A Model for the CO-Inhibited Form of [NiFe] Hydrogenase: Synthesis of $(CO)_3 Fe(\mu - S^t Bu)_3 Ni\{ SC_6 H_3 - 2,6 - (mesityl)_2 \}$ and Reversible CO Addition at the Ni Site
A [NiFe] hydrogenase model compound having a distorted trigonal-pyramidal nickel center, (CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni(SDmp), 1 (Dmp= C₆ H₃ -2; 6-(mesityl)₂), was synthesized from the reaction of the tetranuclear Fe-Ni-Ni-Fe complex [(CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni]₂ (µ-Br) 2# 2 with NaSDmp at -40 °...
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| Veröffentlicht in: | Proceedings of the National Academy of Sciences - PNAS 2010-03, Vol.107 (9), p.3994-3997 |
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| container_title | Proceedings of the National Academy of Sciences - PNAS |
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| creator | Ohki, Yasuhiro Yasumura, Kazunari Ando, Masaru Shimokata, Satoko Tatsumi, Kazuyuki Halpern, Jack |
| description | A [NiFe] hydrogenase model compound having a distorted trigonal-pyramidal nickel center, (CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni(SDmp), 1 (Dmp= C₆ H₃ -2; 6-(mesityl)₂), was synthesized from the reaction of the tetranuclear Fe-Ni-Ni-Fe complex [(CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni]₂ (µ-Br) 2# 2 with NaSDmp at -40 ° C. The nickel site of complex 1 was found to add CO or CN f Bu at -40 ° C to give (CO)₃ $Fe(\mu - S_t Bu)$$Fe(\mu - S_t Bu_2 )$ Ni(CO) (SDmp), 3, or (CO)₃ $Fe(\mu - S_t Bu)$(/ |
| doi_str_mv | 10.1073/pnas.0913399107 |
| format | Article |
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The nickel site of complex 1 was found to add CO or CN f Bu at -40 ° C to give (CO)₃ $Fe(\mu - S_t Bu)$$Fe(\mu - S_t Bu_2 )$ Ni(CO) (SDmp), 3, or (CO)₃ $Fe(\mu - S_t Bu)$(/<-S t Bu)₂ Ni(CN t Bu)(SDmp) f 4, respectively. One of the CO bands of 3, appearing at 2055crrr 1 in the infrared spectrum, was assigned as the Ni-CO band, and this frequency is comparable to those observed for the CO-inhibited forms of [NiFe] hydrogenase. Like the CO-inhibited forms of [NiFe] hydrogenase, the coordination of CO at the nickel site of 1 is reversible, while the CN'Bu adduct 4 is more robust.</description><identifier>ISSN: 0027-8424</identifier><identifier>EISSN: 1091-6490</identifier><identifier>DOI: 10.1073/pnas.0913399107</identifier><language>eng</language><publisher>National Academy of Sciences</publisher><subject>Active sites ; Adducts ; Atoms ; Chemical bonding ; Desulfovibrio ; Infrared radiation ; Ligands ; Molecular structure ; Reactivity ; Sulfur</subject><ispartof>Proceedings of the National Academy of Sciences - PNAS, 2010-03, Vol.107 (9), p.3994-3997</ispartof><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c1497-54aa94f553eba13f0307535c0e6d898227ba3cd6ec0a6b1f60399879681715393</citedby><cites>FETCH-LOGICAL-c1497-54aa94f553eba13f0307535c0e6d898227ba3cd6ec0a6b1f60399879681715393</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.jstor.org/stable/pdf/40537067$$EPDF$$P50$$Gjstor$$H</linktopdf><linktohtml>$$Uhttps://www.jstor.org/stable/40537067$$EHTML$$P50$$Gjstor$$H</linktohtml><link.rule.ids>314,776,780,799,27901,27902,57992,58225</link.rule.ids></links><search><creatorcontrib>Ohki, Yasuhiro</creatorcontrib><creatorcontrib>Yasumura, Kazunari</creatorcontrib><creatorcontrib>Ando, Masaru</creatorcontrib><creatorcontrib>Shimokata, Satoko</creatorcontrib><creatorcontrib>Tatsumi, Kazuyuki</creatorcontrib><creatorcontrib>Halpern, Jack</creatorcontrib><title>A