二氧化鈦與碳黑之複合光觸媒於批式及續流攪拌式反應器降解甲基橙之效能

毛致中

doi:10.6844/NCKU.2011.00492

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二氧化鈦與碳黑之複合光觸媒於批式及續流攪拌式反應器降解甲基橙之效能

The Performance of Titanium Dioxide Incorporated with Carbon Black in Batch and CSTR Reactors for Photodegradation of Methyl Orange

毛致中 , Ph.D　　Advisor：翁鴻山　　

繁體中文 DOI： 10.6844/NCKU.2011.00492

二氧化鈦；碳黑；複合光觸媒；甲基橙；光催化降解；續流攪拌式反應器； titania ； carbon black ； composite catalyst ； photocatalytic degradation ； methyl orange ； CSTR

Abstract │ Reference (90) │ Altmetrics

Abstract 〈TOP〉

為了增強二氧化鈦的光催化性能，本研究使用溶膠凝膠法將二氧化鈦擔載在數種碳材上，製成粉末狀的複合光觸媒，碳材包括活性碳、碳黑、中孔碳與奈米碳管，並且以批式反應器測定複合光觸媒對甲基橙降解反應的光催化活性；也以相同條件製備不含有碳材的純二氧化鈦光觸媒，並與複合光觸媒的光催化活性比較。結果顯示：二氧化鈦與碳材結合的複合光觸媒之光催化活性比純二氧化鈦高，而且碳材的孔洞尺寸、結構、導電性及二氧化鈦與碳材之間的作用力等，都會影響複合光觸媒的光催化活性。碳材中，由於碳黑具有較大的孔洞、高吸附能力、高導電性、二氧化鈦可以附著且分散在碳黑表面等優點，二氧化鈦與碳黑結合的複合光觸媒之光催化活性最高。
二氧化鈦與碳黑結合的比例(簡稱鈦碳比)會影響複合光觸媒的吸附能力及二氧化鈦的光照面積。鈦碳比過高時，因碳量少，使得複合光觸媒的吸附能力薄弱，並且二氧化鈦微粒也會部份聚集，減少被入射光照射的面積；鈦碳比過低時，過多的碳黑會遮蔽入射光照射在二氧化鈦表面。當鈦碳比為1時，光催化活性最高，而且本質反應速率常數比純二氧化鈦之視反應速率常數高。
雖然二氧化鈦與碳黑結合可提高光催化活性，但是仍然比商售Degussa P-25低。為了改良複合光觸媒的效能，接著由原先在空氣環境下進行鍛燒，改在氮氣環境下進行熱處理，並且尋找包括鈦碳比、水添加量及熱處理溫度等最適的製備條件。結果顯示：熱處理溫度提高至600℃，複合光觸媒的光催化活性最高，而且在500、600及700℃進行熱處理的複合光觸媒之光催化活性皆比Degussa P-25高。在光觸媒製備過程中，水添加量的改變對純二氧化鈦有極大的影響，水添加量增加，純二氧化鈦的光催化活性提高，當水量超過5 mL時，純二氧化鈦的光催化活性就不再改變；然而，複合光觸媒的光催化活性並不受水添加量的影響，即使沒有水的存在，600℃熱處理得到的複合光觸媒仍具有高光催化活性。
本研究也探討續流式操作的可行性。由於上述以懸浮態存在於批式反應器之粉末狀觸媒不適用於續流式操作，因此以旋轉塗佈(Spin-coating)技術製備薄膜型觸媒(包括複合光觸媒與純二氧化鈦)，每次將四片固定在反應器中進行續流式操作降解甲基橙，也進行批式操作互相比較。結果顯示：薄膜型複合光觸媒的穩定性極佳，其光催化活性不會隨著使用次數增加而衰減。比較批式與續流式操作的效能，意外地發現兩者之甲基橙去除率相差不大。探究原因是中間產物濃度有很大的影響，由於續流式操作的中間產物濃度比批式操作低，使得薄膜型光觸媒有較多的機會催化甲基橙的降解反應。實驗結果也顯示：薄膜型複合光觸媒的光催化活性仍然比薄膜型純二氧化鈦高。
對於使用薄膜型觸媒的續流攪拌式反應系統， Langmuir-Hinshelwood (L-H)速率表示式只適用於甲基橙濃度少於45 μM的範圍。在這種情況下，反應速率常數及吸附平衡常數皆可求出。當甲基橙濃度高於45 μM時，L-H速率表示式需要經過修正才能適用。

