Pd基双金属催化剂对2,4-D的液相催化加氢脱氯

周鑫; 罗豪鹏; 王唯; 陈泉源; 周娟

PDF(708 KB)

中国环境科学 ›› 2019, Vol. 39 ›› Issue (10) : 4337-4342.

环境生态

Pd基双金属催化剂对2,4-D的液相催化加氢脱氯

周鑫, 罗豪鹏, 王唯, 陈泉源, 周娟

作者信息 +

Liquid phase catalytic hydrodechlorination of 2, 4-dichlorophenoxyacetic acid over Pd-M(M=Fe, Co, Cu) bimetallic catalysts

ZHOU Xin, LUO Hao-peng, WANG Wei, CHEN Quan-yuan, ZHOU Juan

Author information +

文章历史 +

摘要

以CeO₂为载体，采用浸渍法分别合成了负载型Pd基催化剂（Pd/CeO₂，Pd-Fe/CeO₂，Pd-Co/CeO₂和Pd-Cu/CeO₂），并用于水中2，4-二氯苯氧乙酸的催化加氢脱氯.使用等离子体发射光谱仪、扫描电子显微镜和X-射线光电子能谱仪和CO化学吸附对材料进行表征.结果表明，CeO₂作为载体可有效分散金属颗粒，双金属间的协同作用改善了其催化性能.其中Pd-Fe双金属催化剂具有相对优异的催化效果，随着Fe负载量的增加，Pd-Fe/CeO₂的催化活性先升后降.2，4-二氯苯氧乙酸的催化脱氯以同步脱氯和逐步脱氯2种方式同时进行.

Abstract

Supported bimetallic catalysts Pd-M/CeO₂(M=Fe, Co, Cu) were prepared by the impregnation method and the liquid phase catalytic hydrodechlorination (HDC) of 2,4-dichlorophenoxyacetic acid (2,4-D) was investigated over these catalysts. The catalysts were characterized by inductive coupled plasma optical emission, scanning electron microscope, X-ray photoelectron spectrometer and CO chemisorption. The results showed that cerium oxide could effectively disperse metal particles, and the synergy between metals improved catalytic performance. The Pd-Fe bimetallic catalyst has a relatively excellent catalytic effect. The catalytic activity of Pd-Fe/CeO₂ increased first and then decreased with the increase of Fe loading. In addition, the dechlorination of 2,4-D were proceeded via both the stepwise and concerted pathways.

导出引用

周鑫, 罗豪鹏, 王唯, 陈泉源, 周娟. Pd基双金属催化剂对2,4-D的液相催化加氢脱氯[J]. 中国环境科学. 2019, 39(10): 4337-4342

ZHOU Xin, LUO Hao-peng, WANG Wei, CHEN Quan-yuan, ZHOU Juan. Liquid phase catalytic hydrodechlorination of 2, 4-dichlorophenoxyacetic acid over Pd-M(M=Fe, Co, Cu) bimetallic catalysts[J]. China Environmental Science. 2019, 39(10): 4337-4342

