Structural and biochemical properties of bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate and adenosine 5'-diphosphate
The structural and biochemical properties of the alpha,beta-bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate [Rh(H2O)4PP] and adenosine diphosphate [Rh(H2O)4ADP] are examined. These Rh(III) complexes are exchange-inert analogues of the corresponding physiologically important MgII...
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| Veröffentlicht in: | Biochemistry (Easton) 1987-04, Vol.26 (7), p.2060-2066 |
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| creator | Shorter, Andrew L Haromy, Tuli P Scalzo-Brush, Theresa Knight, Wilson B Dunaway-Mariano, Debra Sundaralingam, Muttaiya |
| description | The structural and biochemical properties of the alpha,beta-bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate [Rh(H2O)4PP] and adenosine diphosphate [Rh(H2O)4ADP] are examined. These Rh(III) complexes are exchange-inert analogues of the corresponding physiologically important MgIIPP and MgIIADP complexes. The crystal structure of [Rh(H2O)4H2P2O7]+Cl- shows that the six-membered chelate ring adopts a twist-boat conformation with an unusually high puckering amplitude of 0.756 (3) A. The Rh coordination distances average 2.02 (1) A, while the bridge P-O bonds are virtually equal in length. All 10 protons of the complex participate in hydrogen bonding. There are two intramolecular hydrogen bonds between the phosphate oxygen atoms and the axially coordinated water molecules. The Rh(H2O)4PP complex was found to be a substrate for yeast inorganic pyrophosphatase, with Ki = 0.063 (7) mM and Vm = 500 (100) min-1. The two screw sense isomers of Rh(H2O)4ADP were prepared from (Rp)-[alpha-16O,18O]ADP and assigned configuration on the basis of the magnitude of their 31P NMR isotopic chemical shifts. The Rh(H2O)4ADP complex binds a number of kinases as tightly as MgADP. Arginine kinase and creatine kinase were shown to bind the delta Rh(H2O)4ADP isomer 7 and 45 times tighter, respectively, than the lambda isomer. The reactivity of Rh(H2O)4PP with pyrophosphatase is comparable to that of Cr(H2O)4PP, and the binding affinities of the Rh(H2O)4ADP screw sense isomers for kinases are also comparable to those observed for the corresponding Cr(H2O)4ADP screw sense isomers. |
| doi_str_mv | 10.1021/bi00381a040 |
| format | Article |
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These Rh(III) complexes are exchange-inert analogues of the corresponding physiologically important MgIIPP and MgIIADP complexes. The crystal structure of [Rh(H2O)4H2P2O7]+Cl- shows that the six-membered chelate ring adopts a twist-boat conformation with an unusually high puckering amplitude of 0.756 (3) A. The Rh coordination distances average 2.02 (1) A, while the bridge P-O bonds are virtually equal in length. All 10 protons of the complex participate in hydrogen bonding. There are two intramolecular hydrogen bonds between the phosphate oxygen atoms and the axially coordinated water molecules. The Rh(H2O)4PP complex was found to be a substrate for yeast inorganic pyrophosphatase, with Ki = 0.063 (7) mM and Vm = 500 (100) min-1. The two screw sense isomers of Rh(H2O)4ADP were prepared from (Rp)-[alpha-16O,18O]ADP and assigned configuration on the basis of the magnitude of their 31P NMR isotopic chemical shifts. The Rh(H2O)4ADP complex binds a number of kinases as tightly as MgADP. Arginine kinase and creatine kinase were shown to bind the delta Rh(H2O)4ADP isomer 7 and 45 times tighter, respectively, than the lambda isomer. The reactivity of Rh(H2O)4PP with pyrophosphatase is comparable to that of Cr(H2O)4PP, and the binding affinities of the Rh(H2O)4ADP screw sense isomers for kinases are also comparable to those observed for the corresponding Cr(H2O)4ADP screw sense isomers.