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Energy Conversion and Management 51 (2010) 11271133

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Energy Conversion and Management


journal homepage: www.elsevier.com/locate/enconman

Combustion of hydrogen-air in micro combustors with catalytic Pt layer


Yang Wang, Zhijun Zhou, Weijuan Yang *, Junhu Zhou, Jianzhong Liu, Zhihua Wang, Kefa Cen
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, China

a r t i c l e

i n f o

a b s t r a c t
Micro power generators have high power density. However, their key components micro combustors have low stability. In this experiment, catalyst is applied to improve the stability. The catalytic micro combustor is made from an alumina ceramic tube. It has inner diameter of 1 mm, outer diameter of 2.02 mm and length of 24.5 mm. It is prepared through impregnation of aqueous solution of H2PtCl6. The ammability limits and surface temperatures under different operation conditions are measured. The ow rates range from 0.08 to 0.4 L/min. According to the experimental results, catalyst is effective to inhibit extinction. For example, At 0.8 L/min, the stability limit is 0.19314.9 in the non-catalytic combustor. After applying catalyst, the lean limit is near 0, and the rich limit is 29.3. But catalyst is less effective to inhibit blow out. Increasing ow rates also inhibits extinction. In the non-catalytic combustor, while the ow rates increase from 0.08 to 0.2 L/min, the lean stability limit decreases from 0.193 to 0.125. The experimental results indicate that catalyst induces shift downstream in the stoichiometric and rich cases. The numeric simulation veries that the heterogeneous reaction weakens the homogeneous reaction through consuming fuels. Thus, the insufcient heat recirculation makes the reaction region shift downstream. However, lean mixture has intense reaction in the catalytic combustor. It is attributed to the high mass diffusion and low thermal diffusion of lean mixture. 2009 Elsevier Ltd. All rights reserved.

Article history: Received 2 April 2009 Received in revised form 30 November 2009 Accepted 13 December 2009 Available online 12 January 2010 Keywords: Catalytic combustion Micro combustor Stability limits Hydrogen

1. Introduction Micro power generators provide electricity for portable electronic devices. They convert chemical energy into electricity directly, thus have longer operation period [1] and higher energy density than the conventional batteries [24]. The rst micro power generator is suggested in 1996 in Massachusetts Institute of Technology [5]. The prototype is a gas turbine generator less than 1 cm3. To overcome the high friction of micro turbine, energy converters based on thermoelectric or thermophotovoltaic material are lately proposed [1,6]. Micro combustors are the key components of micro power generators. They also produce hydrogen for fuel cell [7,8]. But their stability is low [9]. There are many problems different from the macro-scale combustors. For example, high quenching distance, radical quenching, and uniform temperature distribution [10]. The high surface to volume ratio increases the heat loss. Blow out also occurs easily [11]. Micro combustors require improvement. Swiss-roll combustors could increase the enthalpy of the reactants, thus stabilize ame [12,13]. Increasing the heat recirculation along the combustor wall helps inhibit blow out [14]. Catalytic reaction helps stabilize micro

combustion [15,16]. Processing interior wall of micro combustors chemically inhibits radical quenching [17]. Computational uid dynamics (CFD) simulation is effective to investigate the micro combustion [1820]. The thermal behavior of combustor wall affects micro combustion, thus simulation of uid should be combined with solid wall [2123]. There have been literatures about the catalytic micro combustors. Their ignition [24,25] and reaction processes [26,27] are studied. Catalytic combustors with different structures are also compared [28]. Numeric simulation predicts that catalytic combustors have weak reaction intensity [29], which affects their performances accordingly [30]. It is attributed to the competition between homogeneous and heterogeneous reactions [31]. Solution has been proposed to intensify the homogeneous reaction [32]. However, there are few experiments about the comparison of reaction intensity between catalytic and non-catalytic combustors. In this paper, this comparison is made. The combustors are investigated under different operation conditions. The catalytic combustor shows high stability, but also weak reaction intensity. Combining experimental data and numeric simulation, the details of weakening process are analyzed. 2. Experiment apparatus

