Role of Pt atoms on Pd(111) surface in the direct synthesis of hydrogen peroxide: Nano-catalytic experiments and DFT calculations

被引：41

作者：

Quon, Suyeon ^{[1
]}

Jo, Deok Yeon ^{[1
]}

Han, Geun-Ho ^{[1
]}

Han, Sang Soo ^{[2
]}

Seo, Myung-gi ^{[1
]}

Lee, Kwan-Young ^{[1
]}

机构：

[1] Korea Univ, Dept Chem & Biol Engn, 145 Anam Ro, Seoul 02841, South Korea

[2] Korea Inst Sci & Technol, Computat Sci Res Ctr, Hwarangno 14 Gil 5, Seoul 02792, South Korea

来源：

JOURNAL OF CATALYSIS | 2018年 / 368卷

基金：

新加坡国家研究基金会;

关键词：

Hydrogen peroxide; Density functional theory; Morphology-controlled nanoparticle; Nano-catalyst; Bimetallic catalyst; Palladium; Platinum; PD-PT; PREFERENTIAL OXIDATION; SELECTIVE OXIDATION; PALLADIUM; H2O2; H-2; O-2; NANOPARTICLES; OXYGEN; DECOMPOSITION;

D O I：

10.1016/j.jcat.2018.10.007

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Pd-Pt bimetallic catalysts have been studied for improvement of H2O2 selectivity in direct synthesis of H2O2; however, the role of Pt on the Pd surface has not been clearly identified. Herein, we investigated the role of Pt atoms on Pd(1 1 1) facets by realizing the surface in two different ways: nano-synthesis and density functional theory (DFT) calculation model. Pd(1 1 1) were modified into 3 kinds of Pd-Pt alloyed surfaces, a minor Pt-substituted Pd, a major Pt-substituted Pd and a Pt-shell, covering bulk Pd. We successfully embedded Pt atoms in the octahedral Pd surface. Reaction tests showed that the minor Pt-substituted octahedral Pd catalyst had the highest H2O2 selectivity, production rate and the lowest H2O2 decomposition rate. The experimental results were consistent with our DFT calculations which predicted the lowest activation barrier for the O-2 hydrogenation step and the highest one for the H202 dissociation step on the minor Pt-substituted Pd surface. (C) 2018 Elsevier Inc. All rights reserved.

引用

页码：237 / 247

页数：11

共 57 条

[1] Ru-Pt core-shell nanoparticles for preferential oxidation of carbon monoxide in hydrogen [J].

Alayoglu, Selim ;

Nilekar, Anand U. ;

Mavrikakis, Manos ;

Eichhorn, Bryan .

NATURE MATERIALS, 2008, 7 (04) :333-338

[2] New Pd-Pt and Pd-Au catalysts for an efficient synthesis of H2O2 from H2 and O2 under very mild conditions [J].

Bernardotto, Giulia ;

Menegazzo, Federica ;

Pinna, Francesco ;

Signoretto, Michela ;

Cruciani, Giuseppe ;

Strukul, Giorgio .

APPLIED CATALYSIS A-GENERAL, 2009, 358 (02) :129-135

[3]

Blochl P.E., 2005, Handbook of Materials Modeling: Methods., P93

[4] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[5] Synthesis and characterization of Pd nanoparticles by laser ablation in water using nanosecond laser [J].

Boutinguiza, M. ;

Meixus, M. ;

del Val, J. ;

Riveiro, A. ;

Comesana, R. ;

Lusquinos, F. ;

Pou, J. .

LASER ASSISTED NET SHAPE ENGINEERING 9 INTERNATIONAL CONFERENCE ON PHOTONIC TECHNOLOGIES PROCEEDINGS OF THE LANE 2016, 2016, 83 :36-45

[6]

Cavani F., 2009, Sustainable industrial chemistry: Principles, tools and industrial examples

[7] In situ ion exchange synthesis of the novel Ag/AgBr/BiOBr hybrid with highly efficient decontamination of pollutants [J].

Cheng, Hefeng ;

Huang, Baibiao ;

Wang, Peng ;

Wang, Zeyan ;

Lou, Zaizhu ;

Wang, Junpeng ;

Qin, Xiaoyan ;

Zhang, Xiaoyang ;

Dai, Ying .

CHEMICAL COMMUNICATIONS, 2011, 47 (25) :7054-7056

[8] Direct oxidation of H2 to H2O2 and decomposition of H2O2 over oxidized and reduced Pd-containing zeolite catalysts in acidic medium [J].

Choudhary, VR ;

Sansare, SD ;

Gaikwad, AG .

CATALYSIS LETTERS, 2002, 84 (1-2) :81-87

[9] Activation of supported Pd metal catalysts for selective oxidation of hydrogen to hydrogen peroxide [J].

Choudhary, VR ;

Gaikwad, AG ;

Sansare, SD .

CATALYSIS LETTERS, 2002, 83 (3-4) :235-239

[10] Role of chloride or bromide anions and protons for promoting the selective oxidation of H2 by O2 to H2O2 over supported Pd catalysts in an aqueous medium [J].

Choudhary, VR ;

Samanta, C .

JOURNAL OF CATALYSIS, 2006, 238 (01) :28-38

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