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[1]王子丹,Hameed Sohaib,张诺伟*,等.PdNi/C低温高效催化湿式氧化无害化处理氨氮废水[J].厦门大学学报(自然科学版),2018,57(01):32-37.[doi:10.6043/j.issn.0438-0479.201703025]
 WANG Zidan,HAMEED Sohaib,ZHANG Nuowei*,et al.Efficient Harmless-degrading of Ammonia by Catalytic Wet Air Oxidation with PdNi/C Catalyst Under Mild Conditions[J].Journal of Xiamen University(Natural Science),2018,57(01):32-37.[doi:10.6043/j.issn.0438-0479.201703025]
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《厦门大学学报(自然科学版)》[ISSN:0438-0479/CN:35-1070/N]

卷:
57卷
期数:
2018年01期
页码:
32-37
栏目:
研究论文
出版日期:
2018-01-26

文章信息/Info

Title:
Efficient Harmless-degrading of Ammonia by Catalytic Wet Air Oxidation with PdNi/C Catalyst Under Mild Conditions
文章编号:
0438-0479(2018)01-0032-06
作者:
王子丹Hameed Sohaib张诺伟*陈秉辉
厦门大学 化学化工学院,醇醚酯化工清洁生产国家工程实验室,福建 厦门 361005
Author(s):
WANG ZidanHAMEED SohaibZHANG Nuowei*CHEN Binghui
National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China
关键词:
催化湿式氧化 PdNi/C 氨氮废水
Keywords:
catalytic wet air oxidation(CWAO) PdNi/C ammonia nitrogen wastewater
分类号:
TQ 032
DOI:
10.6043/j.issn.0438-0479.201703025
文献标志码:
A
摘要:
氨氮废水对环境的危害日益严重,催化湿式氧化技术能高效无害化处理氨氮废水,但现有催化剂工作条件苛刻.采用化学还原法制备2%Pd1%Ni/C双金属催化剂,并考察了其氨氮废水催化湿式氧化性能.结果表明:Pd和Ni的结合使得PdNi/C催化剂在更低贵金属用量的前提下,比相对应的单贵金属催化剂(Pd/C)具有更优的催化性能,尤其是低温催化性能.在每千克催化剂每小时处理约33 L模拟废水(氨氮的质量浓度为1 000 mg/L,pH=12)及反应压强为2 MPa处理3 h的条件下:在140 ℃时,2%Pd1%Ni/C催化剂能催化氧化脱除废水中99.0%的氨氮,且N2选择性为90.5%; 而3%Pd/C 和3%Ni/C催化剂的氨氮转化率仅分别为86.4%和50.6%; 即使在120 ℃的温和条件下,采用2%Pd1%Ni/C催化剂也能脱除80%以上的氨氮.采用X射线衍射(XRD)、X射线光电子能谱(XPS)、CO程序升温还原(CO-TPR)对PdNi/C催化剂进行表征,结果表明Pd和Ni之间的协同作用调变了催化剂的亲氧性能,进而提高了氨氮转化率.
Abstract:
The pollution of wastewater containing ammonia becomes more and more serious.Ammonia can be efficiently removed by catalytic wet air oxidation(CWAO)technology.However,most of CWAO processes are operated at high pressures and temperatures,because the applied catalysts exhibited poor catalytic prefromance under mild conditions.In this study,PdNi/C bimetallic catalyst was prepared via a chemical reduction method and investigated for CWAO of ammonia to N2.It is found that the combining of Pd and Ni enables PdNi/C bimetallic catalyst to possess higher catalytic performance,especially at low temperatures,although it contains a lower Pd loading,compared with Pd/C.At 140 ℃,almost 100% ammonia can be removed by 2%Pd1%Ni/C bimetallic catalyst,while only 86.4% and 50.6% can be removed respectively with 3%Pd/C and 3%Ni/C,under the capacity around 33 L wastewater(ρ</sup>0</sub>NH</sub></sub>3=1 000 mg/L,pH=12)per kilo catalyst per hour with the pressure of 2 MPa conduct for 3 h.Even at 120 ℃,more than 80% ammonia can be removed using 2%Pd 1%Ni/C.Moreover,the selectivity to N2 for 2%Pd1%Ni/C is higher than 90%.The characterization results of X-ray diffraction(XRD),CO temperature programmed reduction(CO-TPR)and X-ray photo-electron spectroscopy(XPS)indicate that the synergy between Pd and Ni modifies the redox properties and thus promotes the catalytic performance.