* Corresponding author. E-mail address: 10508107@zju.edu.cn (W. Yang). 0196-8904/$ - see front matter 2009 Elsevier Ltd. All rights reserved. doi:10.1016/j.enconman.2009.12.021

Fig. 1 gives the schematic diagram of the experimental apparatus. It is made up of gas feed system, measurement instruments,

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Nomenclature Qa k T x Qsurf At available chemical energy [W] thermal conductivity [W/(m K)] temperature [K] axial location [mm] heat loss rate on the combustor surface [W] transverse section area of the combustor [mm2] ER xp Tp Qcon Qex equivalence ratio, mH2/mAir/(mH2/mAir)stoi axial location of the wall peak temperature peak temperature on the combustor wall [C] average heat conduction rate on the combustor wall [W] exhaust-gas heat loss [W]

and the micro combustor. Hydrogen and air come from the highpressure tanks and ow through the pressure reducing valves and ow meters. After premixed, they are injected into the micro combustor. Two thermal mass ow controllers (D07-7B) are used to control the ow rates of mixture and hydrogen, respectively. A digital data acquisition system (WSP-D806) read the ow-rate signal and transfers it to the computer. An infrared camera (ThermaCam S65) measures the temperature distribution on the combustor surface, which is placed with a distance of 30 cm from the combsutor. The micro combustor is made of an alumina ceramic tube. Its has length of 24.5 mm, inner diameter of 1 mm and outer diameter of 2.02 mm. The catalytic layer is prepared on the surface of the micro combustor by impregnation. The combustor is impregnated in the aqueous solution of hydrochloroplatinic acid (H2PtCl6) [24] (47.4 g/L). After 12 h, H2PtCl6 is dispersed onto the surface. Then, the micro combustor is heated at 500 C for 2 h. Finally, its surface turns black, indicating Pt attached. Fig. 2 shows the transverse section of the micro combustor under micro scope. The weight of the combustor increased by 0.0579 g after impregnation. The weight difference is multiplied by the solution concentration and divided by combustor surface area, then the Pt site density on the combustor surface is about 3.98 ug/mm2. The X-ray powder diffraction patterns (XRD) of the Pt layer are shown in Fig. 3. The peaks around 40, 48, 68 indicate the existence of Pt. The peak around 26 indicates alumina ceramic. Both C (catalytic) and N (non-catalytic) combustors are tested under the similar operation conditions. The stability limits at the total ow rates from 0.08 to 0.4 L/min are measured. The upper and lower stability limits in different cases are found following the process below. Start the micro combustor at the equivalence ratio of 1 to achieve sable ame and wait until it reaches stability. Adjust the ow rate of hydrogen until extinction or blow out occurs, with the total ow rate xed. Adjust the total ow rate and

repeat the steps above until the ammable region over the owrate range from 0.08 to 0.4 L/min is obtained. Heat loss rate (Qloss) and average heat conduction rate (Qcon) of the micro combustor are calculated with Eqs. (1) and (2). The former one is integrated from the location of peak temperature (xp) to the nozzle outlet (xn), which is the reaction area. The latter one is calculated from the location of peak temperature to the upstream end of combustor (xend), which is the preheating area.

Q loss Q cov Q rad R xp Q con


xend

xp

xn
w Sc k dT dx dx

4 DT h db e T 4 w T 1 dSw

xp xend

Fig. 2. Part of the transverse section of the micro combustor. The black rim indicates the catalytic lay of Pt. The overall picture is on the top left.

Fig. 1. Schematic of the experimental apparatus. The solid lines are the gas routes, the long-dashed lines are the signal routes.

Fig. 3. X-ray powder diffraction spectra of alumina ceramic after impregnation of H2PtCl6. The tiny pictures on the top left and right show the spectra detail.

