Gerhard Schenk

Summary

Affiliation: University of Queensland
Country: Australia

Publications

  1. ncbi request reprint Binuclear metallohydrolases: complex mechanistic strategies for a simple chemical reaction
    Gerhard Schenk
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Australia
    Acc Chem Res 45:1593-603. 2012
  2. pmc Crystal structures of a purple acid phosphatase, representing different steps of this enzyme's catalytic cycle
    Gerhard Schenk
    School of Molecular and Microbial Sciences, The University of Queensland, St, Lucia, QLD 4072, Australia
    BMC Struct Biol 8:6. 2008
  3. pmc Phosphate forms an unusual tripodal complex with the Fe-Mn center of sweet potato purple acid phosphatase
    Gerhard Schenk
    Department of Biochemistry and Molecular Biology, School of Molecular and Microbial Sciences, University of Queensland, Brisbane 4072, Australia
    Proc Natl Acad Sci U S A 102:273-8. 2005
  4. ncbi request reprint Probing the role of the divalent metal ion in uteroferrin using metal ion replacement and a comparison to isostructural biomimetics
    Gerhard Schenk
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, QLD, 4072, Australia
    J Biol Inorg Chem 13:139-55. 2008
  5. doi request reprint Substrate-promoted formation of a catalytically competent binuclear center and regulation of reactivity in a glycerophosphodiesterase from Enterobacter aerogenes
    Kieran S Hadler
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, Queensland 4072, Australia
    J Am Chem Soc 130:14129-38. 2008
  6. doi request reprint Phosphate-bound structure of an organophosphate-degrading enzyme from Agrobacterium radiobacter
    Fernanda Ely
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Queensland, Australia
    J Inorg Biochem 106:19-22. 2012
  7. doi request reprint Spectroscopic and catalytic characterization of a functional Fe(III)Fe(II) biomimetic for the active site of uteroferrin and protein cleavage
    Sarah J Smith
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane 4072, Australia
    Inorg Chem 51:2065-78. 2012
  8. ncbi request reprint The reaction mechanism of the Ga(III)Zn(II) derivative of uteroferrin and corresponding biomimetics
    Sarah J Smith
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, QLD, Australia
    J Biol Inorg Chem 12:1207-20. 2007
  9. pmc The divalent metal ion in the active site of uteroferrin modulates substrate binding and catalysis
    Natasa Mitic
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Queensland, 4072, Australia
    J Am Chem Soc 132:7049-54. 2010
  10. doi request reprint Promiscuity comes at a price: catalytic versatility vs efficiency in different metal ion derivatives of the potential bioremediator GpdQ
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, QLD 4072, Australia
    Biochim Biophys Acta 1834:425-32. 2013

Collaborators

Detail Information

Publications50

  1. ncbi request reprint Binuclear metallohydrolases: complex mechanistic strategies for a simple chemical reaction
    Gerhard Schenk
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Australia
    Acc Chem Res 45:1593-603. 2012
    ..Here we only focus on catalytic strategies applied by the former group...
  2. pmc Crystal structures of a purple acid phosphatase, representing different steps of this enzyme's catalytic cycle
    Gerhard Schenk
    School of Molecular and Microbial Sciences, The University of Queensland, St, Lucia, QLD 4072, Australia
    BMC Struct Biol 8:6. 2008
    ..However, despite considerable effort in the last 10 years various aspects of the basic molecular mechanism of action are still not fully understood...
  3. pmc Phosphate forms an unusual tripodal complex with the Fe-Mn center of sweet potato purple acid phosphatase
    Gerhard Schenk
    Department of Biochemistry and Molecular Biology, School of Molecular and Microbial Sciences, University of Queensland, Brisbane 4072, Australia
    Proc Natl Acad Sci U S A 102:273-8. 2005
    ..The structure and kinetics support the hypothesis that the bridging oxygen atom initiates hydrolysis...
  4. ncbi request reprint Probing the role of the divalent metal ion in uteroferrin using metal ion replacement and a comparison to isostructural biomimetics
    Gerhard Schenk
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, QLD, 4072, Australia
    J Biol Inorg Chem 13:139-55. 2008
    ....
  5. doi request reprint Substrate-promoted formation of a catalytically competent binuclear center and regulation of reactivity in a glycerophosphodiesterase from Enterobacter aerogenes
    Kieran S Hadler
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, Queensland 4072, Australia
    J Am Chem Soc 130:14129-38. 2008
    ..Thus, it is proposed that GpdQ employs an intricate regulatory mechanism for catalysis, where coordination flexibility in one of the two metal binding sites is essential for optimal activity...