参考文献/References:

[1] 吴悦颖,文宇立,刘伟江.“十二五”氨氮总量怎么减? [J].环境经济,2013(3):39-41.
[2] 付迎春,钱仁渊,金鸣林.催化湿式氧化法处理氨氮废水的研究 [J].煤炭转化,2004(2):72-75.
[3] KAEWPUANG-NGAM S,INAZU K,KOBAYASHI T,et al.Selective wet-air oxidation of diluted aqueous ammonia solutions over supported Ni catalysts [J].Water Research,2004,38(3):778-782.
[4] IMAMURA S,DOI A,ISHIDA S.Wet oxidation of ammonia catalyzed by cerium-based composite oxides [J].Industrial & Engineering Chemistry Product Research and Development,1985,24(1):75-80.
[5] QIN J Y,AIKA K.Catalytic wet air oxidation of ammonia over alumina supported metals [J].Applied Catalysis B:Environmental,1998,16(3):261-268.
[6] BARBIER J,JR,OLIVIERO L,RENARD B,et al.Catalytic wet air oxidation of ammonia over M/CeO2 ca-talysts in the treatment of nitrogen-containing pollutants [J].Catalysis Today,2002,75(1/2/3/4):29-34.
[7] CAO S L,CHEN G H,HU X J,et al.Catalytic wet air oxidation of wastewater containing ammonia and phenol over activated carbon supported Pt catalysts [J].Catalysis Today,2003,88(1/2):37-47.
[8] TAKAYAMA H,QIN J Y,INAZU K,et al.Hydrogen-treated active carbon supported palladium catalysts for wet air oxidation of ammonia [J].Chemistry Letters,1999,28(5):377-378.
[9] LEE D K,CHO J S,YOON W L.Catalytic wet oxidation of ammonia:why is N2 formed preferentially against NO3-? [J].Chemosphere,2005,61(4):573-578.
[10] LOUSTEAU C,BESSON M,DESCORME C.Catalytic wet air oxidation of ammonia over supported noble metals [J].Catalysis Today,2015,241:80-85.
[11] FU J L,YANG K X,MA C J,et al.Bimetallic Ru-Cu as a highly active,selective and stable catalyst for catalytic wet oxidation of aqueous ammonia to nitrogen [J].Applied Catalysis B:Environmental,2016,184:216-222.
[12] LIU Z,ZHANG X,HONG L.Physical and electrochemical characterizations of nanostructured Pd/C and PdNi/C catalysts for methanol oxidation [J].Electrochemistry Communications,2009,11(4):925-928.
[13] HOLADE Y,MORAIS C,ARRII-CLACENS S,et al.New preparation of PdNi/C and PdAg/C nanocatalysts for glycerol electrooxidation in alkaline medium[J].Electrocatalysis,2013,4(3):167-178.
[14] SHEN S Y,ZHAO T S,XU J B,et al.Synthesis of PdNi catalysts for the oxidation of ethanol in alkaline direct ethanol fuel cells [J].Journal of Power Sources,2010,195(4):1001-1006.
[15] JIN C C,SUN X J,CHEN Z D,et al.Electrocatalytic activity of PdNi/C catalysts for allyl alcohol oxidation in alkaline solution [J].Materials Chemistry and Physics,2012,135(2/3):433-437.
[16] 高艳伟,邓超,邬冰,等.PdNi/C催化剂的制备及对甲酸的电催化氧化 [J].化学工程师,2010,24(5):1-3.
[17] 沈阳市环境监测中心站.水质 氨氮的测定 纳氏试剂分光光度法:HJ 535—2009 [S].北京:中国环境科学出版社,2009.
[18] ZHU H Q,QIN Z F,SHAN W J,et al.Pd/CeO2-TiO2 catalyst for CO oxidation at low temperature:a TPR study with H2 and CO as reducing agents [J].Journal of Catalysis,2004,225(2):267-277.
[19] LEE D K.Mechanism and kinetics of the catalytic oxidation of aqueous ammonia to molecular nitrogen [J].Environmental Science and Technology,2003,37(24):5745-5749.
[20] WANG Z,HAMEED S,WEN Y,et al.The effect of weak acid anions on the selective catalytic wet air oxidation of aqueous ammonia to nitrogen [J].Scientific Reports,2017,7(1):3911.[1] 吴悦颖,文宇立,刘伟江.“十二五”氨氮总量怎么减? [J].环境经济,2013(3):39-41.