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Qloss is the heat loss rate; Qcov is the natural convective heat loss rate; Qrad is the radiative heat loss rate; DT is the temperature difference between wall and ambient; Sw is the external-wall area; h is the convective heat transfer coefcient; db is the black body radiation constant; e is the radiative emissivity; Tw is the wall temperature; T1 is the ambient temperature; Qcon is the heat conduction rate; Sc is the cross-section area; k is the thermal conductivity of wall; x is the axial location on the combustor wall, the subscripts p, n and end are peak temperature, nozzle outlet and combustor upstream end, respectively. The errors in calculating heat loss and heat conduction are analyzed. The independent parameters measured in the experiments are: wall temperature, ambient temperature, combustor dimension. A constant value is taken as the emissivity of the micro combustor, its error is lower than 4.6%. Uncertainty of empirical correlation of h is less than 5% [33]. Error of Tw is 2%, according to the instruction of infrared camera. Errors of x and combustor diameter are both less than 1%. Error of k is 8.4%. Conclusively, the maximum possible uncertainty of Qloss and Qcon are 12.7% and 8.7%, respectively. Qex has the similar uncertainty as Qloss. Numeric simulation is applied to investigate the combustion process. The conservation equations of mass, chemical species, momentum and energy are solved for two-dimensional steady low Re number laminar ow, heat transfer and chemical reaction using the FLUENT 6.0 [34] CFD package. Grid with cells in the gas/solid phase is employed. The rst-order upwind scheme is used for discretization and the Simple algorithm is employed for the pressurevelocity coupling [35]. The micro combustor is mod-

eled as an axisymmetric 2D system (shown in Fig. 4), and only half of it is simulated for simplicity. Non-uniform mesh is applied, and its density is about 2 103 node/mm2 in the reaction region. Fixed velocity and pressure are specied at the inlet and the outlet, respectively. The uid and solid phases are linked with coupled interface. Measured surface temperature is specied on the outer edge of combustor. It is more accurate than simply specifying it as convective boundary [36]. Detailed chemistry kinetics are applied in both homogenous and heterogeneous reactions. The chemical mechanism provide by Chemkin 4.0 [37] database is imported into Fluent 6.0 for simulation. The homogeneous mechanism involves eight gaseous species (H2, O2, H2O, O, OH, H, HO2, and H2O2) and 20 reaction steps. The heterogeneous mechanism involves ve surface species (Pt(s), H(s), H2O(s), OH(s) and O(s)) and 12 reaction steps.

3. Results and discussion 3.1. Flammability limits Stability limits are shown in Fig. 5. Extinction occurs mainly in the lean cases. On the contrast, blow out occurs mainly in the rich cases. Catalyst is more effective to inhibit extinction. For example, at 0.8 L/min, extinction occurs. In the N combustor, the stability limit is 0.19314.9. In the C combustor, the lean limit decreases to almost 0 (beyond the measurement range of owmeter), and the rich limit increases to 29.3. At 0.4 L/min, blow out occurs. The stability limits are 0.2495.23 and 0.2495.17 in the N and C combustors, respectively. Increasing ow rates inhibits extinction at lower ow rates. For example, in the N combustor, extinction occurs in the lean cases. While the ow rates increase from 0.08 to 0.2 L/min, the lean limits decrease from 0.193 to 0.125. To compare the stability between lean and rich cases, Qa (available chemical energy at the critical ER) at different ow rates are analyzed (given in Fig. 6). The lean cases require less Qa to sustain

Fig. 4. The schematic of the combustor model. Only half of the combustor is simulated. The solid phase has heat exchange with the uid. Heterogeneous reaction occurs on the catalytic surface. The temperature distribution measured on the combustor surface is imported as the boundary condition.

Fig. 6. Qa vs. ow rate from 0.08 to 0.4 L/min.

Fig. 5. Stability limits of the micro combustors at ow rates from 0.08 to 0.4 L/min. (E: extinction, B: blow out).

