Electrocatalytic Water Oxidation at Neutral pH by a Nanostructured Co(PO3)2 Anode

被引:226
作者
Ahn, Hyun S. [1 ,2 ]
Tilley, T. Don [1 ,2 ]
机构
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[2] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA
关键词
catalysis; electrodes; ceramics; nanoparticles; OXYGEN-EVOLVING CATALYST; COLLOIDAL IRIDIUM OXIDE; TERT-BUTYL PHOSPHATE; COBALT OXIDE; DI(TERT-BUTYL)PHOSPHATE COMPLEXES; HETEROGENEOUS CATALYSTS; MULTICOMPONENT OXIDES; MOLECULAR PRECURSORS; MESOPOROUS SILICA; NONPOLAR MEDIA;
D O I
10.1002/adfm.201200920
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Cobalt metaphosphate Co(PO3)2 nanoparticles are prepared via the thermolytic molecular precursor (TMP) method. A Ni form electrode decorated with Co(PO3)2 nanoparticles is evaluated as an anode for water oxidation electrocatalysis in pH 6.4 phosphate-buffered water. Catalytic onset occurs at an overpotential of ca. 310 mV, which is 100 mV lower than that observed for Co3O4 nanoparticles, with a comparable surface area under identical conditions. A per-metal turnover frequency (TOF) of 0.100.21 s-1 is observed at an overpotential, ?, of 440 mV, which is comparable to the highest rate reported for a first-row metal heterogeneous catalyst. Post-catalytic characterization of the catalyst resting state by X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy reveals that surface rearrangement occurs, resulting in an oxide-like surface overlayer.
引用
收藏
页码:227 / 233
页数:7
相关论文
共 85 条
[1]  
[Anonymous], 1992, INORGANIC MAT
[2]  
Bard A.J., 2001, ELECTROCHEMICAL METH, V2th, P103
[3]   THE DETERMINATION OF PORE VOLUME AND AREA DISTRIBUTIONS IN POROUS SUBSTANCES .1. COMPUTATIONS FROM NITROGEN ISOTHERMS [J].
BARRETT, EP ;
JOYNER, LG ;
HALENDA, PP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1951, 73 (01) :373-380
[4]   Half-Sandwich Iridium Complexes for Homogeneous Water-Oxidation Catalysis [J].
Blakemore, James D. ;
Schley, Nathan D. ;
Balcells, David ;
Hull, Jonathan F. ;
Olack, Gerard W. ;
Incarvito, Christopher D. ;
Eisenstein, Odile ;
Brudvig, Gary W. ;
Crabtree, Robert H. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (45) :16017-16029
[5]   The nature of cobalt species in Co and PtCoZSM5 used for the SCR of NOx with CH4 [J].
Boix, A ;
Miró, EE ;
Lombardo, EA ;
Bañares, MA ;
Mariscal, R ;
Fierro, JLG .
JOURNAL OF CATALYSIS, 2003, 217 (01) :186-194
[6]  
Bomben K.D., 1992, HDB XRAY PHOTOELECTR
[7]   Sustained water oxidation photocatalysis by a bioinspired manganese cluster [J].
Brimblecombe, Robin ;
Swiegers, Gerhard F. ;
Dismukes, G. Charles ;
Spiccia, Leone .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (38) :7335-7338
[8]   Adsorption of gases in multimolecular layers [J].
Brunauer, S ;
Emmett, PH ;
Teller, E .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1938, 60 :309-319
[9]   MECHANISMS OF WATER OXIDATION TO OXYGEN - COBALT(IV) AS AN INTERMEDIATE IN THE AQUOCOBALT(II)-CATALYZED REACTION [J].
BRUNSCHWIG, BS ;
CHOU, MH ;
CREUTZ, C ;
GHOSH, P ;
SUTIN, N .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1983, 105 (14) :4832-4833
[10]   LAYERED METAL PHOSPHATES AND PHOSPHONATES - FROM CRYSTALS TO MONOLAYERS [J].
CAO, G ;
HONG, HG ;
MALLOUK, TE .
ACCOUNTS OF CHEMICAL RESEARCH, 1992, 25 (09) :420-427