New insight into the CO formation mechanism during formic acid oxidation on Pt(111)

被引：33

作者：

Zhong, Wenhui ^{[1
]}

Zhang, Dongju ^{[1
]}

机构：

[1] Shandong Univ, Key Lab Colloid & Interface Chem, Minist Educ, Inst Theoret Chem, Jinan 250100, Peoples R China

来源：

CATALYSIS COMMUNICATIONS | 2012年 / 29卷

基金：

中国国家自然科学基金;

关键词：

Formic acid oxidation; Formic acid dimmer; Pt (111); DFT; GENERALIZED GRADIENT APPROXIMATION; ELECTROCATALYTIC OXIDATION; PLATINUM NANOPARTICLES; INFRARED-SPECTROSCOPY; CARBON-MONOXIDE; METHANOL; ELECTROOXIDATION; ELECTRODES; SURFACES; HCOOH;

D O I：

10.1016/j.catcom.2012.09.002

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：

Density functional theory (DFT) calculations show a new concerted mechanism of formic acid (HCOOH) oxidation on Pt (111), which involves the simultaneous formation of CO2 and CO via the HCOOH dimer in an elementary step. The newly proposed mechanism rationalizes the easy CO poisoning of Pt-based catalysts and improves our understanding for the mechanism of catalytic HCOOH oxidation. (C) 2012 Elsevier B.V. All rights reserved.

引用

收藏

页码：82 / 86

页数：5

相关论文

共 30 条

[1] Mechanisms of methanol decomposition on platinum: A combined experimental and ab initio approach [J].

Cao, D ;

Lu, GQ ;

Wieckowski, A ;

Wasileski, SA ;

Neurock, M .

JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (23) :11622-11633

[2]

CAPON A, 1973, J ELECTROANAL CHEM, V45, P205, DOI 10.1016/0368-1874(73)85076-2

[3] Kinetics and mechanism of the electrooxidation of formic acid - Spectroelectrochemical studies in a flow cell [J].

Chen, YX ;

Heinen, M ;

Jusys, Z ;

Behm, RJ .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (06) :981-985

[4] MECHANISMS OF FORMIC-ACID, METHANOL, AND CARBON-MONOXIDE ELECTROOXIDATION AT PLATINUM AS EXAMINED BY SINGLE POTENTIAL ALTERATION INFRARED-SPECTROSCOPY [J].

CORRIGAN, DS ;

WEAVER, MJ .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1988, 241 (1-2) :143-162

[5] Theoretical Elucidation of the Competitive Electro-oxidation Mechanisms of Formic Acid on Pt(111) [J].

Gao, Wang ;

Keith, John A. ;

Anton, Josef ;

Jacob, Timo .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (51) :18377-18385

[6] Oxidation of formic acid on the Pt(111) surface in the gas phase [J].

Gao, Wang ;

Keith, John A. ;

Anton, Josef ;

Jacob, Timo .

DALTON TRANSACTIONS, 2010, 39 (36) :8450-8456

[7] Modelling electron-induced processes in "condensed" formic acid -: Resonant states of (HCOOH)-2 at low energies [J].

Gianturco, FA ;

Lucchese, RR ;

Langer, J ;

Martin, I ;

Stano, M ;

Karwasz, G ;

Illenberger, E .

EUROPEAN PHYSICAL JOURNAL D, 2005, 35 (02) :417-428

[8] A generalized synchronous transit method for transition state location [J].

Govind, N ;

Petersen, M ;

Fitzgerald, G ;

King-Smith, D ;

Andzelm, J .

COMPUTATIONAL MATERIALS SCIENCE, 2003, 28 (02) :250-258

[9] ORBITAL MIXING IN CO CHEMISORPTION ON TRANSITION-METAL SURFACES [J].

HU, P ;

KING, DA ;

LEE, MH ;

PAYNE, MC .

CHEMICAL PHYSICS LETTERS, 1995, 246 (1-2) :73-78

[10] GRADIENT CORRECTIONS IN DENSITY-FUNCTIONAL THEORY CALCULATIONS FOR SURFACES - CO ON PD(110) [J].

HU, P ;

KING, DA ;

CRAMPIN, S ;

LEE, MH ;

PAYNE, MC .

CHEMICAL PHYSICS LETTERS, 1994, 230 (06) :501-506