Fig. 7. T contour in the N combustor at 0.08 L/min [K].

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the combustion, thus they are more stable. For example, in the N combustor, at 0.2 L/min, Qa is 2.11 and 4.70 W in the lean and rich cases, respectively. 3.2. Numeric simulation Fig. 7 gives the T (temperature) contour at 0.08 L/min in the N combustor. The preheating process exists at the inlet, where T increases along the axis until it reaches the ignition point (847 K). The reactants are preheated by the heat diffusion upstream and heat recirculation. The peak temperature is 1774 K and locates around 1.5 mm length, indicating the reaction center. After reaction, T decreases continuously due to the heat loss. H2 mass fraction contour is given in Fig. 8. It decreases abruptly along the axis. At 1 mm length, it reaches 0.006. The sharp increase of T and abrupt decrease of H2 indicate intensive homogeneous reaction. It is veried by the OH mass fraction in Fig. 9, which is 0.0035. Figs. 1012 give the simulation results at 0.2 L/min in the N combustor. The phenomenon indicates that larger amount of fuel intensies the reaction, thus increases the reaction temperature. Because the fuels require more residence time for preheating and reaction, the reaction region extends and shifts downstream. Compared with 0.08 L/min, the peak values of T and OH increase to 1806 K and 0.00968. Reaction center shifts downstream to 1.7 mm length. H2 reaches 0.004 at 1 mm length.

Fig. 1315 give the simulation results at 0.2 L/min in the C combustor. Compared with the N combustor at 0.2 L/min, the results show that under the similar operation condition, catalytic combustor has lower reaction intensity. The peak temperature in the reaction region decreases to 1749 K, and the peak OH decreases to 0.00933. According to the Arrhenius Equation, (Eq. (3), k is the rate constant of chemical reactions; T is the temperature, A is the prefactor and R is the gas constant and Ea is the activation energy), the lower reaction temperature induces slower reaction rate. The lower OH concentration indicates that the homogeneous reaction intensity decreases [32]. Due to the slow reaction rate, the reaction center shifts downstream further to 2 mm length. The H2 contour shows that the H2 reaches 0.004 at 1 mm.

k AeRT

Ea

Fig. 1618 give the simulation results at 0.4 L/min in the C combustor. The simulation at higher ow rate shows that the catalytic combustor has low reaction intensity because the heterogeneous reaction weakens the homogeneous reaction through consuming fuel in the gaseous phase [31]. According to Fig. 17, there is H2 concentrating at the catalytic surface near the inlet, where the mass fraction is 0.032. Accordingly, the H2 concentration near the axis decreases. At the inlet, the premixture has initial mass fraction of 0.28 before reaction. Through preheating, the catalytic surface ad-

Fig. 8. H2 mass fraction contour of the uid region in the N combustor at 0.08 L/min [kg/kg].

Fig. 11. H2 mass fraction contour of the uid region in the N combustor at 0.2 L/min [kg/kg].

Fig. 9. OH mass fraction contour of the uid region in the N combustor at 0.08 L/ min [kg/kg].

Fig. 12. HO mass fraction contour of the uid region in the N combustor at 0.2 L/ min [kg/kg].

Fig. 10. T contour in the N combustor at 0.2 L/min [K].

Fig. 13. T contour in the C combustor at 0.2 L/min [K].

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Fig. 14. H2 mass fraction contour of the uid region in the C combustor at 0.2 L/min [kg/kg].

