인공 핵산분해효소로서 수화된 전이금속 착 화합물에 의한 DNA분자의 가수분해에 대한 전산화학적인 접근
A Computational Chemistry Approach for the Hydrolysis of DNA Molecule by Hydrated Transition Metal Complexes as Artificial Metallonuclease
2
조회
0
다운로드
2
인용
0
참고문헌
키워드
초록
인공 핵산분해효소로 작용하는 10종의 수화된 단일 리간드 전이금속 착 화합물([M(H2O)6]z+ 및 [M(OH)6]z-)과 DNA분자의 해리반응(pKa)전 후 조건에서, 전산화학적인 경계분자궤도(FMO) 이론에 따른 이들 화합물의 반응성을 정량적으로 검토하였다. 그리고 분자 간 FMO에너지 차이(△E)로부터, Lewis acid 촉매로서 금속 착 화합물의 친핵성 리간드 활성화(A)에 따른 궤도조절(orbital control) 반응과 금속 착 화합물의 활성화(B)로 인한 전하조절(charge control) 반응이 각각 예측되었다. 모든 경우에 반응성은 물 분자 리간드 금속 착 화합물([M(H2O)6]z+)보다 hydroxo 리간드 금속 착 화합물([M(OH)6]z-)이 높았으며, 그리고 2가 화합물([M(H2O)6]2+ 및 [M(OH)6]4-)이 3가 화합물([M(H2O)6]3+ 및 [M(OH)6]3-)보다 빠른 반응성을 나타내었다. 이들의 반응성은 주로 [M(OH)6]z-과 해리 후 DNA분자 사이의 음 이온성 반발력이나 착 이온의 입체효과와 전하크기에 의존적이었다. 그러므로 이 같은 리간드 효과로부터 가장 빠른 반응조건에서(6M) HOMO에너지에 의존적인 주 반응(A)에 따른 [M(OH)6]z-에 의한 DNA 분자의 가수분해 전환과정(turnover process)을 제시하였다.
Abstract
The acting as artificial metallonucleases under the condition at before and after dissociation (pKa) of DNA molecule and 10 hydrated homoleptic transition metal complexes ([M(H2O)6]z+ & [M(OH)6]z-) are reviewed quantitatively based on the frontier molecule orbital (FMO) theory in computational chemistry. In additions, from the FMO energy difference (△E) between the complexes and DNA molecule, the orbital control reaction by nucleophilic ligand activation (A) of the metal complexes as Lewis acid catalyst, and the charge control reaction by activation (B) of the metal complexes are predicted, respectively. Hence, the reactivity of [M(OH)6]z- was higher than that of [M(H2O)6]z+ in all cases. Moreover, divalent ([M(H2O)6]2+ and [M(OH)6]4-) show rapid responses comparing to the trivalent compounds ([M(H2O)6]3+ and [M(OH)6]3-). Their reactivity was mainly dependent on the anionic repulsive force between hydroxo ligand metal complex and dissociated DNA molecule, or steric effect and charge size of complexe ions. Therefore, from these results of ligand effect, the turnover process on the hydrolytic decomposition of contaminated DNA molecule by homoleptic hydroxo metal complexes ([M(OH)6]z-) in the fastest reaction condition (6M) was proposed as the major reaction (A) depend upon the HOMO energy.
참고문헌 (41)
- NT Lappas, "Quality Assurance and Quality Control", pp.77~94 (2016), Elsevier
- RA Wickenheiser, "Trace DNA: A review, disscussion of theory, and application of the transfer of trace quantities of DNA through skin contact", J Forensic Sci, 38(2), pp.442~450 (2003)
- RAH van Oorschot, "Forensic trace DNA: A review", Investig Genet, 1, pp.14~ (2010)
- L Ragle, "Crime Scene: From Fingerprints to DNA Testing-Astonishing Inside Look at the Real World of CSI" (2002), Avon Books
- 최미정, "총설: DNA 감식에 미치는 잠재지문 현출시약들에 의한 금속이온과유기용매의 영향", 과학수사학회지, 11(1), pp.1~17 (2017), 한국과학수사학회[DOI]
- 홍주은, "이중성 지문시약으로서 Ruhemann’s Purple 화합물과 그 금속이온착 화합물의 생성 반응성 및 DNA분자 보호 가능성", 과학수사학회지, 12(2), pp.69~79 (2018), 한국과학수사학회[DOI]
- 나윤주, "DNA 분자를 보호할 수 있는 HFE-7100 용매 유사체들의 유기금속 착 화합물 생성 반응성", 과학수사학회지, 12(4), pp.217~227 (2018), 한국과학수사학회[DOI]
- 윤신규, "형광단-아미노산 생성물과 그의 전이금속 착 화합물에 의한 잠재지문 현출성 및 DNA분자 보호 가능성", 과학수사학회지, 13(1), pp.1~10 (2019), 한국과학수사학회[DOI]
- R Murugavel, "Metal complexes of Organophosphate Esters and Open-Framework Metal Phosphates : Synthesis, Structure, Transformations, and Applications", Chem Rev, 108, pp.3549~3655 (2008)
- TA Brettell, "Review; Forensic Science", Anal Chem, 75(12), pp.2877~2890 (2003)
- P Kanokwongnuwut, "Detection of latent DNA", Forensic Sci Int; Genet, 37, pp.95~101 (2018)