  6. doi request reprint Phosphate-bound structure of an organophosphate-degrading enzyme from Agrobacterium radiobacter
    Fernanda Ely
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Queensland, Australia
    J Inorg Biochem 106:19-22. 2012
    ..Thus, similar to the binuclear metallohydrolases urease and purple acid phosphatase the tripodal arrangement of PO(4) is interpreted in terms of a role of the μOH as a reaction nucleophile...
  7. doi request reprint Spectroscopic and catalytic characterization of a functional Fe(III)Fe(II) biomimetic for the active site of uteroferrin and protein cleavage
    Sarah J Smith
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane 4072, Australia
    Inorg Chem 51:2065-78. 2012
    ..It is interesting to note that aqueous solutions of [Fe(III)Fe(II)L1(μ-OAc)(2)](+) are also capable of protein cleavage, at mild temperature and pH conditions, thus further expanding the scope of this complex's catalytic promiscuity...
  8. ncbi request reprint The reaction mechanism of the Ga(III)Zn(II) derivative of uteroferrin and corresponding biomimetics
    Sarah J Smith
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, QLD, Australia
    J Biol Inorg Chem 12:1207-20. 2007
    ....
  9. pmc The divalent metal ion in the active site of uteroferrin modulates substrate binding and catalysis
    Natasa Mitic
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Queensland, 4072, Australia
    J Am Chem Soc 132:7049-54. 2010
    ....
  10. doi request reprint Promiscuity comes at a price: catalytic versatility vs efficiency in different metal ion derivatives of the potential bioremediator GpdQ
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, QLD 4072, Australia
    Biochim Biophys Acta 1834:425-32. 2013
    ..This article is part of a Special Issue entitled: Chemistry and mechanism of phosphatases, diesterases and triesterases...
  11. ncbi request reprint Human tartrate-resistant acid phosphatase becomes an effective ATPase upon proteolytic activation
    Natasa Mitic
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, Australia
    Arch Biochem Biophys 439:154-64. 2005
    ..Notably, at low pH this residue may act as a proton donor for the leaving group. In this respect the mechanism of cleaved TRAcP resembles that of sweet potato purple acid phosphatase...
  12. doi request reprint The organophosphate-degrading enzyme from Agrobacterium radiobacter displays mechanistic flexibility for catalysis
    Fernanda Ely
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, QLD 4072, Australia
    Biochem J 432:565-73. 2010
    ..The observed mechanistic flexibility may reconcile contrasting reaction models that have been published previously and may be beneficial for the rapid adaptation of OP-degrading enzymes to changing environmental pressures...
  13. doi request reprint Synthesis, magnetic properties, and phosphoesterase activity of dinuclear cobalt(II) complexes
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane QLD 4072, Australia
    Inorg Chem 52:2029-43. 2013
    ..Functional studies of the complexes with the substrate bis(2,4-dinitrophenyl) phosphate showed them to be active towards hydrolysis of phosphoester substrates...
  14. doi request reprint Electronic structure analysis of the dinuclear metal center in the bioremediator glycerophosphodiesterase (GpdQ) from Enterobacter aerogenes
    Kieran S Hadler
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Queensland, 4072, Australia
    Inorg Chem 49:2727-34. 2010
    ..This is the first study to investigate the electronic structure of an enzyme with a mu-1,1-carboxylate bridged dicobalt(II) center...
  15. doi request reprint The bioremediator glycerophosphodiesterase employs a non-processive mechanism for hydrolysis
    Kieran S Hadler
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Queensland 4072, Australia
    J Inorg Biochem 104:211-3. 2010
    ..Furthermore, the data indicate that the diester bonds are cleaved in two separate (non-processive) reactions, indicating that only a single nucleophile (the terminal hydroxide molecule) is likely to be employed as a nucleophile for GpdQ...
  16. doi request reprint Structural and catalytic characterization of a heterovalent Mn(II)Mn(III) complex that mimics purple acid phosphatases
    Sarah J Smith
    School of Chemistry and Molecular Biosciences, University of Queensland, Brisbane 4072, Australia
    Inorg Chem 48:10036-48. 2009
    ..2) is detected. Mechanistic implications are discussed...
  17. doi request reprint Identification of purple acid phosphatase inhibitors by fragment-based screening: promising new leads for osteoporosis therapeutics
    Daniel Feder
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, QLD 4072, Australia
    Chem Biol Drug Des 80:665-74. 2012
    ..These studies open the way to the design of more potent and selective inhibitors of purple acid phosphatases that can be tested as anti-osteoporotic drug leads...
