO X, QI F, YIN Y, DAI X. CO2 reforming of CH4 by combination of thermal plasma and catalyst[J]. Int J Hydrogen Energy, 2008, 33(4): 1262-1265. TAO X, BAI M, WU Q, HUANG Z, YIN Y, DAI X. CO2 reforming of CH4 by binode thermal plasma[J]. Int J Hydrogen Energy, 2009, 34(23): 9373-9378. NI G, LAN Y, CHENG C, MENG Y, WANG X. Reforming of methane and carbon dioxide by DC water plasma at atmospheric pressure[J]. Int J Hydrogen Energy, 2011, 36(20): 12869-12876.
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