Preparation of mono- or zerovalent nickel by single or successive one-electron-transfer steps in the photoreduction of silica-supported nickel catalysts
Ni/SiO/sub 2/ supported catalysts prepared by competitive cation exchange can be reduced by UV irradiation in hydrogen at 77 K to lead by a one-electron process to Ni/sup +/ species. These Ni/sup +/ ions which exhibit an EPR signal at g/sub 1/ = 2.68, g/sub 2/ = 2.32, and g/sub 3/ = 2.007 and a band...
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| Veröffentlicht in: | J. Phys. Chem.; (United States) 1987-11, Vol.91 (23), p.5912-5921 |
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| container_title | J. Phys. Chem.; (United States) |
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| creator | Bonneviot, L Cai, F. X Che, M Kermarec, M Legendre, O Lepetit, C Olivier, D |
| description | Ni/SiO/sub 2/ supported catalysts prepared by competitive cation exchange can be reduced by UV irradiation in hydrogen at 77 K to lead by a one-electron process to Ni/sup +/ species. These Ni/sup +/ ions which exhibit an EPR signal at g/sub 1/ = 2.68, g/sub 2/ = 2.32, and g/sub 3/ = 2.007 and a band at 838 nm in the UV-vis and near-IR reflectance spectra bind molecular hydrogen to form (similarly ordered Ni(H/sub 2/))/sup +/ pseudotetrahedral surface complexes. The photoreduction process in carbon monoxide occurs appreciably only at 25/sup 0/C and depends on the CO pressure. It is a one-electron-reduction process, and (Ni(CO)/sub n/)/sup +/ species (n = 2-4) are observed by EPR and IR for pressures above 10 Torr. For lower pressures, the formation of metal is observed by IR and ferromagnetic resonance via the reduction by two consecutive one-electron-transfer steps. The first step proceeds from the photoproduction of (Ni/sup +/-O/sup -/)* excited states. The second step is due to the release of electrons from a reservoir which has been tentatively identified to pseudo-carbonates characterized by IR bands at 1750-1850 cm/sup -1/ and by TPD peaks of CO at 803 K and of CO/sub 2/ at 513 and 803 K. The formation of the latter species is the result of the quenching of the excited state by CO molecules which react with the O/sup -/ activated surface oxygens to lead to CO/sub 2//sup -/ which with O/sup 2 -/ ions generates CO/sub 3//sup 3 -/ radical ions. |
| doi_str_mv | 10.1021/j100307a020 |
| format | Article |
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X ; Che, M ; Kermarec, M ; Legendre, O ; Lepetit, C ; Olivier, D</creator><creatorcontrib>Bonneviot, L ; Cai, F. X ; Che, M ; Kermarec, M ; Legendre, O ; Lepetit, C ; Olivier, D ; Universite P. et M. Curie, Paris, France</creatorcontrib><description>Ni/SiO/sub 2/ supported catalysts prepared by competitive cation exchange can be reduced by UV irradiation in hydrogen at 77 K to lead by a one-electron process to Ni/sup +/ species. These Ni/sup +/ ions which exhibit an EPR signal at g/sub 1/ = 2.68, g/sub 2/ = 2.32, and g/sub 3/ = 2.007 and a band at 838 nm in the UV-vis and near-IR reflectance spectra bind molecular hydrogen to form (similarly ordered Ni(H/sub 2/))/sup +/ pseudotetrahedral surface complexes. The photoreduction process in carbon monoxide occurs appreciably only at 25/sup 0/C and depends on the CO pressure. It is a one-electron-reduction process, and (Ni(CO)/sub n/)/sup +/ species (n = 2-4) are observed by EPR and IR for pressures above 10 Torr. For lower pressures, the formation of metal is observed by IR and ferromagnetic resonance via the reduction by two consecutive one-electron-transfer steps. The first step proceeds from the photoproduction of (Ni/sup +/-O/sup -/)* excited states. The second step is due to the release of electrons from a reservoir which has been tentatively identified to pseudo-carbonates characterized by IR bands at 1750-1850 cm/sup -1/ and by TPD peaks of CO at 803 K and of CO/sub 2/ at 513 and 803 K. The formation of the latter species is the result of the quenching of the excited state by CO molecules which react with the O/sup -/ activated surface oxygens to lead to CO/sub 2//sup -/ which with O/sup 2 -/ ions generates CO/sub 3//sup 3 -/ radical ions.