</description><identifier>ISSN: 0006-2960</identifier><identifier>EISSN: 1520-4995</identifier><identifier>DOI: 10.1021/bi00381a040</identifier><identifier>PMID: 3036218</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>550201 - Biochemistry- Tracer Techniques ; Adenosine Diphosphate - analogs & derivatives ; Adenosine Diphosphate - chemical synthesis ; Adenosine Diphosphate - pharmacology ; ADP ; BASIC BIOLOGICAL SCIENCES ; BIOCHEMICAL REACTION KINETICS ; Biological and medical sciences ; Chemical Phenomena ; CHEMICAL PROPERTIES ; CHEMICAL SHIFT ; Chemistry ; COMPLEXES ; Diphosphates - pharmacology ; ELEMENTS ; ENZYMES ; Fundamental and applied biological sciences. Psychology ; ISOTOPES ; KINETICS ; LIGHT NUCLEI ; MAGNETIC RESONANCE ; Magnetic Resonance Spectroscopy ; METALS ; Models, Molecular ; Molecular biophysics ; Molecular Conformation ; MOLECULAR STRUCTURE ; NMR SPECTRA ; NUCLEAR MAGNETIC RESONANCE ; NUCLEI ; NUCLEOTIDES ; ODD-EVEN NUCLEI ; ORGANIC COMPOUNDS ; Organophosphorus Compounds - chemical synthesis ; Organophosphorus Compounds - pharmacology ; OXYGEN COMPOUNDS ; OXYGEN ISOTOPES ; PHOSPHORUS 31 ; PHOSPHORUS COMPOUNDS ; PHOSPHORUS ISOTOPES ; Phosphorus Radioisotopes ; PHOSPHORUS-GROUP TRANSFERASES ; PHOSPHOTRANSFERASES ; Phosphotransferases - antagonists & inhibitors ; PLATINUM METALS ; PYROPHOSPHATES ; REACTION KINETICS ; RESONANCE ; RHODIUM ; Rhodium - pharmacology ; SPECTRA ; STABLE ISOTOPES ; Structure in molecular biology ; TRANSFERASES ; TRANSITION ELEMENTS ; Tridimensional structure</subject><ispartof>Biochemistry (Easton), 1987-04, Vol.26 (7), p.2060-2066</ispartof><rights>1988 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a410t-9d95b3a008396615b42b2ff141c04d6018c8872f0323f4eb1be4111fe43191073</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/bi00381a040$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/bi00381a040$$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=7444106$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/3036218$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/6074412$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Shorter, Andrew L</creatorcontrib><creatorcontrib>Haromy, Tuli P</creatorcontrib><creatorcontrib>Scalzo-Brush, Theresa</creatorcontrib><creatorcontrib>Knight, Wilson B</creatorcontrib><creatorcontrib>Dunaway-Mariano, Debra</creatorcontrib><creatorcontrib>Sundaralingam, Muttaiya</creatorcontrib><creatorcontrib>Univ. of Maryland, College Park</creatorcontrib><title>Structural and biochemical properties of bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate and adenosine 5'-diphosphate</title><title>Biochemistry (Easton)</title><addtitle>Biochemistry</addtitle><description>The structural and biochemical properties of the alpha,beta-bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate [Rh(H2O)4PP] and adenosine diphosphate [Rh(H2O)4ADP] are examined. These Rh(III) complexes are exchange-inert analogues of the corresponding physiologically important MgIIPP and MgIIADP complexes. The crystal structure of [Rh(H2O)4H2P2O7]+Cl- shows that the six-membered chelate ring adopts a twist-boat conformation with an unusually high puckering amplitude of 0.756 (3) A. The Rh coordination distances average 2.02 (1) A, while the bridge P-O bonds are virtually equal in length. All 10 protons of the complex participate in hydrogen bonding. There are two intramolecular hydrogen bonds between the phosphate oxygen atoms and the axially coordinated water molecules. The Rh(H2O)4PP complex was found to be a substrate for yeast inorganic pyrophosphatase, with