- AM Haines, "Finding DNA:Using fluorescent in situ detection", Forensic Sci Int Genet. Suppl Ser, 5, pp.e501~e502 (2015)
- D Sero, "Facial recognition from DNA using face-to-DNA classifiers", Nature Communications, 10(1), pp.2557~ (2019)
- 서희진, "Forensic DNA Phenotyping: A Review in Korean Perspective", 대한법의학회지, 41(2), pp.23~31 (2017), 대한법의학회
- DJ Stevens, "In Media and Criminal Justice:The CSI Effect", pp.157~196 (2011), Jones and Bartlett Pub, LLC
- KN Ballantyne, "DNA Contamination minimisation-Finding an Effective cleaning method", Australian J Forensic Sci, 47(4), pp.1~12 (2015)
- 성낙도, "과학수사 증거물에 대한 신규 오염방지제의 이화학적 조성물", 특허출원, ~ (2020)
- F Mancin, "Progress in Artificial Metallo nucleases", Chem Commun, 48, pp.5545~5559 (2012)
- I Persson, "Hydrated metal ions in aqueous solution; How regular are their structure?", Pure Appl Chem, 82(10), pp.1901~1917 (2010)
- LG Zhuo, "A frontier molecular orbital theory approach to understanding the Mayr equation and to quantifying nucleophilicity and electrophilicity by using HOMO and LUMO energies", Asian J Org Chem, 1, pp.336~345 (2012)
- M Zhu, "Quantum Chemical Studies of Mononuclear Zinc Species of Hydration and Hydrolysis", J Phys Chem A, 109, pp.7648~7652 (2005)
- RG Bergman, "Synthesis and reactions of monomeric late transition metal alkoxo, aryloxo and hydroxo complexes", Polyhedron, 14(22), pp.3227~3237 (1995)
- S Grimme, "Semiempirical hybrid density functional with perturbative second-order correlation", J Chem Phys, 124(3), pp.034108~ (2006)[DOI]
- SS Batsanov, "Van der Waals Radii of Elements", Inorganic Materials, 37(9), pp.871~885 (2001)
- VE Jackson, "Prediction of the pKa’s of aqueous metal ion +2complexes", J Phys Chem A, 119(2), pp.2926~2939 (2015)
- S Kobayashi, "Lewis acid catalysis stable in Water. Correlation between catalytic activity in water and hydrolysis constants and exchange rate constants for substitution of inner-sphere water ligands", J Am Chem Soc, 120, pp.8287~8288 (1988)
- W Grzybkpwski, "Nature and properties of metal cations in aqueous solutions", Polish J of Environ Stud, 15(4), pp.655~663 (2006)
- B Schneider, "Hydration of the phosphate group in double-helical DNA", Biophys J, 75(5), pp.2422~2434 (1998)
- T Theophanides, "The effects of metal ion contaminants on the double stranded DNA helix and diseases", J Environ Sci Health, Part A, 52(10), pp.1030~1040 (2017)
- A Erxleben, "Mechanistic Studies of Homoand Heterodinuclear Znic Phosphoesterase Mimics:What Has Been Learned?", Front Chem, 7, pp.21~ (2019)
- KRS Gowda, "Mechanism of DNA binding and cleavage", Biomed & Biotechnol, 2(1), pp.1~9 (2014)
- KS Gates, "An Overview of Chemical Processes That Damage Cellular DNA : Spontaneous Hydrolysis, Alkylation, and Reactions with Radicals", Chem Res Toxicol, 22(11), pp.1747~1760 (2009)
- 김나진, "과학수사 증거물의 연속성(Chain of Custody)을 유지하기 위한 몇 가지 구체적인 대응방안", 박사, pp.2020
- I Fleming, "Frontier Orbitals and Organic Chemical Reactions", pp.35~37 (1976), John Wiley & Sons
- FH Westheimer, "Pseudo-rotation in the hydrolysis of phosphate esters", Acc Chem Res, 1(3), pp.70~78 (1968)
- NH Williams, "Artificial Nucleases", pp.3~17 (2018), Springer
- JS Seo, "Structure and rectivity of dinuclear cobalt(III)with peroxide and phosphodiester analogues bridging metal ions", J Am Chem Soc, 120, pp.9943~9944 (1996)
- F Mancin, "Metal Complex-DNA Interactions", pp.369~394 (2009), Wiley
- G Palermo, "Catalytic Metal Ions and Enzymatic Processing of DNA and RNA", Acc Chem Res, 48(2), pp.220~228 (2015)