</description><identifier>ISSN: 0022-3654</identifier><identifier>EISSN: 1541-5740</identifier><identifier>DOI: 10.1021/j100307a020</identifier><identifier>CODEN: JPCHAX</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>400500 - Photochemistry ; CARBON COMPOUNDS ; CARBON MONOXIDE ; CARBON OXIDES ; Catalysis ; CATALYST SUPPORTS ; CATALYSTS ; Catalysts: preparations and properties ; Catalytic reactions ; CHALCOGENIDES ; CHEMICAL PREPARATION ; CHEMICAL REACTIONS ; Chemistry ; DATA ; ELECTRON SPIN RESONANCE ; ELECTRON TRANSFER ; ELEMENTS ; ENERGY LEVELS ; Exact sciences and technology ; EXCITED STATES ; EXPERIMENTAL DATA ; General and physical chemistry ; General. Nomenclature, chemical documentation, computer chemistry ; HYDROGEN ; INFORMATION ; INFRARED SPECTRA ; INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY ; LOW TEMPERATURE ; MAGNETIC RESONANCE ; METALS ; MINERALS ; NICKEL ; NONMETALS ; NUMERICAL DATA ; OXIDE MINERALS ; OXIDES ; OXYGEN COMPOUNDS ; PHOTOCHEMICAL REACTIONS ; REDUCTION ; RESONANCE ; SILICA ; SILICON COMPOUNDS ; SILICON OXIDES ; SPECTRA ; SYNTHESIS ; Theory of reactions, general kinetics ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry ; TRANSITION ELEMENTS</subject><ispartof>J. Phys. Chem.; (United States), 1987-11, Vol.91 (23), p.5912-5921</ispartof><rights>1988 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a374t-38a326e4ac75cd41ae0826e96d83ed5e96ce9493e4a5f0d7a7deba64f7f47e5d3</citedby></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/j100307a020$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/j100307a020$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=7668661$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/5851938$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Bonneviot, L</creatorcontrib><creatorcontrib>Cai, F. X</creatorcontrib><creatorcontrib>Che, M</creatorcontrib><creatorcontrib>Kermarec, M</creatorcontrib><creatorcontrib>Legendre, O</creatorcontrib><creatorcontrib>Lepetit, C</creatorcontrib><creatorcontrib>Olivier, D</creatorcontrib><creatorcontrib>Universite P. et M. Curie, Paris, France</creatorcontrib><title>Preparation of mono- or zerovalent nickel by single or successive one-electron-transfer steps in the photoreduction of silica-supported nickel catalysts</title><title>J. Phys. Chem.; (United States)</title><addtitle>J. Phys. Chem</addtitle><description>Ni/SiO/sub 2/ supported catalysts prepared by competitive cation exchange can be reduced by UV irradiation in hydrogen at 77 K to lead by a one-electron process to Ni/sup +/ species. These Ni/sup +/ ions which exhibit an EPR signal at g/sub 1/ = 2.68, g/sub 2/ = 2.32, and g/sub 3/ = 2.007 and a band at 838 nm in the UV-vis and near-IR reflectance spectra bind molecular hydrogen to form (similarly ordered Ni(H/sub 2/))/sup +/ pseudotetrahedral surface complexes. The photoreduction process in carbon monoxide occurs appreciably only at 25/sup 0/C and depends on the CO pressure. It is a one-electron-reduction process, and (Ni(CO)/sub n/)/sup +/ species (n = 2-4) are observed by EPR and IR for pressures above 10 Torr. For lower pressures, the formation of metal is observed by IR and ferromagnetic resonance via the reduction by two consecutive one-electron-transfer steps. The first step proceeds from the photoproduction of (Ni/sup +/-O/sup -/)* excited states. The second step is due to the release of electrons from a reservoir which has been tentatively identified to pseudo-carbonates characterized by IR bands at 1750-1850 cm/sup -1/ and by TPD peaks of CO at 803 K and of CO/sub 2/ at 513 and 803 K. The formation of the latter species is the result of the quenching of the excited state by CO molecules which react with the O/sup -/ activated surface oxygens to lead to CO/sub 2//sup -/ which with O/sup 2 -/ ions generates CO/sub 3//sup 3 -/ radical ions.