Ki = 0.063 (7) mM and Vm = 500 (100) min-1. The two screw sense isomers of Rh(H2O)4ADP were prepared from (Rp)-[alpha-16O,18O]ADP and assigned configuration on the basis of the magnitude of their 31P NMR isotopic chemical shifts. The Rh(H2O)4ADP complex binds a number of kinases as tightly as MgADP. Arginine kinase and creatine kinase were shown to bind the delta Rh(H2O)4ADP isomer 7 and 45 times tighter, respectively, than the lambda isomer. The reactivity of Rh(H2O)4PP with pyrophosphatase is comparable to that of Cr(H2O)4PP, and the binding affinities of the Rh(H2O)4ADP screw sense isomers for kinases are also comparable to those observed for the corresponding Cr(H2O)4ADP screw sense isomers.</description><subject>550201 - Biochemistry- Tracer Techniques</subject><subject>Adenosine Diphosphate - analogs & derivatives</subject><subject>Adenosine Diphosphate - chemical synthesis</subject><subject>Adenosine Diphosphate - pharmacology</subject><subject>ADP</subject><subject>BASIC BIOLOGICAL SCIENCES</subject><subject>BIOCHEMICAL REACTION KINETICS</subject><subject>Biological and medical sciences</subject><subject>Chemical Phenomena</subject><subject>CHEMICAL PROPERTIES</subject><subject>CHEMICAL SHIFT</subject><subject>Chemistry</subject><subject>COMPLEXES</subject><subject>Diphosphates - pharmacology</subject><subject>ELEMENTS</subject><subject>ENZYMES</subject><subject>Fundamental and applied biological sciences. Psychology</subject><subject>ISOTOPES</subject><subject>KINETICS</subject><subject>LIGHT NUCLEI</subject><subject>MAGNETIC RESONANCE</subject><subject>Magnetic Resonance Spectroscopy</subject><subject>METALS</subject><subject>Models, Molecular</subject><subject>Molecular biophysics</subject><subject>Molecular Conformation</subject><subject>MOLECULAR STRUCTURE</subject><subject>NMR SPECTRA</subject><subject>NUCLEAR MAGNETIC RESONANCE</subject><subject>NUCLEI</subject><subject>NUCLEOTIDES</subject><subject>ODD-EVEN NUCLEI</subject><subject>ORGANIC COMPOUNDS</subject><subject>Organophosphorus Compounds - chemical synthesis</subject><subject>Organophosphorus Compounds - pharmacology</subject><subject>OXYGEN COMPOUNDS</subject><subject>OXYGEN ISOTOPES</subject><subject>PHOSPHORUS 31</subject><subject>PHOSPHORUS COMPOUNDS</subject><subject>PHOSPHORUS ISOTOPES</subject><subject>Phosphorus Radioisotopes</subject><subject>PHOSPHORUS-GROUP TRANSFERASES</subject><subject>PHOSPHOTRANSFERASES</subject><subject>Phosphotransferases - antagonists & inhibitors</subject><subject>PLATINUM METALS</subject><subject>PYROPHOSPHATES</subject><subject>REACTION KINETICS</subject><subject>RESONANCE</subject><subject>RHODIUM</subject><subject>Rhodium - pharmacology</subject><subject>SPECTRA</subject><subject>STABLE ISOTOPES</subject><subject>Structure in molecular biology</subject><subject>TRANSFERASES</subject><subject>TRANSITION ELEMENTS</subject><subject>Tridimensional structure</subject><issn>0006-2960</issn><issn>1520-4995</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>1987</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNptkc1rFTEUxYMo9VlduRYGKVaR0ZuP-VpK1fqgoNLnxk3IZO44qTPJNMlA-y_4V5vHPB4uXIXL-d2TyzmEPKfwjgKj71sDwGuqQMADsqEFg1w0TfGQbACgzFlTwmPyJISbNAqoxAk54cBLRusN-XMd_aLj4tWYKdtlrXF6wMnoNM_ezeijwZC5Pikd2qgiZhGjV-p2UX5wnVmm19vt9k2m3TSPeLfCxjr_S1mjs_k-uQwuzMN-df-FSj4uGItZcZ535ig-JY96NQZ8dnhPyY_Pn3YXX_Krr5fbiw9XuRIUYt50TdFyBVDzpixp0QrWsr6ngmoQXQm01nVdsR44473AlrYoKKU9Ck4bChU_JS9XXxeikUGbiHrQzlrUUZYpH0FZgl6tUArhdsEQ5WSCxnFUFt0SZFUVouL13u3tCmrvQvDYy9mbSfl7SUHu65H_1JPoFwfbpZ2wO7KHPpJ-dtBVSBX0XlltwhFLt6UMyoTlK2ZCxLujrPxvWVa8KuTu27X8zj7u-OXPUu6PPF95pYO8cYu3KeD_HvgXYZuzYA</recordid><startdate>19870407</startdate><enddate>19870407</enddate><creator>Shorter, Andrew