  18. doi request reprint Structural flexibility enhances the reactivity of the bioremediator glycerophosphodiesterase by fine-tuning its mechanism of hydrolysis
    Kieran S Hadler
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Queensland, 4072, Australia
    J Am Chem Soc 131:11900-8. 2009
    ..Overall, the mechanism employed by GpdQ is a paradigm of a substrate- and metal-ion-induced fit to optimize catalysis...
  19. doi request reprint Penicillin inhibitors of purple acid phosphatase
    - Faridoon
    The University of Queensland, School of Chemistry and Molecular Biosciences, Brisbane, QLD 4072, Australia
    Bioorg Med Chem Lett 22:2555-9. 2012
    ..Molecular modelling has been used to examine the binding modes of these compounds in the active site of the enzyme and to rationalise their activities...
  20. doi request reprint Electronic and geometric structures of the organophosphate-degrading enzyme from Agrobacterium radiobacter (OpdA)
    Fernanda Ely
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, Australia
    J Biol Inorg Chem 16:777-87. 2011
    ..Mechanistic implications of these observations are discussed...
  21. doi request reprint Metal-ion mutagenesis: conversion of a purple acid phosphatase from sweet potato to a neutral phosphatase with the formation of an unprecedented catalytically competent Mn(II)Mn(II) active site
    Natasa Mitic
    School of Chemistry and Molecular Biosciences, University of Queensland, Queensland, Australia, 4072
    J Am Chem Soc 131:8173-9. 2009
    ....
  22. doi request reprint The identification of new metallo-β-lactamase inhibitor leads from fragment-based screening
    Peter Vella
    The University of Queensland, School of Chemistry and Molecular Biosciences, Brisbane, QLD 4072, Australia
    Bioorg Med Chem Lett 21:3282-5. 2011
    ..The interactions between identified inhibitory fragments and the active site of the MBL from Klebsiella pneumoniae and Pseudomonas aeruginosa were probed by in silico docking studies...
  23. doi request reprint Cadmium(II) complexes of the glycerophosphodiester-degrading enzyme GpdQ and a biomimetic N,O ligand
    Ruth E Mirams
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, QLD, 4072, Australia
    J Biol Inorg Chem 13:1065-72. 2008
    ..9, with k(cat) = 0.004 s(-1). In summary, the model is both an adequate structural and a reasonable functional mimic of GpdQ...
  24. doi request reprint The role of Zn-OR and Zn-OH nucleophiles and the influence of para-substituents in the reactions of binuclear phosphatase mimetics
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, QLD 4072, Australia
    Dalton Trans 41:1695-708. 2012
    ..The results are discussed with respect to the potential nucleophilic species (coordinated deprotonated alcohol versus coordinated hydroxide)...
  25. ncbi request reprint Phosphotyrosyl peptides and analogues as substrates and inhibitors of purple acid phosphatases
    Mohsen Valizadeh
    Department of Biochemistry, The University of Queensland, St Lucia, QLD 4072, Australia
    Arch Biochem Biophys 424:154-62. 2004
    ..These compounds are thus the most potent organic inhibitors yet reported for the purple acid phosphatases...
  26. doi request reprint Synthesis, modelling and kinetic assays of potent inhibitors of purple acid phosphatase
    Siti Hajar Mohd-Pahmi
    The University of Queensland, School of Chemistry and Molecular Biosciences, Brisbane, QLD 4072, Australia
    Bioorg Med Chem Lett 21:3092-4. 2011
    ....
  27. doi request reprint 3-mercapto-1,2,4-triazoles and N-acylated thiosemicarbazides as metallo-β-lactamase inhibitors
    - Faridoon
    The University of Queensland, School of Chemistry and Molecular Biosciences, Brisbane, QLD 4072, Australia
    Bioorg Med Chem Lett 22:380-6. 2012
    ..The interactions of these inhibitors with the active site of IMP-1 were examined using in silico methods...
  28. doi request reprint Asymmetric zinc(II) complexes as functional and structural models for phosphoesterases
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, QLD 4072, Australia
    Dalton Trans 42:9574-84. 2013
    ..45 mmol g(-1) resin. The resin bound complex was active towards BDNPP and displayed similar pH dependence to the complex in solution...