Parallel Abstract 〈TOP〉

For the purpose of improving the photocatalytic performance of titania (TiO2), the powder of composite catalysts were prepared by incorporating TiO2 with different carbon substrates, including activated carbon (AC), carbon black (CB), mesoporous carbon and carbon nanotubes, using the sol-gel method. The photocatalytic activities of composite catalysts were  determined by the photodegradation of methyl orange (MO) in slurry solution using a Pyrex reactor equipped with a circulating cooling tube made of quartz at the center of the reactor. The photocatalytic activity of bare TiO2 prepared under the same condition was also determined and compared with composite catalysts. The results show that the photocatalytic activities of all composite catalysts, higher than that of bare TiO2, are affected by the pore sizes, structure and electrical conductivities of carbon substrates as well as the interactions between TiO2 and carbon substrates. The photocatalytic activity of TiO2/CB is the highest among the compsite catalysts due to the large pore, high adsorption capacity, high electrical conductivity of CB and the particles of TiO2 well dispersed on the surface of CB.
The ratio of TiO2 to CB largely affects the adsorption capacity of composite catalyst and the surface of TiO2 irradiated. When the ratio of TiO2 to CB is higher, the adsorption capacity of composite catalyst is less and the surface of TiO2 irradiated is reduced because of the TiO2 particles aggregated. When the ratio of TiO2 to CB is lower, more CB will shelter the surface of TiO2 irradiated and absorb incident light. An optimal weight ratio of 1 (TCB-1) for the highest photocatalytic activity was found and the intrinsic photocatalytic reaction rate constants of composite catalysts were also found higher than that of bare TiO2. 
However, the photocatalytic activity of TCB-1, which is the highest among the composite catalysts, is lower than Degussa P-25. Therefore, in order to improve the activity of composite catalyst, the calcination of catalysts under air was changed to annealing under N2-flowing surrounding. The optimal preparation condition, including the ratio of TiO2 to CB, the amount of water added and annealing temperature was searched. Experimental results reveal that the photocatalytic activities of composite catalysts annealed at 500, 600 and 700℃ are higher than Degussa P-25 and an optimal annealing temperature of 600℃ maximizes the activity. The amount of water which added into the solution of TiO2 precursor remarkably affects the photocatalytic activities of bare TiO2. The photocatalytic activity of bare TiO2 increases with increasing the amount of water and unchanges when the amount of water added exceeds 5 mL. However, the photocatalytic activities of composite catalysts are not varied with the amount of water added. A high photocatalytic activity can be obtained when the composite catalyst calcined at 600℃ even without the addition of water.
The feasibility of a continuous-flowing system for the MO degradation was also studied. Because the photocatalyst in the powder form may not be used for a continuous-flow stirred-tank reactor (CSTR), the catalysts in the form of thin film (catalyst films) including composite catalyst and bare TiO2, were prepared by spin-coating method. Four pieces of the catalyst films were placed in the reactor for both batch and continuous-flow operations. The results show that the stability of composite catalyst thin film is good and the photocatalytic activity does not decay with the number of operation times. Unexpectedly, the removing percentages of MO for both batch and continuous-flow operations are almost the same. This fact is caused by the suppressing effect of intermediates. The concentration of intermediates for the continuous-flow operation is lower than batch operation, thereby the chance for the degradation of MO on the catalyst surface for the continuous-flow operation is higher. Experimental results also show that the photocatalytic activity of composite catalyst thin film is higher than that of bare TiO2 thin film. 
For the CSTR with the catalyst film, Langmuir-Hinshelwood (L-H) model can only apply to the case where the concentration of MO is less than 45 μM. Under such a circumstance, the rate constant and the adsorption constant can be obtained. When the concentration of MO exceeds 45 μM, the L-H model should be modified.

Reference ( 90 ) 〈TOP〉

Ao, Y.H, Xu, J.J., Fu, D.G. and Yuan, C.W., “A simple route for the preparation of anatase titania-coated magnetic porous carbons with enhanced photocatalytic activity.” Carbon, 46, 596-603, (2008).
連結：
Arana, J., Dona Rodriguez, J.M., Tello Rendon, E., Garriga i Cabo, C., Gonzalez-Diaz, O., Herrera-Melian, J.A., Perez-Pena, J., Colon, G. and Navio, J.A., “TiO2 activation by using activated carbon as a support Part I. Surface characterisation and decantability study.” Appl. Catal. B: Environ., 44, 161-172, (2003).
連結：
Arana, J., Dona Rodriguez, J.M., Tello Rendon, E., Garriga i Cabo, C., Gonzalez-Diaz, O., Herrera-Melian, J.A., Perez-Pena, J., Colon, G. and Navio, J.A., “TiO2 activation by using activated carbon as support part II. Photoreactivity and FTIR study.” Appl. Catal. B: Environ., 44, 153-160, (2003).
連結：
Arana, J., Dona Rodriguez, J.M., Gonzalez Diaz, O., Herrera Melian, J.A. and Perez Pena, J., “The effect of modifying TiO2 on catechol and resorcinol photocatalytic degradation.” J. sol. energ.-T. Asme, 129, 80-86, (2007).
連結：
Auer, E., Freund, A., Pietsch, J. and Tacke, T., “Carbon as supports for industrial precious metal catalysts.” Appl. Catal. A-Gen., 173, 259-271, (1998).
連結：

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