Fig. 15. HO mass fraction contour of the uid region in the C combustor at 0.2 L/ min [kg/kg].

sorbs gaseous species and heterogeneous reaction develops [38]. Then more H2 diffuses to the catalytic surface. Therefore, the absorption and diffusion of H2 decreases its concentration in the gaseous phase [39]. The homogeneous reaction does not occur until it reaches the ignition temperature. According to the Arrhenius Equation, its reaction rate decreases with the fuel concentration. Therefore, the homogeneous reaction weakens due to lack of fuels. In Fig. 16, the heat released by the catalytic surface at the preheating region also veries the exist of heterogeneous reaction region, which coincides with the H2-concentrating region. The OH contour in Fig. 18 shows the extension and shift downstream of reaction region due to the slow reaction rate and high feed amount of fuel. Compare our simulation results with the ones by Guan-Bang Chen [31], whose combustor has the similar diameter of 1 mm as ours and operated with lower ow rates ranging from 1.3 105 to 1.3 104 L/min. Both results show the similar phenomenon, such as the shift downstream of ame and the extension of reaction region at higher ow rates. Moreover, the reaction temperatures and the mass fractions of OH have the similar quantity level, which are around 1800 K and 0.009 kg/kg, respectively. However, the simulation result by Chen shows more obvious shift downstream of ame in the combustor, which is around 10 mm from the inlet. But the ame in our combustor locates within 5 mm from the inlet, which should be farther than Chens, due to its higher ow rates. In the micro combustor, the temperature distribution on its surface affects the ame location importantly by heat recirculation [14]. Because our boundary condition of surface temperature is obtained from the experiment, the induced simulation result should be more accurate. 3.3. Heat loss Heat loss of the upstream half of combustor affects the combustion directly, and is analyzed. It is from the axial location of 0 to 10 mm. The heat released from combustion is lost by Qsurf (heat loss of the combustor surface) and Qex (heat loss of the exhaust gas). Fig. 19 gives Qsurf and Qex at different ow rates. N combustor has slightly higher Qsurf than C combustor, because catalyst weakens the reaction. For example, at 0.2 L/min, Qsurf are 10.0 and 9.57 W in the N and C combustor, respectively. Therefore, catalyst does not decreases Qsurf effectively. It inhibits extinction mainly because heterogeneous reaction occurs at low temperature. Increasing ow rates also inhibits extinction. Because at high ow rates, there is lower percentages of heat lost from the combus-

Fig. 16. T contour in the C combustor at 0.4 L/min [K].

Fig. 17. H2 mass fraction contour of the uid region in the C combustor at 0.4 L/min [kg/kg].

Fig. 18. HO mass fraction contour of the uid region in the C combustor at 0.4 L/ min [kg/kg].

Fig. 19. Qsurf vs. ow rate at ER of 1 (stoichiometric).

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Fig. 20. xp vs. ow rate at ER of 0.34 (lean), 1 (stoichiometric) and 5.55 (rich).

Fig. 22. Qcon vs. ow rate at ER of 0.34 (lean), 1 (stoichiometric) and 5.55 (rich).

tor wall [10]. At 0.08 L/min, Qsurf occupies 84.5% of the total energy in the N combustor. At 0.2 L/min, it decreases to 78.9%. 3.4. Shift downstream in catalytic combustor Fig. 20 shows the proles of xp (location of surface peak temperature) at different cases. Data from 0.28 to 0.4 L/min in the rich cases is not given, because the combustor does work under the conditions. The proles show that catalyst induces shift downstream except in the lean cases. At ER of 1, xp stays around 0.5 mm in the N combustor, and shifts to 3 mm in the C combustor. At ER of 5.55, xp keeps increasing with the ow rates. But xp in the C combustor is 4 mm higher than in the N combustor. At ER of 0.34, xp increases with ow rates in the N combustor. But in the C combustor, the reaction region is xed around 2 mm. Fig. 21 gives the proles of Tp (peak surface temperature) vs. ow rate. Low Tp indicates weak reaction. Catalyst decreases Tp in the rich and stoichiometric cases, but increases Tp in the lean case. For example, at 0.2 L/min and ER of 1, Tp are 982 and 783 C in the N and C combustors, respectively. At ER of 5.55, Tp decreases from 750 to 561 C after applying catalyst. But at ER of 0.34, Tp increases from 561 to 686 C after applying catalyst. Comparing Figs. 20 and 21, the proles of Tp and xp have the similar trends. It indicates that weak reaction induces shift downstream. Qcon (average heat conduction on the combustor wall) in the preheating region is analyzed. It makes an important route for heat recirulation [40], thus affects the shift downstream [1]. The preheating region is from the location of peak surface temperature to the upstream end of the combustor. Fig. 22 gives the proles of Qcon at different ow rates. Catalyst decreases Qcon in the rich and stoichiometric cases, but increases Qcon in the lean cases. Take 0.2 L/min as an example, at ER of 1, Qcon decreases from 13.3 to 7.45 W after applying catalyst. At ER of 5.55,

