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

被引：32
|
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
收藏
页码：4375 / 4381
页数：7
相关论文
共 50 条
  • [1] Oxygen adsorption on silver catalysts during the course of partial oxidation of ethylene
    Ayame, A
    Eimaeda, S
    Feng, L
    Hayasaka, H
    APPLIED CATALYSIS A-GENERAL, 2006, 304 (01) : 93 - 108
  • [2] MECHANISM OF ETHYLENE OXIDATION BY OXYGEN ADDITON TO ETHYLENE OXIDE ON SILVER CATALYSTS
    IMRE, L
    BERICHTE DER BUNSEN-GESELLSCHAFT FUR PHYSIKALISCHE CHEMIE, 1970, 74 (03): : 220 - &
  • [3] REACTIVITY OF OXYGEN SPECIES ADSORBED ON SILVER FOR CO OXIDATION
    KOBAYASHI, M
    TAKEGAMI, H
    KOBAYASHI, H
    JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1977, (02) : 37 - 39
  • [4] FORMATION OF ADSORBED OXYGEN AND ITS REACTIVITY WITH ETHYLENE OVER SILVER CATALYSTS
    KAGAWA, S
    IWAMOTO, M
    MORI, H
    SEIYAMA, T
    JOURNAL OF PHYSICAL CHEMISTRY, 1981, 85 (04): : 434 - 439
  • [5] NATURE AND REACTIVITY OF CARBONACEOUS SPECIES DEPOSITED BY ETHYLENE ON SUPPORTED RUTHENIUM CATALYSTS
    GUPTA, NM
    KAMBLE, VS
    IYER, RM
    JOURNAL OF CATALYSIS, 1984, 88 (02) : 457 - 465
  • [6] Structure and Reactivity of Active Oxygen Species on Silver Surfaces for Ethylene Epoxidation
    Guo, Man
    Dongfang, Nanchen
    Iannuzzi, Marcella
    van Bokhoven, Jeroen Anton
    Artiglia, Luca
    ACS CATALYSIS, 2024, 14 (13): : 10234 - 10244
  • [7] MECHANISM OF ETHYLENE OXIDATION ON SILVER CATALYSTS
    HERZOG, W
    BERICHTE DER BUNSEN-GESELLSCHAFT FUR PHYSIKALISCHE CHEMIE, 1970, 74 (03): : 216 - &
  • [8] Colloidal silver catalysts for oxidation of ethylene
    Shiraishi, Y
    Toshima, N
    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1999, 141 (1-3) : 187 - 192
  • [9] SKELETAL SILVER CATALYSTS FOR THE OXIDATION OF ETHYLENE TO ETHYLENE OXIDE
    CAMBRON, A
    ALEXANDER, WA
    CANADIAN JOURNAL OF CHEMISTRY-REVUE CANADIENNE DE CHIMIE, 1956, 34 (05): : 665 - 671
  • [10] EFFECT OF TRANSPORT PHENOMENA ON THE SELECTIVITY OF SILVER CATALYSTS DURING ETHYLENE OXIDATION
    PAVLOU, S
    STOUKIDES, M
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 1984, 187 (APR): : 33 - COLL
12345