Model for the CO-Inhibited Form of [NiFe] Hydrogenase: Synthesis of $(CO)_3 Fe(\mu - S^t Bu)_3 Ni\{ SC_6 H_3 - 2,6 - (mesityl)_2 \}$ and Reversible CO Addition at the Ni Site</title><title>Proceedings of the National Academy of Sciences - PNAS</title><description>A [NiFe] hydrogenase model compound having a distorted trigonal-pyramidal nickel center, (CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni(SDmp), 1 (Dmp= C₆ H₃ -2; 6-(mesityl)₂), was synthesized from the reaction of the tetranuclear Fe-Ni-Ni-Fe complex [(CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni]₂ (µ-Br) 2# 2 with NaSDmp at -40 ° C. The nickel site of complex 1 was found to add CO or CN f Bu at -40 ° C to give (CO)₃ $Fe(\mu - S_t Bu)$$Fe(\mu - S_t Bu_2 )$ Ni(CO) (SDmp), 3, or (CO)₃ $Fe(\mu - S_t Bu)$(/<-S t Bu)₂ Ni(CN t Bu)(SDmp) f 4, respectively. One of the CO bands of 3, appearing at 2055crrr 1 in the infrared spectrum, was assigned as the Ni-CO band, and this frequency is comparable to those observed for the CO-inhibited forms of [NiFe] hydrogenase. Like the CO-inhibited forms of [NiFe] hydrogenase, the coordination of CO at the nickel site of 1 is reversible, while the CN'Bu adduct 4 is more robust.</description><subject>Active sites</subject><subject>Adducts</subject><subject>Atoms</subject><subject>Chemical bonding</subject><subject>Desulfovibrio</subject><subject>Infrared radiation</subject><subject>Ligands</subject><subject>Molecular structure</subject><subject>Reactivity</subject><subject>Sulfur</subject><issn>0027-8424</issn><issn>1091-6490</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2010</creationdate><recordtype>article</recordtype><recordid>eNpFUE1Lw0AUXETB-nH2JLyDhwpG32aT3ay3GqwVtAWrJ6thk2x0pU3KbhSK-J_8iW5U9PIeM8y8NwwhexSPKQp2sqyVO0ZJGZPSE2ukRz0KeCRxnfQQQxEkURhtki3nXhBRxgn2yOcArptSz6FqLLTPGtJJcFk_m9y0uoRhYxfQVHA_NkP9AKNVaZsn7R_pU5iuaq93xnWCg346OcwYDHV_tniFAKaPLZy9dtTYzN5hmmYcRh4FEB5xP_sLb21X88MshNnHAai6hBv9pq0z-bxLAYOyNK1palDtd7CxgakPtUM2KjV3evd3b5O74fltOgquJheX6eAqKGgkRRBHSsmoimOmc0VZhQxFzOICNS8TmYShyBUrSq4LVDynFUdfWyIkT6igMZNsm5z83C1s45zVVba0ZqHsKqOYdYVnXeHZf-Hesf_jeHFtY__kEcZMIBfsC9pld_g</recordid><startdate>20100302</startdate><enddate>20100302</enddate><creator>Ohki, Yasuhiro</creator><creator>Yasumura, Kazunari</creator><creator>Ando, Masaru</creator><creator>Shimokata, Satoko</creator><creator>Tatsumi, Kazuyuki</creator><creator>Halpern, Jack</creator><general>National Academy of Sciences</general><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20100302</creationdate><title>A Model for the CO-Inhibited Form of [NiFe] Hydrogenase: Synthesis of $(CO)_3 Fe(\mu - S^t Bu)_3 Ni\{ SC_6 H_3 - 2,6 - (mesityl)_2 \}$ and Reversible CO Addition at the Ni Site</title><author>Ohki, Yasuhiro ; Yasumura, Kazunari ; Ando, Masaru ; Shimokata, Satoko ; Tatsumi, Kazuyuki ; Halpern, Jack</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c1497-54aa94f553eba13f0307535c0e6d898227ba3cd6ec0a6b1f60399879681715393</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2010</creationdate><topic>Active sites</topic><topic>Adducts</topic><topic>Atoms</topic><topic>Chemical bonding</topic><topic>Desulfovibrio</topic><topic>Infrared radiation</topic><topic>Ligands</topic><topic>Molecular structure</topic><topic>Reactivity</topic><topic>Sulfur</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ohki, Yasuhiro</creatorcontrib><creatorcontrib>Yasumura, Kazunari</creatorcontrib><creatorcontrib>Ando, Masaru</creatorcontrib><creatorcontrib>Shimokata, Satoko</creatorcontrib><creatorcontrib>Tatsumi, Kazuyuki</creatorcontrib><creatorcontrib>Halpern, Jack</creatorcontrib><collection>CrossRef</collection><jtitle>Proceedings of the National Academy of Sciences - PNAS</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ohki, Yasuhiro</au><au>Yasumura, Kazunari</au><au>Ando, Masaru</au><au>Shimokata, Satoko</au><au>Tatsumi, Kazuyuki</au><au>Halpern, Jack</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>A Model for the CO-Inhibited Form of [NiFe] Hydrogenase: Synthesis of $(CO)_3 Fe(\mu - S^t Bu)_3 Ni\{ SC_6 H_3 - 2,6 - (mesityl)_2 \}$ and Reversible CO Addition at the Ni Site</atitle><jtitle>Proceedings of the National Academy of Sciences - PNAS</jtitle><date>2010-03-02</date><risdate>2010</risdate><volume>107</volume><issue>9</issue><spage>3994</spage><epage>3997</epage><pages>3994-3997</pages><issn>0027-8424</issn><eissn>1091-6490</eissn><abstract>A [NiFe] hydrogenase model compound having a distorted trigonal-pyramidal nickel center, (CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni(SDmp), 1 (Dmp= C₆ H₃ -2; 6-(mesityl)₂), was synthesized from the reaction of the tetranuclear Fe-Ni-Ni-Fe complex [(CO)₃ $Fe(\mu - S_t Bu_3 )$ Ni]₂ (µ-Br) 2# 2 with NaSDmp at -40 ° C. The nickel site of complex 1 was found to add CO or CN f Bu at -40 ° C to give (CO)₃ $Fe(\mu - S_t Bu)$$Fe(\mu - S_t Bu_2 )$ Ni(CO) (SDmp), 3, or (CO)₃ $Fe(\mu - S_t Bu)$(/<-S t Bu)₂ Ni(CN t Bu)(SDmp) f 4, respectively. One of the CO bands of 3, appearing at 2055crrr 1 in the infrared spectrum, was assigned as the Ni-CO band, and this frequency is comparable to those observed for the CO-inhibited forms of [NiFe] hydrogenase. Like the CO-inhibited forms of [NiFe] hydrogenase, the coordination of CO at the nickel site of 1 is reversible, while the CN'Bu adduct 4 is more robust.</abstract><pub>National Academy of Sciences</pub><doi>10.1073/pnas.0913399107</doi><tpages>4</tpages><oa>free_for_read</oa></addata></record> |
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| source | Jstor Complete Legacy; PubMed Central; Alma/SFX Local Collection; Free Full-Text Journals in Chemistry |
| subjects | Active sites Adducts Atoms Chemical bonding Desulfovibrio Infrared radiation Ligands Molecular structure Reactivity Sulfur |
| title | A Model for the CO-Inhibited Form of [NiFe] Hydrogenase: Synthesis of $(CO)_3 Fe(\mu - S^t Bu)_3 Ni\{ SC_6 H_3 - 2,6 - (mesityl)_2 \}$ and Reversible CO Addition at the Ni Site |
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