Nature and Reactivity of Oxygen Species on/in Silver Catalysts during Ethylene Oxidation

被引：33

作者：

Pu, Tiancheng ^{[1
]}

Setiawan, Adhika ^{[2
]}

Lis, Bar Mosevitzky ^{[1
]}

Zhu, Minghui ^{[3
]}

Ford, Michael E. ^{[1
]}

Rangarajan, Srinivas ^{[2
]}

Wachs, Israel E. ^{[1
]}

机构：

[1] Lehigh Univ, Dept Chem & Biomol Engn, Operando Mol Spect & Catalysis Lab, Bethlehem, PA 18015 USA

[2] Lehigh Univ, Dept Chem & Biomol Engn, Computat Catalysis & Mat Design Grp, Bethlehem, PA 18015 USA

[3] East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

来源：

ACS CATALYSIS | 2022年 / 12卷 / 08期

基金：

美国国家科学基金会;

关键词：

ethylene; oxidation; ethylene oxide; silver; NAP-XPS; in situ Raman; TPSR; DFT; IN-SITU RAMAN; SURFACE; EPOXIDATION; AG(110); XPS;

D O I：

10.1021/acscatal.1c05939

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：

The nature of surface oxygen species on/in a silver powder catalystand their reactivity with ethylene were systematically investigated with multiplespectroscopies and DFT calculations. Unique quasiin situHS-LEIS,in situNAP-XPS, andin situRaman spectroscopy demonstrated that the silver surface iscovered by a thin oxide layer (1-3 nm) after an oxidation treatment and duringethylene oxidation. Periodic DFT models allowed assignments of oxygen speciesdetected byin situRaman spectroscopy with detailed structures on p(4x4)-O-Ag(111) surfaces.In situNAP-XPS and Raman spectroscopy suggest that Ag4-O2on oxidized Ag is the active oxygen species for ethylene epoxidation. Theexperimental and theoretical methodologies developed in the present work serve asan efficient toolbox for the scientific investigation of the silver-oxygen system forselective oxidation reactions and rational guidance of computational calculationscoupled with experimentalfindings.

引用

页码：4375 / 4381

页数：7

共 50 条

[41] Taming Nitrene Reactivity with Silver Catalysts
Vine, Logan E.
Zerull, Emily E.
Schomaker, Jennifer M.
SYNLETT, 2021, 32 (01) : 30 - 44
[42] Interaction of oxygen adsorbed on silver film with hydrogen and ethylene
Khasin, AV
Nechaev, SV
REACTION KINETICS AND CATALYSIS LETTERS, 1996, 58 (01): : 125 - 132
[43] Ethylene epoxidation over supported silver catalysts - influence of catalyst pretreatment on conversion and selectivity
Aho, Atte
Eranen, Kari
Lemus-Yegres, Lived J.
Voss, Bodil
Gabrielsson, Anders
Salmi, Tapio
Murzin, Dmitry Yu
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY, 2018, 93 (06) : 1549 - 1557
[44] A possible role for surface carbon during ethylene epoxidation over silver catalysts
Bradford, MCJ
Fuentes, DX
CATALYSIS COMMUNICATIONS, 2002, 3 (02) : 51 - 60
[45] ON THE NATURE OF THE ACTIVE STATE OF SILVER DURING CATALYTIC-OXIDATION OF METHANOL
BAO, X
MUHLER, M
PETTINGER, B
SCHLOGL, R
ERTL, G
CATALYSIS LETTERS, 1993, 22 (03) : 215 - 225
[46] Ethylene oxidation on unpromoted silver catalysts: Reaction pathway and selectivity analysis using DFT calculations
Wu, Siyuan
Tatarchuk, Bruce J.
Adamczyk, Andrew J.
SURFACE SCIENCE, 2021, 708
[47] TRANSIENT-RESPONSE AND INFRARED STUDIES OF ETHYLENE-OXIDE REACTIONS ON SILVER CATALYSTS AND SUPPORTS
BULUSHEV, DA
PAUKSHTIS, EA
NOGIN, YN
BALZHINIMAEV, BS
APPLIED CATALYSIS A-GENERAL, 1995, 123 (02) : 301 - 322
[48] Reaction of ethylene with oxygen adsorbed on a silver film. Dependence of the selectivity to ethylene oxide on the ethylene pressure
Khasin, AV
REACTION KINETICS AND CATALYSIS LETTERS, 1998, 64 (02): : 289 - 294
[49] Kinetic behavior of ethylene oxidation on silver
Goncharova, S.N.
Khasin, A.V.
Filimonova, S.N.
Bulushev, D.A.
Kinetics and Catalysis, 1992, 32 (4 pt 1) : 768 - 774
[50] Reaction of ethylene with oxygen adsorbed on a silver film. Dependence of the selectivity to ethylene oxide on the ethylene pressure
A. V. Khasin
Reaction Kinetics and Catalysis Letters, 1998, 64 : 289 - 294

← 1 2 3 4 5 →