厦门大学化学化工学院,福建 厦门 361005
杨霁豪(1996—),男,硕士研究生,20620171151213@stu.xmu.edu.cn
陈秉辉(1961—),男,博士,教授,chenbh@ xmu.edu.cn
收稿:2020-04-11,
修回:2020-07-06,
网络首发:2020-12-17,
纸质出版:2020-12-05
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杨霁豪, 耿莉莉, 叶松寿, 谢建榕, 张诺伟, 陈秉辉. 稳定高效Ru/TiO2-ZrO2催化剂处理苯酚磺酸废水[J]. 化工学报, 2020, 71(12): 5561-5567 DOI: 10.11949/0438-1157.20200407.
YANG Jihao, GENG Lili, YE Songshou, XIE Jianrong, ZHANG Nuowei, CHEN Binghui. Stable and efficient Ru/TiO2-ZrO2 catalysts for catalytic wet air oxidation of phenolsulfonic acid wastewater treatment[J]. CIESC Journal, 2020, 71(12): 5561-5567 DOI: 10.11949/0438-1157.20200407.
杨霁豪, 耿莉莉, 叶松寿, 谢建榕, 张诺伟, 陈秉辉. 稳定高效Ru/TiO2-ZrO2催化剂处理苯酚磺酸废水[J]. 化工学报, 2020, 71(12): 5561-5567 DOI: 10.11949/0438-1157.20200407. DOI:
YANG Jihao, GENG Lili, YE Songshou, XIE Jianrong, ZHANG Nuowei, CHEN Binghui. Stable and efficient Ru/TiO2-ZrO2 catalysts for catalytic wet air oxidation of phenolsulfonic acid wastewater treatment[J]. CIESC Journal, 2020, 71(12): 5561-5567 DOI: 10.11949/0438-1157.20200407. DOI:
催化湿式氧化(CWAO)技术可高效处理有机废水,但现有催化剂的性能,尤其是其稳定性距工业应用还有很大差距。利用ZrO
2
对TiO
2
载体进行掺杂调变,研制出了具有良好稳定性的Ru/TiO
2
-ZrO
2
催化湿式氧化催化剂。结果表明, Ru/TiO
2
催化剂在进行连续5次催化湿式氧化降解苯酚磺酸(phenolsulfonic acid,PSA)废水的反应后,总有机碳(total organic carbon,TOC)转化率由99.1%降低至65.3%;而Ru/TiO
2
-ZrO
2
催化剂在Ti/Zr质量比为9∶1~7∶3范围内,能表现出优良的反应性能,在连续5次反应后, TOC转化率稳定保持在90%以上。X射线仪衍射(XRD)、N
2
吸脱附(BET)、X射线扫描微探针电子能谱仪(XPS)、氢气程序升温还原(H
2
-TPR)和电感耦合等离子体发射光谱(ICP-OES
)表征结果表明:ZrO
2
能够进入TiO
2
的晶格,TiO
2
-ZrO
2
固溶体的生成阻止了TiO
2
由锐钛矿相向金红石相的转变。另外,ZrO
2
的调变加强了Ru与载体的相互作用,有效抑制了活性金属Ru的流失。稳定的载体结构和良好的抗流失性能是Ru/TiO
2
-ZrO
2
催化剂具有优良反应性能的主要原因。
Catalytic wet air oxidation (CWAO) technology can efficiently treat organic wastewater
but the performance of existing catalysts
especially its stability
is far from industrial applications. In this study
ZrO
2
was used to modify TiO
2
support to form the stable Ru/TiO
2
-ZrO
2
catalysts. It was found that the Ru/TiO
2
-ZrO
2
catalysts showed excellent performance for catalytic wet air oxidation of phenolsulfonic acid wastewater. They gave high total organic carbon (TOC) conversions (
>
90%) and remained stable in 5 consecutive running in the Ti/Zr ratio range from 9∶1 to 7∶3. On the other hand
TOC conversion decreased from 99.1% to 65.3% in 5 consecutive cycles for the conventional Ru/TiO
2
catalyst. The characterization results of XRD
BET
XPS
H
2
-TPR and ICP-OES indicated that ZrO
2
can enter the lattice of TiO
2
to form TiO
2
-ZrO
2
solid solution
which prevented the transformation of TiO
2
from anatase to rutile. In addition
the modification of ZrO
2
strengthened the interaction between Ru and the support
which effectively inhibited the leaching of Ru metal. The stable support structure and good anti-loss performance are the main reasons for the excellent reaction performance of Ru/TiO
2
-ZrO
2
catalyst.
林史奇. 化工行业有机废水的处理工艺[J ] . 化工设计通讯, 2019, 45 (1): 222.
Lin S Q. Treatment technology of organic wastewater in chemical industry [J ] . Chemical Engineering Design Communications, 2019, 45 (1): 222.
郭桂悦, 梁忠越, 韩云艳, 等. 曝气生物滤池处理化工污水研究[J ] . 油气田环境保护, 2008, 18 (2): 22-24.
Guo G Y, Liang Z Y, Han Y Y, et al. Treatment of chemical wastewater by biological aerated filter [J ] . Environmental Protection of Oil and Gas Felds, 2008, 18 (2): 22-24.
Comninellis C. Electrocatalysis in the electrochemical conversion/combustion of organic pollutants for waste water treatment [J ] . Electrochemical Acta, 1994, 39 (11/12): 1857-1862.
Andreozzi R, Caprio V, Insola A, et al. Advanced oxidation processes (AOP) for water purification and recovery [J ] . Catalysis Today, 1999, 53 (1): 51-59.
Aaron J J. Advanced oxidation processes in water/wastewater treatment: principles and applications. A review [J ] . Critical Reviews in Environmental Science and Technology, 2014, 44 (23): 2577-2641.