</description><subject>400500 - Photochemistry</subject><subject>CARBON COMPOUNDS</subject><subject>CARBON MONOXIDE</subject><subject>CARBON OXIDES</subject><subject>Catalysis</subject><subject>CATALYST SUPPORTS</subject><subject>CATALYSTS</subject><subject>Catalysts: preparations and properties</subject><subject>Catalytic reactions</subject><subject>CHALCOGENIDES</subject><subject>CHEMICAL PREPARATION</subject><subject>CHEMICAL REACTIONS</subject><subject>Chemistry</subject><subject>DATA</subject><subject>ELECTRON SPIN RESONANCE</subject><subject>ELECTRON TRANSFER</subject><subject>ELEMENTS</subject><subject>ENERGY LEVELS</subject><subject>Exact sciences and technology</subject><subject>EXCITED STATES</subject><subject>EXPERIMENTAL DATA</subject><subject>General and physical chemistry</subject><subject>General. Nomenclature, chemical documentation, computer chemistry</subject><subject>HYDROGEN</subject><subject>INFORMATION</subject><subject>INFRARED SPECTRA</subject><subject>INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY</subject><subject>LOW TEMPERATURE</subject><subject>MAGNETIC RESONANCE</subject><subject>METALS</subject><subject>MINERALS</subject><subject>NICKEL</subject><subject>NONMETALS</subject><subject>NUMERICAL DATA</subject><subject>OXIDE MINERALS</subject><subject>OXIDES</subject><subject>OXYGEN COMPOUNDS</subject><subject>PHOTOCHEMICAL REACTIONS</subject><subject>REDUCTION</subject><subject>RESONANCE</subject><subject>SILICA</subject><subject>SILICON COMPOUNDS</subject><subject>SILICON OXIDES</subject><subject>SPECTRA</subject><subject>SYNTHESIS</subject><subject>Theory of reactions, general kinetics</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><subject>TRANSITION ELEMENTS</subject><issn>0022-3654</issn><issn>1541-5740</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>1987</creationdate><recordtype>article</recordtype><recordid>eNpt0FFvFCEQB_CN0cSz-uQXIMbEB4PCssDeo2lqNZ6xiaevZMrOely3sGG4xvOT-HGlWdv44BNM5gcD_6Z5LsUbKVr5di-FUMKCaMWDZiV1J7m2nXjYrIRoW66M7h43T4j2QgiplFw1vy8yzpChhBRZGtl1iomzlNkvzOkGJoyFxeCvcGKXR0Yh_pjwtk0H75Eo3NQqIscJfckp8pIh0ogVFJyJhcjKDtm8SyVlHA7-bg6FKXjgdJjnlAsOd0M8FJiOVOhp82iEifDZ3_Wk-fb-bHv6gW--nH88fbfhoGxXuOpBtQY78Fb7oZOAoq_12gy9wkHXjcd1t1ZV6FEMFuyAl2C60Y6dRT2ok-bFcm-iEhz5UNDvfIqxfsjpXsu16it6vSCfE1HG0c05XEM-OincbfLun-SrfrnoGcjDNNZIfKD7I9aY3hhZGV9YqFn9vG9DvnLGKqvd9uKr237uPm225rs7r_7V4sGT26dDjjWX_z7gD9UFom8</recordid><startdate>198711</startdate><enddate>198711</enddate><creator>Bonneviot, L</creator><creator>Cai, F. X</creator><creator>Che, M</creator><creator>Kermarec, M</creator><creator>Legendre, O</creator><creator>Lepetit, C</creator><creator>Olivier, D</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope></search><sort><creationdate>198711</creationdate><title>Preparation of mono- or zerovalent nickel by single or successive one-electron-transfer steps in the photoreduction of silica-supported nickel catalysts</title><author>Bonneviot, L ; Cai, F. X ; Che, M ; Kermarec, M ; Legendre, O ; Lepetit, C ; Olivier, D</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a374t-38a326e4ac75cd41ae0826e96d83ed5e96ce9493e4a5f0d7a7deba64f7f47e5d3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>1987</creationdate><topic>400500 - Photochemistry</topic><topic>CARBON COMPOUNDS</topic><topic>CARBON MONOXIDE</topic><topic>CARBON OXIDES</topic><topic>Catalysis</topic><topic>CATALYST SUPPORTS</topic><topic>CATALYSTS</topic><topic>Catalysts: preparations and properties</topic><topic>Catalytic reactions</topic><topic>CHALCOGENIDES</topic><topic>CHEMICAL PREPARATION</topic><topic>CHEMICAL REACTIONS</topic><topic>Chemistry</topic><topic>DATA</topic><topic>ELECTRON SPIN RESONANCE</topic><topic>ELECTRON TRANSFER</topic><topic>ELEMENTS</topic><topic>ENERGY LEVELS</topic><topic>Exact sciences and technology</topic><topic>EXCITED STATES</topic><topic>EXPERIMENTAL DATA</topic><topic>General and physical chemistry</topic><topic>General. Nomenclature, chemical documentation, computer chemistry</topic><topic>HYDROGEN</topic><topic>INFORMATION</topic><topic>INFRARED SPECTRA</topic><topic>INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY</topic><topic>LOW TEMPERATURE</topic><topic>MAGNETIC RESONANCE</topic><topic>METALS</topic><topic>MINERALS</topic><topic>NICKEL</topic><topic>NONMETALS</topic><topic>NUMERICAL DATA</topic><topic>OXIDE MINERALS</topic><topic>OXIDES</topic><topic>OXYGEN COMPOUNDS</topic><topic>PHOTOCHEMICAL REACTIONS</topic><topic>REDUCTION</topic><topic>RESONANCE</topic><topic>SILICA</topic><topic>SILICON COMPOUNDS</topic><topic>SILICON OXIDES</topic><topic>SPECTRA</topic><topic>SYNTHESIS</topic><topic>Theory of reactions, general kinetics</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><topic>TRANSITION