(H2 O)Zn(Imidazole)n ]2+ : the vital roles of coordination number and geometry in Zn-OH2 acidity and catalytic hydrolysis

Physical Chemistry Chemical Physics : PCCP
Douglas P LinderKenton R Rodgers

Abstract

The Zn(ii)-(Imidazole(ate))n coordination motif occurs in numerous biochemical systems, including carbonic anhydrase and the matrix metalloproteinases (MMPs). Additionally, it has been used in synthetic materials, such as the zinc-based zeolitic imidazolate framework (ZIF) structures. Zinc centers in these systems typically act as Lewis acids that form complexes with small molecules, such as H2O, which is activated catalytically toward a number of important and useful hydrolysis reactions. The results reported herein from density functional theory (M05-2X) and ab initio (MP2 and CCSD(T)) calculations demonstrate that both the coordination number and the molecular geometry have a sizable impact on the binding strength, deprotonation energy, and acidity of the Zn(ii) coordinated water. Through a series of quantum mechanical calculations on [(ImH)nZn-OH2]2+ complexes (n = 1-5), both the solution-phase pKa and the gas-phase proton dissociation energy significantly increase as n increases. While this should not be too surprising, the Zn-OH2 bond dissociation energies and bond lengths don't necessarily undergo a concurrent decrease, and therefore would be of limited use as a prediction tool regarding Zn-OH2 acidity. In an effort to d...Continue Reading

References

Mar 30, 2001·The Journal of Biological Chemistry·S J KridelJ W Smith
Feb 8, 2002·Biometals : an International Journal on the Role of Metal Ions in Biology, Biochemistry, and Medicine·D S Auld
Oct 29, 2002·Inorganic Chemistry·Vladimir Pelmenschikov, Per E M Siegbahn
Jan 14, 2003·Nature Structural Biology·Oded KleifeldIrit Sagi
Dec 22, 2004·The Journal of Biological Chemistry·Daniela JozicKlaus Maskos
Jan 7, 2006·Journal of Proteome Research·Claudia AndreiniAntonio Rosato
Jun 24, 2008·The Journal of Physical Chemistry. B·Natalia Díaz, Dimas Suárez
Sep 5, 2009·Chemical Reviews·Wolfgang Maret, Yuan Li
Sep 23, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·Sérgio Filipe SousaMaria João Ramos
Nov 3, 2009·Accounts of Chemical Research·Anh PhanOmar M Yaghi
Mar 25, 2010·The Journal of Chemical Physics·Giovanni Scalmani, Michael J Frisch
May 17, 2011·Physical Chemistry Chemical Physics : PCCP·A P Harding, P L A Popelier
Jul 16, 2013·Oral Diseases·G SapnaK Bagri-Manjrekar
Sep 26, 2013·Inorganic Chemistry·Mikko LaitaojaJanne Jänis
Feb 11, 2014·Biochemistry·Melissa L Zastrow, Vincent L Pecoraro
Oct 21, 2014·Metallomics : Integrated Biometal Science·A Gerard Daniel, Nicholas P Farrell
Nov 11, 2014·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Ibon Alkorta, Paul L A Popelier
Nov 22, 2014·Nature Reviews. Molecular Cell Biology·Caroline BonnansZena Werb
Jul 2, 2015·Journal of Computational Chemistry·Tatiana VasilevskayaWalter Thiel
Nov 20, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·J CanivetD Farrusseng
Sep 10, 2013·Journal of Chemical Theory and Computation·Eve ToomsaluPeeter Burk
Nov 26, 2015·Proceedings of the National Academy of Sciences of the United States of America·Ming GaoMayland Chang
Aug 11, 2017·Chemical Society Reviews·Russell E Morris, Lee Brammer

❮ Previous
Next ❯

Citations

Apr 10, 2020·Physical Chemistry Chemical Physics : PCCP·Jingxian YuAndrew D Abell
Jun 28, 2019·The Journal of Physical Chemistry. a·Rahma DahmaniMajdi Hochlaf

❮ Previous
Next ❯

Methods Mentioned

BETA
X-ray
NMR

Software Mentioned

Gaussian
M05

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.