Qcon decreases from 9.64 to 2.61 W. But at ER of 0.34, Qcon increases from 6.73 to 8.21 W. Comparing Figs. 20 and 22, the proles of Qcon and xp have the similar trends. It indicates that shift downstream occurs due to insufcient heat recirculation. Conclusive, catalyst weakens the homogeneous reaction in the stoichiometric and rich cases. The lower and uniform temperature distribution [14] decreases the heat recirculation, thus causes shift downstream. But in the lean cases, the combustor has intense reaction after applying catalyst. It is attributed to the high mass diffusion and low thermal diffusion of reactants. The heterogeneous reaction rate depends on mass diffusion [14]. In the lean cases, the diffusion of hydrogen determines the heterogeneous reaction rates, which is higher than oxygen in the rich cases (5.83 104 m2/s vs. 1.53 104 m2/s). The low thermal diffusion of lean mixture also helps preserve heat in the reaction region (2.2 107 of air vs. 1.3 104 m2/s of hydrogen). Therefore, the heterogeneous reaction is more intense in the lean cases than in the other cases.

4. Conclusion According to the comparison between C and N combustors, catalyst inhibits extinction. But it is less effective to inhibit blow out. At 0.8 L/min, the stability limit is 0.19314.9 in the N combustor. With catalyst, the lean limit is close to 0, and the rich limit is 29.3. Heterogeneous reaction occurs at much lower temperature than homogeneous reaction, thus catalyst inhibits extinction. The comparison of Qsurf also shows that catalyst decreases Qsurf slightly, but it is less important to inhibit extinction. At 0.2 L/min with ER of 1, Qsurf are 10.0 and 9.57 W in the N and C combustor, respectively. Increasing ow rates inhibits extinction. Qsurf occupies less percentages of the total energy at higher ow rates, thus the intense reaction inhibits extinction. In the N combustor, from 0.08 to 0.2 L/min, the percentage of Qsurf decreases from 84.8% to 78.9%. Numeric simulation also veries the intense reaction. The peak temperature increases from 1774 to 1806 K, and the peak OH mass fraction increases from 0.0035 to 0.0096. Catalyst induces shift downstream in the rich and stoichiometric cases. C combustor has weak reaction and exhibits uniform temperature distribution, thus the heat recirculation is insufcient. At 0.2 L/min with ER of 1, xp stays around 0.5 mm in the N combustor, and shifts to 3 mm in the C combustor. Accordingly, Tp decreases from 982 to 783 C, and Qcon decreases from 13.3 to 7.45 W. According to numeric simulation, heterogeneous reaction consumes part of the fuel, thus weakens the homogeneous reaction. However, C combustor shows intense reaction in the lean cases, where shift downstream is inhibited. It is attributed to the high mass diffusion and low thermal diffusion of lean mixture.

Fig. 21. Peak temperature vs. ow rate at ER of 0.34 (lean), 1 (stoichiometric) and 5.55 (rich).

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Considering that extinction mainly occurs in the lean cases, it also explains why catalyst inhibits extinction more effectively. Acknowledgements This work is supported by the National Nature Science Foundation of China (No. 50606030), Research Fund for the Doctoral Program of Higher Education of China (No. 20060335124), Program of Introducing Talents of Discipline to University (No. B08026) and National Science Foundation for Distinguished Young Scholars (No. 50525620). References
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