Carbon dioxide activation by surface excess electrons:: An EPR study of the CO2- radical ion adsorbed on the surface of MgO

被引：31

作者：

Chiesa, Mario

Giamello, Elio

机构：

[1] Univ Turin, Dept Chim IFM, I-10125 Turin, Italy

[2] Univ Turin, NIS Ctr Excellence, I-10125 Turin, Italy

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2007年 / 13卷 / 04期

关键词：

CO2; activation; electron transfer; EPR spectroscopy; MgO surface;

D O I：

10.1002/chem.200600792

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The CO2- radical anion has been generated at the surface of MgO by direct electron transfer from surface trapped excess electrons and characterized by electron paramagnetic resonance spectroscopy. Both C-13 and O-17 hyperfine structures have been resolved for the first time, leading to a detailed mapping of the unpaired electron spin density distribution over the entire radical anion. The magnetic equivalence of the two O nuclei has been ascertained allowing a side-on a sorption structure at low-coordinate Mg2+ ions to be proposed for the surface stabilized radical.

引用

收藏

页码：1261 / 1267

页数：7

相关论文

共 35 条

[1] Application of EPR spectroscopy for elucidation of vanadium speciation in VOx/ZrO2 catalysts subject to redox treatment [J].

Adamski, A ;

Spalek, T ;

Sojka, Z .

RESEARCH ON CHEMICAL INTERMEDIATES, 2003, 29 (7-9) :793-804

[2] Catalysis research of relevance to carbon management: Progress, challenges, and opportunities [J].

Arakawa, H ;

Aresta, M ;

Armor, JN ;

Barteau, MA ;

Beckman, EJ ;

Bell, AT ;

Bercaw, JE ;

Creutz, C ;

Dinjus, E ;

Dixon, DA ;

Domen, K ;

DuBois, DL ;

Eckert, J ;

Fujita, E ;

Gibson, DH ;

Goddard, WA ;

Goodman, DW ;

Keller, J ;

Kubas, GJ ;

Kung, HH ;

Lyons, JE ;

Manzer, LE ;

Marks, TJ ;

Morokuma, K ;

Nicholas, KM ;

Periana, R ;

Que, L ;

Rostrup-Nielson, J ;

Sachtler, WMH ;

Schmidt, LD ;

Sen, A ;

Somorjai, GA ;

Stair, PC ;

Stults, BR ;

Tumas, W .

CHEMICAL REVIEWS, 2001, 101 (04) :953-996

[3] INFRARED-SPECTRA OF FREE-RADICALS PREPARED IN A ROTATING CRYOSTAT - SPECTRA OF CO2-, CCL3 AND CH3CO [J].

BENNETT, JE ;

GRAHAM, SC ;

MILE, B .

SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1973, A 29 (02) :375-383

[4]

CARRINGTON A, 1967, INTRO MAGNETIC RESON, P138

[5] CHARACTERIZATION AND REACTIVITY OF MONONUCLEAR OXYGEN SPECIES ON OXIDE SURFACES [J].

CHE, M ;

TENCH, AJ .

ADVANCES IN CATALYSIS, 1982, 31 :77-133

[6] THE ROLE OF THE O-17 ISOTOPE IN THE CHARACTERIZATION BY ELECTRON-PARAMAGNETIC-RES OF ADSORBED OXYGEN SPECIES ON OXIDE SURFACES [J].

CHE, M ;

GIAMELLO, E ;

TENCH, AJ .

COLLOIDS AND SURFACES, 1985, 13 (2-3) :231-248

[7] Electron traps on oxide surfaces:: (H+)(e-) pairs stabilized on the surface of 17O enriched CaO [J].

Chiesa, M ;

Paganini, MC ;

Giamello, E ;

Di Valentin, C ;

Pacchioni, G .

CHEMPHYSCHEM, 2006, 7 (03) :728-734

[8] Reductive activation of the nitrogen molecule at the surface of "electron-rich" MgO and CaO.: The N2- surface adsorbed radical ion [J].

Chiesa, M ;

Giamello, E ;

Murphy, DM ;

Pacchioni, G ;

Paganini, MC ;

Soave, R ;

Sojka, Z .

JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (02) :497-505

[9] Single electron traps at the surface of polycrystalline MgO: Assignment of the main trapping sites [J].

Chiesa, M ;

Paganini, MC ;

Spoto, G ;

Giamello, E ;

Di Valentin, C ;

Del Vitto, A ;

Pacchioni, G .

JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (15) :7314-7322

[10] Continuous wave electron paramagnetic resonance investigation of the hyperfine structure of 17O2- adsorbed on the MgO surface [J].

Chiesa, M ;

Giamello, E ;

Paganini, MC ;

Sojka, Z ;

Murphy, DM .

JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (10) :4266-4274

← 1 2 3 4 →