L</creator><creator>Haromy, Tuli P</creator><creator>Scalzo-Brush, Theresa</creator><creator>Knight, Wilson B</creator><creator>Dunaway-Mariano, Debra</creator><creator>Sundaralingam, Muttaiya</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>IQODW</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>OTOTI</scope></search><sort><creationdate>19870407</creationdate><title>Structural and biochemical properties of bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate and adenosine 5'-diphosphate</title><author>Shorter, Andrew L ; Haromy, Tuli P ; Scalzo-Brush, Theresa ; Knight, Wilson B ; Dunaway-Mariano, Debra ; Sundaralingam, Muttaiya</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a410t-9d95b3a008396615b42b2ff141c04d6018c8872f0323f4eb1be4111fe43191073</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>1987</creationdate><topic>550201 - Biochemistry- Tracer Techniques</topic><topic>Adenosine Diphosphate - analogs & derivatives</topic><topic>Adenosine Diphosphate - chemical synthesis</topic><topic>Adenosine Diphosphate - pharmacology</topic><topic>ADP</topic><topic>BASIC BIOLOGICAL SCIENCES</topic><topic>BIOCHEMICAL REACTION KINETICS</topic><topic>Biological and medical sciences</topic><topic>Chemical Phenomena</topic><topic>CHEMICAL PROPERTIES</topic><topic>CHEMICAL SHIFT</topic><topic>Chemistry</topic><topic>COMPLEXES</topic><topic>Diphosphates - pharmacology</topic><topic>ELEMENTS</topic><topic>ENZYMES</topic><topic>Fundamental and applied biological sciences. Psychology</topic><topic>ISOTOPES</topic><topic>KINETICS</topic><topic>LIGHT NUCLEI</topic><topic>MAGNETIC RESONANCE</topic><topic>Magnetic Resonance Spectroscopy</topic><topic>METALS</topic><topic>Models, Molecular</topic><topic>Molecular biophysics</topic><topic>Molecular Conformation</topic><topic>MOLECULAR STRUCTURE</topic><topic>NMR SPECTRA</topic><topic>NUCLEAR MAGNETIC RESONANCE</topic><topic>NUCLEI</topic><topic>NUCLEOTIDES</topic><topic>ODD-EVEN NUCLEI</topic><topic>ORGANIC COMPOUNDS</topic><topic>Organophosphorus Compounds - chemical synthesis</topic><topic>Organophosphorus Compounds - pharmacology</topic><topic>OXYGEN COMPOUNDS</topic><topic>OXYGEN ISOTOPES</topic><topic>PHOSPHORUS 31</topic><topic>PHOSPHORUS COMPOUNDS</topic><topic>PHOSPHORUS ISOTOPES</topic><topic>Phosphorus Radioisotopes</topic><topic>PHOSPHORUS-GROUP TRANSFERASES</topic><topic>PHOSPHOTRANSFERASES</topic><topic>Phosphotransferases - antagonists & inhibitors</topic><topic>PLATINUM METALS</topic><topic>PYROPHOSPHATES</topic><topic>REACTION KINETICS</topic><topic>RESONANCE</topic><topic>RHODIUM</topic><topic>Rhodium - pharmacology</topic><topic>SPECTRA</topic><topic>STABLE ISOTOPES</topic><topic>Structure in molecular biology</topic><topic>TRANSFERASES</topic><topic>TRANSITION ELEMENTS</topic><topic>Tridimensional structure</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Shorter, Andrew L</creatorcontrib><creatorcontrib>Haromy, Tuli P</creatorcontrib><creatorcontrib>Scalzo-Brush, Theresa</creatorcontrib><creatorcontrib>Knight, Wilson B</creatorcontrib><creatorcontrib>Dunaway-Mariano, Debra</creatorcontrib><creatorcontrib>Sundaralingam, Muttaiya</creatorcontrib><creatorcontrib>Univ. of Maryland, College Park</creatorcontrib><collection>Istex</collection><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV</collection><jtitle>Biochemistry (Easton)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Shorter, Andrew L</au><au>Haromy, Tuli P</au><au>Scalzo-Brush, Theresa</au><au>Knight, Wilson B</au><au>Dunaway-Mariano, Debra</au><au>Sundaralingam, Muttaiya</au><aucorp>Univ. of Maryland, College Park</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Structural and biochemical properties of bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate and adenosine 5'-diphosphate</atitle><jtitle>Biochemistry (Easton)</jtitle><addtitle>Biochemistry</addtitle><date>1987-04-07</date><risdate>1987</risdate><volume>26</volume><issue>7</issue><spage>2060</spage><epage>2066</epage><pages>2060-2066</pages><issn>0006-2960</issn><eissn>1520-4995</eissn><abstract>The structural and biochemical properties of the alpha,beta-bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate [Rh(H2O)4PP] and adenosine diphosphate [Rh(H2O)4ADP] are examined. These Rh(III) complexes are exchange-inert analogues of the corresponding physiologically important MgIIPP and MgIIADP complexes. The crystal structure of [Rh(H2O)4H2P2O7]+Cl- shows that the six-membered chelate ring adopts a twist-boat conformation with an unusually high puckering amplitude of 0.756 (3) A. The Rh coordination distances average 2.02 (1) A, while the bridge P-O bonds are virtually equal in length. All 10 protons of the complex participate in hydrogen bonding. There are two intramolecular hydrogen bonds between the phosphate oxygen atoms and the axially coordinated water molecules. The Rh(H2O)4PP complex was found to be a substrate for yeast inorganic pyrophosphatase, with Ki = 0.063 (7) mM and Vm = 500 (100) min-1. The two screw sense isomers of Rh(H2O)4ADP were prepared from (Rp)-[alpha-16O,18O]ADP and assigned configuration on the basis of the magnitude of their 31P NMR isotopic chemical shifts. The Rh(H2O)4ADP complex binds a number of kinases as tightly as MgADP. Arginine kinase and creatine kinase were shown to bind the delta Rh(H2O)4ADP isomer 7 and 45 times tighter, respectively, than the lambda isomer. The reactivity of Rh(H2O)4PP with pyrophosphatase is comparable to that of Cr(H2O)4PP, and the binding affinities of the Rh(H2O)4ADP screw sense isomers for kinases are also comparable to those observed for the corresponding Cr(H2O)4ADP screw sense isomers.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>3036218</pmid><doi>10.1021/bi00381a040</doi><tpages>7</tpages></addata></record> |
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| ispartof | Biochemistry (Easton), 1987-04, Vol.26 (7), p.2060-2066 |
| issn | 0006-2960 1520-4995 |
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| subjects | 550201 - Biochemistry- Tracer Techniques Adenosine Diphosphate - analogs & derivatives Adenosine Diphosphate - chemical synthesis Adenosine Diphosphate - pharmacology ADP BASIC BIOLOGICAL SCIENCES BIOCHEMICAL REACTION KINETICS Biological and medical sciences Chemical Phenomena CHEMICAL PROPERTIES CHEMICAL SHIFT Chemistry COMPLEXES Diphosphates - pharmacology ELEMENTS ENZYMES Fundamental and applied biological sciences. Psychology ISOTOPES KINETICS LIGHT NUCLEI MAGNETIC RESONANCE Magnetic Resonance Spectroscopy METALS Models, Molecular Molecular biophysics Molecular Conformation MOLECULAR STRUCTURE NMR SPECTRA NUCLEAR MAGNETIC RESONANCE NUCLEI NUCLEOTIDES ODD-EVEN NUCLEI ORGANIC COMPOUNDS Organophosphorus Compounds - chemical synthesis Organophosphorus Compounds - pharmacology OXYGEN COMPOUNDS OXYGEN ISOTOPES PHOSPHORUS 31 PHOSPHORUS COMPOUNDS PHOSPHORUS ISOTOPES Phosphorus Radioisotopes PHOSPHORUS-GROUP TRANSFERASES PHOSPHOTRANSFERASES Phosphotransferases - antagonists & inhibitors PLATINUM METALS PYROPHOSPHATES REACTION KINETICS RESONANCE RHODIUM Rhodium - pharmacology SPECTRA STABLE ISOTOPES Structure in molecular biology TRANSFERASES TRANSITION ELEMENTS Tridimensional structure |
| title | Structural and biochemical properties of bidentate tetraaquarhodium(III) complexes of inorganic pyrophosphate and adenosine 5'-diphosphate |
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