CATALYTIC COMBUSTION OF HYD RO GEN/ AIR IN MICROCHANNEL REACTOR
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1 55 1 Vol Journal of Chemical Industry and Engineering (China) January 2004 (, ) /,,, H 2 3 % (mol) 15 %(mol), H 2 8 %(mol) h - 1, 90 % TQ A (2004) CATALYTIC COMBUSTIO OF HYD RO GE/ AIR I MICROCHAEL REACTOR CAO Bin, CHE Guangwen and YUA Quan ( Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian , Liaoning, China) Abstract The catalytic combustion reaction of hydrogen/ air mixture was studied in a microchannel reactor The effects of operation conditions on reactor behavior were investigated in detail by using both mathematic modeling and experiment work Explosive mixtures of hydrogen/ air [ 3 % (mol) 15 % (mol) ] were safely handled in this reactor The results showed that catalytic combustion reaction can be operated at high space velocity, isothermal and kinetic controlled regimes Under the conditions of inlet hydrogen concentration of 8 % (mol), reaction temperature of 150, space velocity of 10 6 h - 1, hydrogen conversion was still higher than 90 % Keywords microchannel reactor, hydrogen, catalytic combustion 20 80,,,,, [1 ] [3, ],,,, [2 ] , : :,, 27, Received date : Corresponding author : Prof YUA Quan E - mail : : ( o , o , dicp1ac1cn o ), (o12001cb711203) Foundation item : supported by the ational atural Science (o G ) Foundation of China ( o , o , o ), the Key Program for International Cooperation of Science and Technology (o12001cb711203) and the State Key Development Program for Basic Research of China (o G ) China Academic Journal Electronic Publishing House All rights reserved
![55 1 : 43 [4 6 ] Janicke Pt/ 2Al 2 O 3 113 [5 ] 011 0112 MPa, 30 170,, 310 10 5 110 10 6 h - 1, 3 % / 15 %(mol) GC8810, 1 111 1 10 %, 2 min - 1 350,, 4 h, H 2, 2 1 118 10-4 218 10-4 m 5A, 1 m ; Ar,](/docs-images/91/106019395/images/2-1.jpg "40 ml min - 1 ; 30, 70, 100 ma,, ( GHSV) : GHSV = / ( ) 2 Fig11 Schematic diagram of experimental flow 1 feed gas ; 2 pressure gauge ; 3 mass flow controller ; 4 desiccator ; 5 regulating valve ; 6")
2 55 1 : 43 [4 6 ] Janicke Pt/ 2Al 2 O [5 ] MPa, ,, h - 1, 3 % / 15 %(mol) GC8810, %, 2 min ,, 4 h, H 2, m 5A, 1 m ; Ar, 40 ml min - 1 ; 30, 70, 100 ma,, ( GHSV) : GHSV = / ( ) 2 Fig11 Schematic diagram of experimental flow 1 feed gas ; 2 pressure gauge ; 3 mass flow controller ; 4 desiccator ; 5 regulating valve ; 6 reactor ; 7 heater ; 8 three2way valve ; 9 GC8810 gas chromatograph H 2,, 2 Fig13 Effect of H 2 concentration vs H 2 conversion Fig12 Schematic of reactor T thermocouples ; P pressure transducer ( GHSV = h - 1 ) calculation ; 77 ; 88F ; 97 Length of reaction zone/ m Tabel 1 Parameters of reactor Height of reaction zone/ m Width of reaction zone / m Amount of support / mg Amount of Pt / mg h - 1 (5 % 8 %),,,, H 2 8 % 112 (mol) 150, 90 % , 2Al 2 O 3, 5 m Pt 5, China Academic Journal Electronic Publishing House All rights reserved
3 Fig14 Effect of reaction temperature vs H 2 conversion ( GHSV = h - 1 ) H 2 mole fraction : 10 % ; 8 % ; 5 % ; calculation,,,, 2,, 212 2,, 2 %,, Fig15 Effect of reaction temperature vs H 2 conversion (H 2 mole fraction = 8 %) GHSV/ h - 1 : ; ; ; calculation Table 2 Pressure drop of reactor GHSV 10-4 / h - 1 ( p in - p out ) in / % ,,, ;,,, 2,,,,,,, 6,,, 3 6,, p - 1 Fig16 Effect of space velocity vs H 2 conversion (H 2 mole fraction = 8 %) 100 ; 60 ; calculation Fig17 Effect of GHSV on gas temperature profile (H 2 mole fraction = 8 %) GHSV/ h - 1 : ; ; reactor control temperature/ : 100 ; China Academic Journal Electronic Publishing House All rights reserved