  29. ncbi request reprint The catalytic mechanisms of binuclear metallohydrolases
    Natasa Mitic
    School of Molecular and Microbial Sciences, The University of Queensland, Brisbane, QLD 4072, Australia
    Chem Rev 106:3338-63. 2006
  30. doi request reprint Cadmium(II) complexes: mimics of organophosphate pesticide degrading enzymes and metallo-β-lactamases
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, QLD 4072, Australia
    Inorg Chem 51:7669-81. 2012
    ....
  31. doi request reprint Structural and spectroscopic studies of a model for catechol oxidase
    Sarah J Smith
    School of Molecular and Microbial Sciences, The University of Queensland, St Lucia, QLD 4072, Australia
    J Biol Inorg Chem 13:499-510. 2008
    ..The complex also displays catecholase activity (k(cat) = 15 +/- 1.5 min(-1), K(M) = 6.4 +/- 1.8 mM), which is compared with other dicopper catechol oxidase models...
  32. ncbi request reprint Direct electrochemistry of porcine purple acid phosphatase (uteroferrin)
    Paul V Bernhardt
    Center for Metals in Biology, Department of Chemistry, University of Queensland, Brisbane 4072, Australia
    Biochemistry 43:10387-92. 2004
    ..The effect of pH on the redox potentials has been investigated in the range 3 < pH < 6.5, enabling acid dissociation constants for Uf(o) and its phosphate and arsenate complexes to be calculated...
  33. doi request reprint Identification and characterization of an unusual metallo-β-lactamase from Serratia proteamaculans
    Peter Vella
    School of Chemistry and Molecular Biosciences, The University of Queensland, St Lucia, QLD, 4072, Australia
    J Biol Inorg Chem 18:855-63. 2013
    ..In contrast, kinetic data suggest that the enzyme may operate as a binuclear enzyme, and it is thus proposed that a catalytically active di-Zn(2+) center is formed only once the substrate is present...
  34. doi request reprint Inhibition of purple acid phosphatase with alpha-alkoxynaphthylmethylphosphonic acids
    Ross P McGeary
    The University of Queensland, School of Molecular and Microbial Sciences, Brisbane, QLD, Australia
    Bioorg Med Chem Lett 19:163-6. 2009
    ..This manuscript describes the design and synthesis of derivatives of 1-naphthylmethylphosphonic acids as inhibitors of PAP. The K(i) values of these compounds are as low as 4 microM, the lowest reported to date for a PAP inhibitor...
  35. pmc Identification of a non-purple tartrate-resistant acid phosphatase: an evolutionary link to Ser/Thr protein phosphatases?
    Kieran S Hadler
    School of Molecular and Microbial Sciences, The University of Queensland, St, Lucia, 4072, Australia
    BMC Res Notes 1:78. 2008
    ..Due to its role in bone resorption the 35 kDa TRAcP has become a promising target for the development of anti-osteoporotic chemotherapeutics...
  36. doi request reprint Immobilization of the enzyme GpdQ on magnetite nanoparticles for organophosphate pesticide bioremediation
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane QLD 4072, Australia
    J Inorg Biochem 131:1-7. 2014
    ..39μmolmg(-1)min(-1) and after 120days 3.36μmolmg(-1)min(-1), demonstrating that the immobilized enzyme was active for multiple cycles and could be stored on the nanoparticles for a prolonged period. ..
  37. doi request reprint Spectroscopic and mechanistic studies of dinuclear metallohydrolases and their biomimetic complexes
    Lena J Daumann
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, QLD 4072, Australia
    Dalton Trans 43:910-28. 2014
    ..This review summarises some of our work and illustrates the significance and contributions of model studies to knowledge in the area. ..
  38. doi request reprint Bacterial and plant ketol-acid reductoisomerases have different mechanisms of induced fit during the catalytic cycle
    Sze Ho Wong
    School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Queensland 4072, Australia
    J Mol Biol 424:168-79. 2012
    ..Support is thereby provided for the idea that plant and bacterial KARIs have evolved different mechanisms of induced fit to prepare the active site for catalysis...
  39. doi request reprint Improving a natural enzyme activity through incorporation of unnatural amino acids
    Isaac N Ugwumba
    Commonwealth Scientific and Industrial Research Organization, Black Mountain, Canberra, Australia
    J Am Chem Soc 133:326-33. 2011
    ..These results demonstrate that designer amino acids provide easy access to new and valuable sequence and functional space for the engineering and evolution of existing enzyme functions...
  40. pmc Anomalous scattering analysis of Agrobacterium radiobacter phosphotriesterase: the prominent role of iron in the heterobinuclear active site
    Colin J Jackson
    Research School of Chemistry, Building 35, Australian National University, Canberra, ACT 0200, Australia
    Biochem J 397:501-8. 2006
    ..These results suggest an essential role for iron in the catalytic mechanism of bacterial phosphotriesterases, and that these phosphotriesterases are natively heterobinuclear iron-zinc enzymes...
