Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency

Glaser T, Hedman B, Hodgson KO, Solomon EI (2000)
Accounts of Chemical Research 33(12): 859-868.

Zeitschriftenaufsatz | Veröffentlicht | Englisch
 
Download
Es wurden keine Dateien hochgeladen. Nur Publikationsnachweis!
Autor*in
Glaser, ThorstenUniBi; Hedman, B; Hodgson, KO; Solomon, EI
Abstract / Bemerkung
Ligand K-edge X-ray absorption spectroscopy (XAS) is a new experimental probe of the covalency of a metal-ligand bond. The intensity of the ligand pre-edge feature is proportional to the mixing of ligand orbitals into the metal d orbitals. The methodology to determine covalencies in one-electron (hole) and many-electron systems is described and demonstrated for a series of metal tetrachlorides [MCl4](n-), metal tetrathiolates [M(SR)(4)](n-), and dimeric iron-sulfur (Fe-S) clusters [Fe2S2(SR)(4)](2-). It is there applied to blue Cu proteins, the Cu-A site, hydrogen bonding in Fe-S clusters, and the delocalization behavior in [2Fe-2S] vs [4Fe-4S] clusters. The covalencies determined in these studies provide important electronic structure insight into function.
Erscheinungsjahr
2000
Zeitschriftentitel
Accounts of Chemical Research
Band
33
Ausgabe
12
Seite(n)
859-868
ISSN
0001-4842
eISSN
1520-4898
Page URI
https://pub.uni-bielefeld.de/record/2398021

Zitieren

Glaser T, Hedman B, Hodgson KO, Solomon EI. Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency. Accounts of Chemical Research. 2000;33(12):859-868.
Glaser, T., Hedman, B., Hodgson, K. O., & Solomon, E. I. (2000). Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency. Accounts of Chemical Research, 33(12), 859-868. https://doi.org/10.1021/ar990125c
Glaser, Thorsten, Hedman, B, Hodgson, KO, and Solomon, EI. 2000. “Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency”. Accounts of Chemical Research 33 (12): 859-868.
Glaser, T., Hedman, B., Hodgson, K. O., and Solomon, E. I. (2000). Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency. Accounts of Chemical Research 33, 859-868.
Glaser, T., et al., 2000. Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency. Accounts of Chemical Research, 33(12), p 859-868.
T. Glaser, et al., “Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency”, Accounts of Chemical Research, vol. 33, 2000, pp. 859-868.
Glaser, T., Hedman, B., Hodgson, K.O., Solomon, E.I.: Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency. Accounts of Chemical Research. 33, 859-868 (2000).
Glaser, Thorsten, Hedman, B, Hodgson, KO, and Solomon, EI. “Ligand K-edge X-ray absorption spectroscopy: A direct probe of ligand-metal covalency”. Accounts of Chemical Research 33.12 (2000): 859-868.

79 Zitationen in Europe PMC

Daten bereitgestellt von Europe PubMed Central.