[2] 付迎春,钱仁渊,金鸣林.催化湿式氧化法处理氨氮废水的研究 [J].煤炭转化,2004(2):72-75.
[3] KAEWPUANG-NGAM S,INAZU K,KOBAYASHI T,et al.Selective wet-air oxidation of diluted aqueous ammonia solutions over supported Ni catalysts [J].Water Research,2004,38(3):778-782.
[4] IMAMURA S,DOI A,ISHIDA S.Wet oxidation of ammonia catalyzed by cerium-based composite oxides [J].Industrial & Engineering Chemistry Product Research and Development,1985,24(1):75-80.
[5] QIN J Y,AIKA K.Catalytic wet air oxidation of ammonia over alumina supported metals [J].Applied Catalysis B:Environmental,1998,16(3):261-268.
[6] BARBIER J,JR,OLIVIERO L,RENARD B,et al.Catalytic wet air oxidation of ammonia over M/CeO2 ca-talysts in the treatment of nitrogen-containing pollutants [J].Catalysis Today,2002,75(1/2/3/4):29-34.
[7] CAO S L,CHEN G H,HU X J,et al.Catalytic wet air oxidation of wastewater containing ammonia and phenol over activated carbon supported Pt catalysts [J].Catalysis Today,2003,88(1/2):37-47.
[8] TAKAYAMA H,QIN J Y,INAZU K,et al.Hydrogen-treated active carbon supported palladium catalysts for wet air oxidation of ammonia [J].Chemistry Letters,1999,28(5):377-378.
[9] LEE D K,CHO J S,YOON W L.Catalytic wet oxidation of ammonia:why is N2 formed preferentially against NO3-? [J].Chemosphere,2005,61(4):573-578.
[10] LOUSTEAU C,BESSON M,DESCORME C.Catalytic wet air oxidation of ammonia over supported noble metals [J].Catalysis Today,2015,241:80-85.
[11] FU J L,YANG K X,MA C J,et al.Bimetallic Ru-Cu as a highly active,selective and stable catalyst for catalytic wet oxidation of aqueous ammonia to nitrogen [J].Applied Catalysis B:Environmental,2016,184:216-222.
[12] LIU Z,ZHANG X,HONG L.Physical and electrochemical characterizations of nanostructured Pd/C and PdNi/C catalysts for methanol oxidation [J].Electrochemistry Communications,2009,11(4):925-928.
[13] HOLADE Y,MORAIS C,ARRII-CLACENS S,et al.New preparation of PdNi/C and PdAg/C nanocatalysts for glycerol electrooxidation in alkaline medium[J].Electrocatalysis,2013,4(3):167-178.
[14] SHEN S Y,ZHAO T S,XU J B,et al.Synthesis of PdNi catalysts for the oxidation of ethanol in alkaline direct ethanol fuel cells [J].Journal of Power Sources,2010,195(4):1001-1006.
[15] JIN C C,SUN X J,CHEN Z D,et al.Electrocatalytic activity of PdNi/C catalysts for allyl alcohol oxidation in alkaline solution [J].Materials Chemistry and Physics,2012,135(2/3):433-437.
[16] 高艳伟,邓超,邬冰,等.PdNi/C催化剂的制备及对甲酸的电催化氧化 [J].化学工程师,2010,24(5):1-3.
[17] 沈阳市环境监测中心站.水质 氨氮的测定 纳氏试剂分光光度法:HJ 535—2009 [S].北京:中国环境科学出版社,2009.
[18] ZHU H Q,QIN Z F,SHAN W J,et al.Pd/CeO2-TiO2 catalyst for CO oxidation at low temperature:a TPR study with H2 and CO as reducing agents [J].Journal of Catalysis,2004,225(2):267-277.
[19] LEE D K.Mechanism and kinetics of the catalytic oxidation of aqueous ammonia to molecular nitrogen [J].Environmental Science and Technology,2003,37(24):5745-5749.
[20] WANG Z,HAMEED S,WEN Y,et al.The effect of weak acid anions on the selective catalytic wet air oxidation of aqueous ammonia to nitrogen [J].Scientific Reports,2017,7(1):3911.

备注/Memo

备注/Memo:
收稿日期:2017-03-15 录用日期:2017-06-20
基金项目:国家科技支撑计划(2014BAC10B01); 福建省自然科学基金(2015J05031)
*通信作者:zhnw@xmu.edu.cn
更新日期/Last Update: 1900-01-01