4 55 1 : 45 Fig18 Effect of feed concentration on gas temperature profile( GHSV = h - 1 ) H 2 mole concentration : 10 % ; 8 % ; 5 % reactor control temperature/ : 100 ; 80, k 1, K 1 H 2, K 2 O 2, 3 311,, (DSS) 2S ; ( DSS = Re 100), ( y E i - y S i) 2 (4) i =1, ; ; i ; y i, ; ( < 200 ; S E ), Pe 1000, [ 7] 312 u z 5 m i 5z = 5 ( u z ) 5z = 0 (1) = 5 5 x D 5 m i i 5 x p RT ( m i / M i ) - 1 i m i = m i0 u z = u 0 ( x), z = 0 ; i = 1, 2, 3 H 2 O 2 H 2 O D i 5 m i 5 x = M i r i u z = 0, x = 0 (2) (3) 5 m i K, 0152 %Pt/ SiO 2 D i = 0 u 5 x z = 0, x = H 715 kj mol - 1, x, z 4,, H B, F B = 0105, B 313 H Ikeda H 2 / Air Pt, 1 % 15 %(mol) H 2, ;, [2 ], 3 ( A B C) r H2 = r H2 = r H2 = k 1 C 015 H 2 C O2 (1 + K 1 C H2 + K 2 C O2 ) (A) k 1 C H2 C O2 (1 + K 1 C H2 + K 2 C O2 ) 3 (B) k 1 C H2 C O2 (1 + K 1 C H2 + K 2 C O2 ) 2 (C) Table 3 Estimated kinetic parameters Parameters A B C k 0 / mol - 1 g - 1 s (m - 3 ) 2 E 1 / kj mol H 1 / kj mol H 2 / kj mol K 0,1 / mol m - 3 K 0,2 / mol m DSS MATLAB SQP, 3 Boudart [8 ] China Academic Journal Electronic Publishing House All rights reserved
5 Fig19 Comparison of experimental outlet H 2 Statistic concentration with simulating Table 4 Statistical test of model Model A B C M U Q L F F 0105 ( M, - M - 1) F 0101 ( M, - M - 1) ote : test number, U = i = 1 U sum of squares of regression ; Q ( y - y^ i) 2 ; M argument numbers ; sum of squares of residual error, Q = ( y i - y^ i) 2 ; L total sum of squares, L = ( y i - y i ) 2 ; i = 1 i = 1 U/ M correlation, = 1 - Q/ L ; F variance test, F = Q/ ( - M - 1) p, kpa 314 R, J mol - 1 K - 1 r i i, mol g - 1 s T, K u z,, y, kg m - 3, 2 Pt, g m E, S,, References ;,, 3,, H 2 4 (1), (2) /, h - 1 H 2 8 %(mol), 90 %, (3) C i i, mol m - 3 D i i, kg m - 2 E, kj mol - 1 H, kj mol - 1 s - 1 K i i, mol m - 3 k, mol - 1 g - 1 s - 1 (m - 3 ) 2 M M i i, kg mol - 1 m i i 1 Jensen K F Microchemical Systems : Status, Challenges, and Opportunities AIChE J, 1999, 45 (10) : Hsing I M, Srinivasan R, Harold M P, Jensen K F, Schmidt MA Simulation of Micromachined Chemical Reactors for Heterogeneous Partial Oxidation Reactions Chem Eng Sci, 2000, 55 : Ikeda H, Sato J, Williams F A Surface Kinetics for Catalytic Combustion of Hydrogen2air Mixtures on Platinum at Atmospheric China Academic Journal Electronic Publishing House All rights reserved
6 55 1 : 47 Pressure in Stagnation flows Surface Science, 1995, 326 : Gotz Veser Experimental and Theoretical Investigation of H 2 Oxidation in a High2temperature Catalytic Microreactor Chem Eng Sci, 2001, 56 : Janicke M T, Kestenbaum H, Hagendorf U, Sch th F, Fichtner M, Schubert K The Controlled Oxidation of Hydrogen from an Explosion Mixture of Gases Using a Microstructured Reactor/ Heat Exchange and Pt/ Al 2 O 3 Catalyst Journal of Catalysis, 2000, 191 : Chen Guangwen, Li Shulian, Yuan Quan Microchannel Reactors for Methanol Autothermal Reforming Reaction Chinese Journal of Catalysis 2002, 23 : Yang Yongrong ( ), Cao Bin ( ) Two2dimensional Modeling of 1,22Dichloroethane Cracking Tubular Reactor Journal of Chemical Industry and Engineering ( China) ( ), 2002, 53 : Hanson V F, Boudart M The Reaction Between H 2 and O 2 Over Supported Platinum Catalysts Journal of Catalysis, 1978, 53 : ( ) : 4,4 - / TiO 2 1,3 - RFCC i Co Mn Zn China Academic Journal Electronic Publishing House All rights reserved
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