  41. pmc Malonate-bound structure of the glycerophosphodiesterase from Enterobacter aerogenes (GpdQ) and characterization of the native Fe2+ metal-ion preference
    Colin J Jackson
    Research School of Chemistry, Australian National University, Australia
    Acta Crystallogr Sect F Struct Biol Cryst Commun 64:681-5. 2008
    ..Catalytic implications of the structure and its Fe2+ metal-ion preference are discussed...
  42. ncbi request reprint Reactivity of M(II) metal-substituted derivatives of pig purple acid phosphatase (uteroferrin) with phosphate
    Mark B Twitchett
    Department of Chemistry, University of Newcastle, Newcastle upon Tyne NE1 7RU, U K
    Inorg Chem 41:5787-94. 2002
    ..8 and independent of M(II) (Fe(II), Zn(II), Mn(II)). The acid dissociation process is assigned to Fe(III)-OH(2) to Fe(III)-OH(-), where OH(-) is less readily displaced by phosphate...
  43. ncbi request reprint A new heterobinuclear FeIIICuII complex with a single terminal FeIII-O(phenolate) bond. Relevance to purple acid phosphatases and nucleases
    Mauricio Lanznaster
    LABINC Laboratório de Bioinorgânica e Cristalografia, Departamento de Quimica, Universidade Federal de Santa Catarina, Campus Trindade, 88040 900 Florianopolis, SC, Brazil
    J Biol Inorg Chem 10:319-32. 2005
    ..5 microM), under physiological conditions (optimum pH of 7.0), with a rate enhancement of 2.7 x 10(7) over the uncatalyzed reaction. Thus, 1 is one of the most effective model complexes to date, mimicking the function of nucleases...
  44. ncbi request reprint Diesterase activity and substrate binding in purple acid phosphatases
    Robynn S Cox
    Department of Chemistry and Biochemistry, Utah State University, Logan, Utah 84322 0300, USA
    J Am Chem Soc 129:9550-1. 2007
  45. pmc Kinetic and spectroscopic studies of N694C lipoxygenase: a probe of the substrate activation mechanism of a nonheme ferric enzyme
    Michael L Neidig
    Department of Chemistry, Stanford University, Stanford, California 94305, USA
    J Am Chem Soc 129:7531-7. 2007
    ....
  46. ncbi request reprint Spectroscopic characterization of soybean lipoxygenase-1 mutants: the role of second coordination sphere residues in the regulation of enzyme activity
    Gerhard Schenk
    Department of Chemistry, Stanford University, California 94305 5080, USA
    Biochemistry 42:7294-302. 2003
    ..We propose that the H-bond between the weak Asn694 ligand and the Gln697 plays a key role in the modulation of the coordination flexibility of Asn694, and thus, is crucial for the regulation of enzyme reactivity...
  47. ncbi request reprint Comparison between the geometric and electronic structures and reactivities of [FeNO]7 and [FeO2]8 complexes: a density functional theory study
    Gerhard Schenk
    Department of Chemistry, Stanford University, Stanford, California 94305 5080, USA
    J Am Chem Soc 126:505-15. 2004
    ..Although NO is, in fact, harder to reduce, the resultant NO(-) species forms a more stable bond to Fe(III) relative to O(2)(-) due to the different bonding interactions...
  48. ncbi request reprint Using directed evolution to improve the solubility of the C-terminal domain of Escherichia coli aminopeptidase P. Implications for metal binding and protein stability
    Jian Wei Liu
    Research School of Chemistry, Australian National University, Canberra, Australia
    FEBS J 274:4742-51. 2007
    ..In this case, directed evolution has identified active site residues that destabilize the domain structure...
  49. ncbi request reprint An unprecedented Fe(III)(mu-OH)Zn(II) complex that mimics the structural and functional properties of purple acid phosphatases
    Ademir Neves
    LABINC, Departamento de Quimica, Universidade Federal de Santa Catarina, 88040 900 Florianopolis, SC, Brazil
    J Am Chem Soc 129:7486-7. 2007
  50. ncbi request reprint Rapid-freeze-quench magnetic circular dichroism of intermediate X in ribonucleotide reductase: new structural insight
    Natasa Mitic
    Department of Chemistry, Stanford University, 333 Campus Street, Stanford, California 94305, USA
    J Am Chem Soc 125:11200-1. 2003
    ....