中图分类号： X505

参考文献

[1] Jaafarzadeh N, Ghanbari F, Ahmadi M. Catalytic degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) by nano-Fe₂O₃ activated peroxymonosulfate:Influential factors and mechanism determination[J]. Chemosphere, 2017,169:568-576.
[2] Garabrant D H, Philbert M A. Review of 2,4-dichlorophenoxyacetic acid (2,4-D) epidemiology and toxicology[J]. Critical reviews in toxicology, 2002,32(4):233-257.
[3] Cao L, Zhou Z, Niu S, et al. Positive-Charge Functionalized Mesoporous Silica Nanoparticles as Nanocarriers for Controlled 2,4-Dichlorophenoxy Acetic Acid Sodium Salt Release[J]. Journal of agricultural and food chemistry, 2018,66(26):6594-6603.
[4] Lemus M A, López T, Recillas S, et al. Photocatalytic degradation of 2,4-dichlorophenoxyacetic acid using nanocrystalline cryptomelane composite catalysts[J]. Journal of Molecular Catalysis A:Chemical, 2008,281(1/2):107-112.
[5] Seck E I, Doña-Rodríguez J M, Fernández-Rodríguez C, et al. Photocatalytic removal of 2,4-dichlorophenoxyacetic acid by using sol-gel synthesized nanocrystalline and commercial TiO₂:Operational parameters optimization and toxicity studies[J]. Applied Catalysis B:Environmental, 2012,125:28-34.
[6] Cai J, Zhou M, Yang W, et al. Degradation and mechanism of 2,4-dichlorophenoxyacetic acid (2,4-D) by thermally activated persulfate oxidation[J]. Chemosphere, 2018,212:784-793.
[7] Hameed B H, Salman J M, Ahmad A L. Adsorption isotherm and kinetic modeling of 2,4-D pesticide on activated carbon derived from date stones[J]. Journal of hazardous materials, 2009,163(1):121-126.
[8] Chenchana A, Nemamcha A, Moumeni H, et al. Photodegradation of 2,4-dichlorophenoxyacetic acid over TiO₂(B)/anatase nanobelts and Au-TiO₂(B)/anatase nanobelts[J]. Applied Surface Science, 2019, 467-468:1076-1087.
[9] Zhou H, Zhao Y, Xiang J, et al. Enhanced dechlorination of 2,4-dichlorophenoxyacetic acid by Pd/Fe nanoparticles in the presence of environment-friendly iminodisuccinic acid[J]. Applied Organometallic Chemistry, 2018,32(12):e4598.
[10] Zhou H Y, Xiang J C, Zhao Y K, et al. Improvements of Pd/Fe nanoparticles by ethylenediamine disuccinic acid for 2,4-D dechlorination[J]. Separation and Purification Technology, 2018, 207:377-386.
[11] Zhou J, Han Y X, Wang W J, et al. Reductive removal of chloroacetic acids by catalytic hydrodechlorination over Pd/ZrO₂ catalysts[J]. Applied Catalysis B:Environmental, 2013,134-135:222-230.
[12] 周娟,陈欢,李晓璐,等.Pd/CeO₂催化水中溴酸盐的加氢还原研究[J]. 中国环境科学, 2011,31(8):1274-1279. Zhou J, Chen H, Li X L, et al. Study on liquid phase catalytic hydrogenation of bromate over Pd/CeO₂ catalyst[J]. China Environmental Science, 2011,31(8):1274-1279.
[13] 李燕妮,陈泉源,周娟,等.石墨烯杂氮载Pd催化剂对2, 4-二氯酚的液相催化加氢脱氯[J]. 中国环境科学, 2017,37(2):577-583. Li Y N, Chen Q Y, Zhou J, et al. The liquid phase catalytic hydrogenation of 2,4-dichlorophenol over Pd catalyst supported on nitrogen-doped graphene[J]. China Environmental Science, 2017, 37(2):577-583.
[14] Wei Q, Ma Q, Zuo P, et al. Hollow structure and electron promotion effect of mesoporous Pd/CeO₂ catalyst for enhanced catalytic hydrogenation[J]. ChemCatChem, 2018,10(5):1019-1026.
[15] Sun J, Zhang J, Fu H, et al. Enhanced catalytic hydrogenation reduction of bromate on Pd catalyst supported on CeO₂ modified SBA-15prepared by strong electrostatic adsorption[J]. Applied Catalysis B:Environmental, 2018,229:32-40.
[16] Saikia H, Borah B J, Bharali P. Room Temperature Reduction of Nitroaromatics Using Pd Nanoparticles Stabilized on Nano-CeO₂[J]. ChemistrySelect, 2017,2(32):10524-10530.
[17] Liu X, Wang D, Li Y. Synthesis and catalytic properties of bimetallic nanomaterials with various architectures[J]. Nano Today, 2012, 7(5):448-466.
[18] Singh A K, Xu Q. Synergistic Catalysis over Bimetallic Alloy Nanoparticles[J]. Chem. Cat. Chem., 2013,5(3):652-676.
[19] Resende K A, Teles C A, Jacobs G, et al. Hydrodeoxygenation of phenol over zirconia supported Pd bimetallic catalysts. The effect of second metal on catalyst performance[J]. Applied Catalysis B:Environmental, 2018,232:213-231.
[20] Li X, Wang X, Liu M, et al. Construction of Pd-M (M=Ni, Ag, Cu) alloy surfaces for catalytic applications[J]. Nano Research, 2018,11(2):780-790.
[21] Zhou J, Chen H, Chen Q, et al. Bimetallic Au-decorated Pd catalyst for the liquid phase hydrodechlorination of 2,4-dichlorophenol[J]. Applied Surface Science, 2016,387:588-594.
[22] Gómez-Sainero L M, Seoane X L, Fierro J LG, et al. Liquid-Phase Hydrodechlorination of CCl₄ to CHCl₃ on Pd/Carbon Catalysts:Nature and Role of Pd Active Species[J]. Journal of Catalysis, 2002, 209(2):279-288.
[23] Baeza J A, Calvo L, Gilarranz M A, et al. Catalytic behavior of size-controlled palladium nanoparticles in the hydrodechlorination of 4-chlorophenol in aqueous phase[J]. Journal of Catalysis, 2012, 293:85-93.