Scrutinizing metal-ligand covalency and redox non-innocence via nitrogen K-edge X-ray absorption spectroscopy.
Lukens JT, DiMucci IM, Kurogi T, Mindiola DJ, Lancaster KM., Chem Sci 10(19), 2019
PMID: 31183055
Aerobic reactions of antitumor active dirhodium(II) tetraacetate Rh2(CH3COO)4 with glutathione.
Enriquez Garcia A, Jalilehvand F., J Biol Inorg Chem 23(2), 2018
PMID: 29214420
Solid energy calibration standards for P K-edge XANES: electronic structure analysis of PPh4Br.
Blake AV, Wei H, Donahue CM, Lee K, Keith JM, Daly SR., J Synchrotron Radiat 25(pt 2), 2018
PMID: 29488933
Formation of the layered conductive magnet CrCl2(pyrazine)2 through redox-active coordination chemistry.
Pedersen KS, Perlepe P, Aubrey ML, Woodruff DN, Reyes-Lillo SE, Reinholdt A, Voigt L, Li Z, Borup K, Rouzières M, Samohvalov D, Wilhelm F, Rogalev A, Neaton JB, Long JR, Clérac R., Nat Chem 10(10), 2018
PMID: 30202103
The electronic properties of three popular high spin complexes [TM(acac)3, TM = Cr, Mn, and Fe] revisited: an experimental and theoretical study.
Carlotto S, Floreano L, Cossaro A, Dominguez M, Rancan M, Sambi M, Casarin M., Phys Chem Chem Phys 19(36), 2017
PMID: 28868556
Probing covalency in halogen bonds through donor K-edge X-ray absorption spectroscopy: polyhalides as coordination complexes.
Mustoe CL, Gunabalasingam M, Yu D, Patrick BO, Kennepohl P., Faraday Discuss 203(), 2017
PMID: 28740986
Mechanistic Aspects of Redox-Induced Assembly and Disassembly of S-Bridged [2M-2S] Structures.
Koch F, Berkefeld A, Speiser B, Schubert H., Chemistry 23(65), 2017
PMID: 28976037
Spectroscopic detection of halogen bonding resolves dye regeneration in the dye-sensitized solar cell.
Parlane FGL, Mustoe C, Kellett CW, Simon SJ, Swords WB, Meyer GJ, Kennepohl P, Berlinguette CP., Nat Commun 8(1), 2017
PMID: 29176734
X-ray Absorption and Emission Spectroscopic Studies of [L2Fe2S2](n) Model Complexes: Implications for the Experimental Evaluation of Redox States in Iron-Sulfur Clusters.
Kowalska JK, Hahn AW, Albers A, Schiewer CE, Bjornsson R, Lima FA, Meyer F, DeBeer S., Inorg Chem 55(9), 2016
PMID: 27097289
Structural Changes Correlated with Magnetic Spin State Isomorphism in the S2 State of the Mn4CaO5 Cluster in the Oxygen-Evolving Complex of Photosystem II.
Chatterjee R, Han G, Kern J, Gul S, Fuller FD, Garachtchenko A, Young I, Weng TC, Nordlund D, Alonso-Mori R, Bergmann U, Sokaras D, Hatakeyama M, Yachandra VK, Yano J., Chem Sci 7(8), 2016
PMID: 28044099
Evidence for 5d-σ and 5d-π covalency in lanthanide sesquioxides from oxygen K-edge X-ray absorption spectroscopy.
Altman AB, Pacold JI, Wang J, Lukens WW, Minasian SG., Dalton Trans 45(24), 2016
PMID: 26979662
Electronic structure of CuTPP and CuTPP(F) complexes: a combined experimental and theoretical study II.
Mangione G, Sambi M, Carlotto S, Vittadini A, Ligorio G, Timpel M, Pasquali L, Giglia A, Nardi MV, Casarin M., Phys Chem Chem Phys 18(36), 2016
PMID: 27412494
Evidence for halogen bond covalency in acyclic and interlocked halogen-bonding receptor anion recognition.
Robinson SW, Mustoe CL, White NG, Brown A, Thompson AL, Kennepohl P, Beer PD., J Am Chem Soc 137(1), 2015
PMID: 25478893
Bacterial iron-sulfur cluster sensors in mammalian pathogens.
Miller HK, Auerbuch V., Metallomics 7(6), 2015
PMID: 25738802
Broken-Symmetry DFT Computations for the Reaction Pathway of IspH, an Iron-Sulfur Enzyme in Pathogenic Bacteria.
Blachly PG, Sandala GM, Giammona DA, Bashford D, McCammon JA, Noodleman L., Inorg Chem 54(13), 2015
PMID: 26098647
X-ray spectroscopy for chemistry in the 2-4 keV energy regime at the XMaS beamline: ionic liquids, Rh and Pd catalysts in gas and liquid environments, and Cl contamination in γ-Al2O3.
