Catalytic reduction of Chlorobenzenes with Pd/Fe nanoparticles: reactive sites, catalyst stability, particle aging, and regeneration

被引：194

作者：

Zhu, Bao-Wei ^{[1
]}

Lim, Teik-Thye ^{[1
]}

机构：

[1] Nanyang Technol Univ, Sch Civil & Environm Engn, Singapore 639798, Singapore

来源：

ENVIRONMENTAL SCIENCE & TECHNOLOGY | 2007年 / 41卷 / 21期

关键词：

D O I：

10.1021/es0712625

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Monochlorobenzene (MCB), dichlorobenzenes (DCBs), and 1,2,4-trichlorobenzene (124TCB) dechlorination experiments in water were carried out with freshly synthesized Pd/Fe particles. The pro- and postreacted Pd/Fe samples were characterized by applying various analytical techniques (XRD, SEM, TEM, and XPS). Chlorinated benzenes could be completely reduced by the Pd/Fe to benzene and the reaction followed the pseudo-first-order kinetics. The reaction rates followed the order TCB < DCBs < MCB, while among the DCBs the order was 1,4-dichlorobenzene >1,3-dichlorobenzene 1,2-dichlorobenzene. Insignificant reactions were observed with the unpalladized iron, suggesting that Pd was the only reactive site in the Pd/Fe particles. The aged Pd/Fe particles exhibited significant decrease in its dechlorination reactivity. The loss of Pd/Fe reactivity could be due to Pd dislodgment from the aged Pd/Fe particles and Pd islets encapsulation by the iron oxides film developed over aging period. Reactivity of the aged Pd/ Fe could be only partially restored after HCI treatment, while regeneration with the NaBH4 reduction method could not restore its activity, although zerovalent state of the iron was reinstated.

引用

页码：7523 / 7529

页数：7

共 31 条

[1] Catalytic hydrodechlorination of 1-chlorooctadecane, 9,10-dichlorostearic acid, and 12,14-dichlorodehydroabietic acid in supercritical carbon dioxide [J].

Aikawa, B ;

Burk, RC ;

Sitholé, BB .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 43 (04) :371-387

[2] Polychlorinated ethane reaction with zero-valent zinc: pathways and rate control [J].

Arnold, WA ;

Ball, WP ;

Roberts, AL .

JOURNAL OF CONTAMINANT HYDROLOGY, 1999, 40 (02) :183-200

[3] The effect of a membrane reactor upon catalyst deactivation during hydrodechlorination of dichloroethane [J].

Chang, CC ;

Reo, CM ;

Lund, CRF .

APPLIED CATALYSIS B-ENVIRONMENTAL, 1999, 20 (04) :309-317

[4] Field assessment of nanoscale biometallic particles for groundwater treatment [J].

Elliott, DW ;

Zhang, WX .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (24) :4922-4926

[5] Dechlorination of p-chlorophenol on a Pd Fe catalyst in a magnetically stabilized fluidized bed;: Implications for sludge and liquid remediation [J].

Graham, LJ ;

Jovanovic, G .

CHEMICAL ENGINEERING SCIENCE, 1999, 54 (15-16) :3085-3093

[6] Reduction of nitrobenzene and formation of corrosion coatings in zerovalent iron systems [J].

Huang, Yong H. ;

Zhang, Tian C. .

WATER RESEARCH, 2006, 40 (16) :3075-3082

[7] Kinetics of halogenated organic compound degradation by iron metal [J].

Johnson, TL ;

Scherer, MM ;

Tratnyek, PG .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1996, 30 (08) :2634-2640

[8] Dechlorination of p-chlorophenol in a microreactor with bimetallic Pd/Fe catalyst [J].

Jovanovic, GN ;

Znidarsic-Plazl, P ;

Sakrittichai, P ;

Al-Khaldi, K .

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2005, 44 (14) :5099-5106

[9] Hydrodehalogenation of haloarenes over Silica supported Pd and Ni - A consideration of catalytic activity/selectivity and haloarene reactivity [J].

Keane, MA .

APPLIED CATALYSIS A-GENERAL, 2004, 271 (1-2) :109-118

[10] The catalytic hydrodechlorination of mono-, di- and trichlorobenzenes over supported nickel [J].

Keane, MA ;

Pina, G ;

Tavoularis, G .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2004, 48 (04) :275-286

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