ELEMENTS</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Bonneviot, L</creatorcontrib><creatorcontrib>Cai, F. X</creatorcontrib><creatorcontrib>Che, M</creatorcontrib><creatorcontrib>Kermarec, M</creatorcontrib><creatorcontrib>Legendre, O</creatorcontrib><creatorcontrib>Lepetit, C</creatorcontrib><creatorcontrib>Olivier, D</creatorcontrib><creatorcontrib>Universite P. et M. Curie, Paris, France</creatorcontrib><collection>Istex</collection><collection>Pascal-Francis</collection><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>J. Phys. Chem.; (United States)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Bonneviot, L</au><au>Cai, F. X</au><au>Che, M</au><au>Kermarec, M</au><au>Legendre, O</au><au>Lepetit, C</au><au>Olivier, D</au><aucorp>Universite P. et M. Curie, Paris, France</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Preparation of mono- or zerovalent nickel by single or successive one-electron-transfer steps in the photoreduction of silica-supported nickel catalysts</atitle><jtitle>J. Phys. Chem.; (United States)</jtitle><addtitle>J. Phys. Chem</addtitle><date>1987-11</date><risdate>1987</risdate><volume>91</volume><issue>23</issue><spage>5912</spage><epage>5921</epage><pages>5912-5921</pages><issn>0022-3654</issn><eissn>1541-5740</eissn><coden>JPCHAX</coden><abstract>Ni/SiO/sub 2/ supported catalysts prepared by competitive cation exchange can be reduced by UV irradiation in hydrogen at 77 K to lead by a one-electron process to Ni/sup +/ species. These Ni/sup +/ ions which exhibit an EPR signal at g/sub 1/ = 2.68, g/sub 2/ = 2.32, and g/sub 3/ = 2.007 and a band at 838 nm in the UV-vis and near-IR reflectance spectra bind molecular hydrogen to form (similarly ordered Ni(H/sub 2/))/sup +/ pseudotetrahedral surface complexes. The photoreduction process in carbon monoxide occurs appreciably only at 25/sup 0/C and depends on the CO pressure. It is a one-electron-reduction process, and (Ni(CO)/sub n/)/sup +/ species (n = 2-4) are observed by EPR and IR for pressures above 10 Torr. For lower pressures, the formation of metal is observed by IR and ferromagnetic resonance via the reduction by two consecutive one-electron-transfer steps. The first step proceeds from the photoproduction of (Ni/sup +/-O/sup -/)* excited states. The second step is due to the release of electrons from a reservoir which has been tentatively identified to pseudo-carbonates characterized by IR bands at 1750-1850 cm/sup -1/ and by TPD peaks of CO at 803 K and of CO/sub 2/ at 513 and 803 K. The formation of the latter species is the result of the quenching of the excited state by CO molecules which react with the O/sup -/ activated surface oxygens to lead to CO/sub 2//sup -/ which with O/sup 2 -/ ions generates CO/sub 3//sup 3 -/ radical ions.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><doi>10.1021/j100307a020</doi><tpages>10</tpages></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 0022-3654 |
| ispartof | J. Phys. Chem.; (United States), 1987-11, Vol.91 (23), p.5912-5921 |
| issn | 0022-3654 1541-5740 |
| language | eng |
| recordid | cdi_crossref_primary_10_1021_j100307a020 |
| source | American Chemical Society Journals |
| subjects | 400500 - Photochemistry CARBON COMPOUNDS CARBON MONOXIDE CARBON OXIDES Catalysis CATALYST SUPPORTS CATALYSTS Catalysts: preparations and properties Catalytic reactions CHALCOGENIDES CHEMICAL PREPARATION CHEMICAL REACTIONS Chemistry DATA ELECTRON SPIN RESONANCE ELECTRON TRANSFER ELEMENTS ENERGY LEVELS Exact sciences and technology EXCITED STATES EXPERIMENTAL DATA General and physical chemistry General. Nomenclature, chemical documentation, computer chemistry HYDROGEN INFORMATION INFRARED SPECTRA INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY LOW TEMPERATURE MAGNETIC RESONANCE METALS MINERALS NICKEL NONMETALS NUMERICAL DATA OXIDE MINERALS OXIDES OXYGEN COMPOUNDS PHOTOCHEMICAL REACTIONS REDUCTION RESONANCE SILICA SILICON COMPOUNDS SILICON OXIDES SPECTRA SYNTHESIS Theory of reactions, general kinetics Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry TRANSITION ELEMENTS |
| title | Preparation of mono- or zerovalent nickel by single or successive one-electron-transfer steps in the photoreduction of silica-supported nickel catalysts |
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