Thompson PB, Nguyen BN, Nicholls R, Bourne RA, Brazier JB, Lovelock KR, Brown SD, Wermeille D, Bikondoa O, Lucas CA, Hase TP, Newton MA., J Synchrotron Radiat 22(6), 2015
PMID: 26524308
Combined Mössbauer spectroscopic, multi-edge X-ray absorption spectroscopic, and density functional theoretical study of the radical SAM enzyme spore photoproduct lyase.
Silver SC, Gardenghi DJ, Naik SG, Shepard EM, Huynh BH, Szilagyi RK, Broderick JB., J Biol Inorg Chem 19(3), 2014
PMID: 24532333
Solvation dependence of valence electronic states of water diluted in organic solvents probed by soft X-ray spectroscopy.
Tokushima T, Horikawa Y, Takahashi O, Arai H, Sadakane K, Harada Y, Takata Y, Shin S., Phys Chem Chem Phys 16(22), 2014
PMID: 24756213
Use of Broken-Symmetry Density Functional Theory To Characterize the IspH Oxidized State: Implications for IspH Mechanism and Inhibition.
Blachly PG, Sandala GM, Giammona DA, Liu T, Bashford D, McCammon JA, Noodleman L., J Chem Theory Comput 10(9), 2014
PMID: 25221444
Experimental determination of redox cooperativity and electronic structures in catalytically active Cu-Fe and Zn-Fe heterobimetallic complexes.
Karunananda MK, Vázquez FX, Alp EE, Bi W, Chattopadhyay S, Shibata T, Mankad NP., Dalton Trans 43(36), 2014
PMID: 25100199
Using solution- and solid-state S K-edge X-ray absorption spectroscopy with density functional theory to evaluate M-S bonding for MS4(2-) (M = Cr, Mo, W) dianions.
Olson AC, Keith JM, Batista ER, Boland KS, Daly SR, Kozimor SA, MacInnes MM, Martin RL, Scott BL., Dalton Trans 43(46), 2014
PMID: 25311904
Electronic properties of CuPc and H2Pc: an experimental and theoretical study.
Nardi MV, Detto F, Aversa L, Verucchi R, Salviati G, Iannotta S, Casarin M., Phys Chem Chem Phys 15(31), 2013
PMID: 23807700
Non-innocent ligand behaviour of a bimetallic Cu complex employing a bridging catecholate.
Dunn TJ, Chiang L, Ramogida CF, Webb MI, Savard D, Sakaguchi M, Ogura T, Shimazaki Y, Storr T., Dalton Trans 41(26), 2012
PMID: 22576939
Origin-independent calculation of quadrupole intensities in X-ray spectroscopy.
Bernadotte S, Atkins AJ, Jacob CR., J Chem Phys 137(20), 2012
PMID: 23205980
Note: Construction of x-ray scattering and x-ray absorption fine structure beamline at the Pohang Light Source.
Lee IJ, Yu CJ, Yun YD, Lee CS, Seo ID, Kim HY, Lee WW, Chae KH., Rev Sci Instrum 81(2), 2010
PMID: 20192520
A low band gap iron sulfide hybrid semiconductor with unique 2D [Fe(16)S(20)](8-) layer and reduced thermal conductivity.
Wu M, Rhee J, Emge TJ, Yao H, Cheng JH, Thiagarajan S, Croft M, Yang R, Li J., Chem Commun (Camb) 46(10), 2010
PMID: 20177604
Solvation effects on S K-edge XAS spectra of Fe-S proteins: normal and inverse effects on WT and mutant rubredoxin.
Sun N, Dey A, Xiao Z, Wedd AG, Hodgson KO, Hedman B, Solomon EI., J Am Chem Soc 132(36), 2010
PMID: 20726554
Electronic structural investigations of ruthenium compounds and anticancer prodrugs.
Harris TV, Szilagyi RK, McFarlane Holman KL., J Biol Inorg Chem 14(6), 2009
PMID: 19350289
Highly oxidized diiron complexes: generation, spectroscopy, and stabilities.
Strautmann JB, Freiherr von Richthofen CG, DeBeer George S, Bothe E, Bill E, Glaser T., Chem Commun (Camb) (19), 2009
PMID: 19532905
S K-edge XAS and DFT calculations on cytochrome P450: covalent and ionic contributions to the cysteine-Fe bond and their contribution to reactivity.
Dey A, Jiang Y, Ortiz de Montellano P, Hodgson KO, Hedman B, Solomon EI., J Am Chem Soc 131(22), 2009
PMID: 19438234
Comparison of Structurally-Related Alkoxide, Amine, and Thiolate-Ligated M (M= Fe, Co) Complexes: the Influence of Thiolates on the Properties of Biologically Relevant Metal Complexes.
Brines LM, Villar-Acevedo G, Kitagawa T, Swartz RD, Lugo-Mas P, Kaminsky W, Benedict JB, Kovacs JA., Inorganica Chim Acta 361(4), 2008
PMID: 21731109