ComninelliS C, Kapalka A, Malato S, et al. Advanced oxidation processes for water treatment: advances and trends for R & D [J ] . Journal of Chemical Technology & Biotechnology, 2008, 83 (6): 769-776.
Barbier J, Oliviero L, Renard B, et al. Role of ceria-supported noble metal catalysts (Ru, Pd, Pt) in wet air oxidation of nitrogen and oxygen containing compounds[J ] . Topics in Catalysis, 2005, 33 (1/2/3/4): 77-86.
Luck F. Wet air oxidation: past, present and future[J ] . Catalysis Today, 1999, 53 (1): 81.
Hamoudi S, Larachi F, Sayari A. Wet oxidation of phenolic solutions over heterogeneous catalysts: degradation profile and catalyst behavior[J ] . Journal of Catalysis, 1998, 177 (2): 247-258.
Debellefontaine H , Chakchouk M, Foussard J N, et al. Treatment of organic aqueous wastes: wet air oxidation and wet peroxide oxidation®[J ] . Environmental Pollution, 1996, 92 (2): 155-164.
Jin G L, Luan M M, Chen T T, et al. Progress of catalytic wet air oxidation technology[J ] . Arabian Journal of Chemistry, 2016, 9 (2): 1208-1213.
Sushma, Manjari K, Saroha A K. Performance of various catalysts on treatment of refractory pollutants in industrial wastewater by catalytic wet air oxidation: a review[J ] . Journal of Environmental Management, 2018, 228 : 169-188.
Mikulová J, Baarbier J, Rossignol S, et al. Wet air oxidation of acetic acid over platinum catalysts supported on cerium-based materials: influence of metal and oxide crystallite size[J ] . Journal of Catalysis, 2007, 251 (1): 172-181.
Albin P, Michele B, Gallezo T P. Catalytic wet-air oxidation of kraft bleach plant effluents in a trickle-bed reactor [J ] . Chemie Ingenieur Technik, 2001, 73 (6): 657.
Castillejos-Lopeze, Maaroto-Valiente A, Nevskaia D M, et al. Comparative study of support effects in ruthenium catalysts applied for wet air oxidation of aromatic compounds[J ] . Catalysis Today, 2009, 143 (3/4): 355-363.
Dükkanc M, Gündüz G. Catalytic wet air oxidation of butyric acid and maleic acid solutions over noble metal catalysts prepared on TiO2[J ] . Catalysis Communications, 2009, 10 (6): 913-919.
Erjavec B, Kaplan R, Djivoni P, et al. Catalytic wet air oxidation of bisphenol A model solution in a trickle-bed reactor over titanate nanotube-based catalysts[J ] . Applied Catalysis B: Environmental, 2013, 132/133 : 342-352.
Santos A, Yustos P, Quintanilla A, et al. Influence of pH on the wet oxidation of phenol with copper catalyst [J ] . Topics in Catalysis, 2005, 33 (1/2/3/4): 181-192.
Espinosa M A, Lafaye G, Cervantes A. Catalytic wet air oxidation of phenol over metal catalyst (Ru, Pt) supported on TiO2-CeO2 oxides[J ] . Catalysis Today, 2015, 258 : 564-569.
Gaalova J, Barbier R, Rossignol R. Ruthenium versus platinum on cerium materials in wet air oxidation of acetic acid[J ] . Journal of Hazardous Materials, 2010, 181 (1/2/3): 633-639.
Song A, Lu G. Selective oxidation of methylamine over zirconia supported Pt-Ru, Pt and Ru catalysts[J ] . Chinese Journal of Chemical Engineering, 2015, 23 : 1206-1213.
Yang S X, Feng Y J, Cai W M, et al. C atalytic wet air oxidation of phenol over RuO2/ γ -Al2O3 catalyst[J ] . Rare Metals, 2004, 23 (2): 131-137.
Yang S, Feng Y, Wan J, et al. Effect of CeO2 addition on the structure and activity of RuO2/ γ -Al2O3 catalyst[J ] . Applied Surface Science, 2005, 246 (1/2/3): 222-228.
Wei H Z, Wang Y M, Yu Y, et al. Effect of TiO2 on Ru/ZrO2 catalysts in the catalytic wet air oxidation of isothiazolone[J ] . Catalysis Science & Technology, 2015, 5 : 1693-1703.
Song M, Wang Y, Guo Y, et al. Catalytic wet oxidation of aniline over Ru catalysts supported on a modified TiO2[J ] . Chinese Journal of Catalysis, 2017, 38 (7): 1155-1165.
Garg A, Saha S, Rastogi V, et al. Catalytic wet air oxidation of pulp and paper mill effluent[J ] . Indian Journal of Chemical Technology, 2003, 10 (3): 305-310.
Lee D K, Kim D S, Kim T H, et al. Deactivation of Pt catalysts during wet oxidation of phenol[J ] . Catalysis Today, 2010, 154 (3/4): 244-249.
Iveete C, Guzman S, Julia L, et al. Catalytic ozonation of 4-chlorophenol and 4-phenolsulfonic acid by CeO2 films[J ] . Catalysis Communications, 2019, 133 : 105827.
Ye S, Guo J, Wang Y, et al. Effect of sodium content on the interaction between Ni and support and catalytic performance for syngas methanation over Ni/Zr-Yb-O catalysts[J ] . Chinese Journal of Chemical Engineering, 2019, 27 : 2705-2711.
Pan C J, Tsai M C, Su W N, et al. Tuning/exploiting strong metal-support interaction (SMSI) in heterogeneous catalysis[J ] . Journal of the Taiwan Institute of Chemical Engineers, 2017, 74 : 154-186.
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