Trinuclear copper complexes with triplesalen ligands: geometric and electronic effects on ferromagnetic coupling via the spin-polarization mechanism.
Glaser T, Heidemeier M, Strautmann JB, Bögge H, Stammler A, Krickemeyer E, Huenerbein R, Grimme S, Bothe E, Bill E., Chemistry 13(33), 2007
PMID: 17937379
Sulfur K-edge X-ray absorption spectroscopy as a probe of ligand-metal bond covalency: metal vs ligand oxidation in copper and nickel dithiolene complexes.
Sarangi R, DeBeer George S, Rudd DJ, Szilagyi RK, Ribas X, Rovira C, Almeida M, Almeida M, Hodgson KO, Hedman B, Solomon EI., J Am Chem Soc 129(8), 2007
PMID: 17269767
S K-edge XAS and DFT calculations on square-planar NiII-thiolate complexes: effects of active and passive H-bonding.
Dey A, Green KN, Jenkins RM, Jeffrey SP, Darensbourg M, Hodgson KO, Hedman B, Solomon EI., Inorg Chem 46(23), 2007
PMID: 17949080
Solvent tuning of electrochemical potentials in the active sites of HiPIP versus ferredoxin.
Dey A, Jenney FE, Adams MW, Babini E, Takahashi Y, Fukuyama K, Hodgson KO, Hedman B, Solomon EI., Science 318(5855), 2007
PMID: 18048692
Sulfur K-edge XAS and DFT calculations on nitrile hydratase: geometric and electronic structure of the non-heme iron active site.
Dey A, Chow M, Taniguchi K, Lugo-Mas P, Davin S, Maeda M, Kovacs JA, Odaka M, Hodgson KO, Hedman B, Solomon EI., J Am Chem Soc 128(2), 2006
PMID: 16402841
Desulfovibrio gigas ferredoxin II: redox structural modulation of the [3Fe-4S] cluster.
Rodrigues PM, Macedo AL, Goodfellow BJ, Moura I, Moura JJ., J Biol Inorg Chem 11(3), 2006
PMID: 16453120
Sulfur: not a "silent" element any more.
Jalilehvand F., Chem Soc Rev 35(12), 2006
PMID: 17225887
How does single oxygen atom addition affect the properties of an Fe-nitrile hydratase analogue? The compensatory role of the unmodified thiolate.
Lugo-Mas P, Dey A, Xu L, Davin SD, Benedict J, Kaminsky W, Hodgson KO, Hedman B, Solomon EI, Kovacs JA., J Am Chem Soc 128(34), 2006
PMID: 16925440
Profile of Edward I. Solomon.
Zagorski N., Proc Natl Acad Sci U S A 103(35), 2006
PMID: 16924096
On the accuracy of density functional theory for iron-sulfur clusters.
Szilagyi RK, Winslow MA., J Comput Chem 27(12), 2006
PMID: 16788911
X-ray spectroscopy of the Mn4Ca cluster in the water-oxidation complex of Photosystem II.
Sauer K, Yano J, Yachandra VK., Photosynth Res 85(1), 2005
PMID: 15977060
Structure, function, and formation of biological iron-sulfur clusters.
Johnson DC, Dean DR, Smith AD, Johnson MK., Annu Rev Biochem 74(), 2005
PMID: 15952888
Sulfur K-edge X-ray absorption spectroscopy as an experimental probe for S-nitroso proteins.
Szilagyi RK, Schwab DE., Biochem Biophys Res Commun 330(1), 2005
PMID: 15781232
A 1,8-naphthalenediol-based unsymmetrical dinucleating ligand.
Glaser T, Liratzis I, Fröhlich R., Dalton Trans (17), 2005
PMID: 16094478
Sulfur K-edge XAS and DFT calculations on P450 model complexes: effects of hydrogen bonding on electronic structure and redox potentials.
Dey A, Okamura TA, Ueyama N, Hedman B, Hodgson KO, Solomon EI., J Am Chem Soc 127(34), 2005
PMID: 16117545
Electronic structure and its relation to function in copper proteins.
Szilagyi RK, Solomon EI., Curr Opin Chem Biol 6(2), 2002
PMID: 12039012
Insights into properties and energetics of iron-sulfur proteins from simple clusters to nitrogenase.
Noodleman L, Lovell T, Liu T, Himo F, Torres RA., Curr Opin Chem Biol 6(2), 2002
PMID: 12039013
Recent advances in bioinorganic spectroscopy.
Lehnert N, George SD, Solomon EI., Curr Opin Chem Biol 5(2), 2001
PMID: 11282345

References

Daten bereitgestellt von Europe PubMed Central.

Export

Markieren/ Markierung löschen
Markierte Publikationen

Open Data PUB

Web of Science

Dieser Datensatz im Web of Science®
Quellen

PMID: 11123885
PubMed | Europe PMC

Suchen in

Google Scholar