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October 02, 2007

Structural Biology and Structure-based Drug Design

On 16 October 2007 we will hold an eCheminfo Community of Practice conference session at Bryn Mawr College, Philadelphia to discuss latest advances in structural biology related to drug discovery. The session will be chaired by Max Cummings (Tibotec Pharmaceuticals) and includes a knowledgeable panel of speakers and discussion leaders: Charles Lesburg (Schering-Plough), Heather Carlson (University of Michigan), Gerard Kleywegt (University of Uppsala), Paul Labute (CCG), Alan Cheng (Amgen), and Ajay Jain (UCSF). A description of the session with presentation abstracts follows:

Structural Biology
http://echeminfo.com/COMTY_conferencesprog07structbio

Structural biology efforts bring the 3D structures of proteins to light, and thereby greatly enable many drug discovery efforts. In the affinity optimization phase of a medicinal chemistry effort the timely determination of the 3D structure of a relevant protein-ligand complex can have a huge positive impact. At the same time it is important to note that a wide range of structural information can be useful in guiding drug design efforts - from a single lowly 2D ligand structure to a set of high resolution 3D structures of protein-ligand complexes.

Talks in this session cover different topics in the areas of structural biology and/or structure-based drug design. Ligand structures and their known activities can help to predict side effects, as well as possible new uses for known drugs. How reliable is a given 3D protein structure, and how can users evaluate this for themselves? Positioning of hydrogen atoms for biomolecular calculations is a longstanding issue, and a new approach to solving this problem is presented. Aspects of the recently popular concept of druggability are explored by two of the speakers. Protein flexibility is discussed in the context of protein-ligand structures related to the regulation of drug metabolism. Attendees will be exposed to various ways in which structural information is used in drug design, and should gain an appreciation for a few currently emerging challenges in the fields of structural biology and structure-based drug design.

(Please follow continuation to read abstracts of sessions talks.)

Abstracts

Engineered Constitutively Active PXR Ligand Binding Domain for Inverse Structure-Based Drug Design or A Tale of Two Conformations
Charles Lesburg, Schering-Plough

The pregnane X receptor (PXR) is responsible for upregulating cytochrome P450 expression in response to a wide variety of xenobiotics. This induction of metabolism negatively impacts drug exposure and forms the basis for detrimental drug-drug interactions. We have engineered a constitutively-active PXR ligand binding domain and demonstrated that it is capable of binding known PXR ligands. Moreover, we used this construct in an inverse structure-assisted drug design effort to understand the structural basis of ligand binding to PXR. During this analysis, we were presented with unexpected binding modes which underscore the plasticity of the PXR ligand binding pocket.

Fundamental differences between high- and low-affinity complexes of enzymes and non-enzymes
Heather A. Carlson, University of Michigan

Stark differences between enzymes and non-enzymes were found through mining the protein-ligand database, Binding MOAD (Mother of All Databases, pronounced "mode" as a pun on the ligand's mode of binding to its protein target). Ligand efficiencies were found to be much higher in non-enzymes. Every atom, every square Ångstrom of contact gives more free energy in non-enzymatic binding sites. This implies they may be more "druggable" targets than enzymes because drug-like affinities can be obtained with smaller molecules which are more easily absorbed and have less functional groups for potential toxicity concerns. Additional data also suggest that divergent approaches may be needed to improve the affinity of ligands for the two classes of proteins. High-affinity ligands are much larger than low-affinity ligands for enzyme complexes. The addition of complementary functional groups is likely to improve the affinity of an enzyme inhibitor through more contact with the pocket, but this process may not be as fruitful for ligands of non-enzymes. High- and low-affinity inhibitors are the same size in non-enzymes. The inherent differences between enzymes and non-enzymes have significant ramifications for scoring functions and structure-based drug design.

Protein crystallography: not as simple as ABC then?
Gerard J Kleywegt, Uppsala University, Uppsala, Sweden

The recent debacle with the ABC transporter structures has shown (not for the first time, unfortunately - and probably not for the last time either) that the mere fact that a pretty crystal structure is reported in the pages of a glossy journal does not guarantee that the structure is even close to being correct. Some of the causes of serious errors in biomacromolecular crystal structures will be discussed. In addition, a few examples of such errors will be given, and simple ways in which non-experts can assess the overall reliability of a protein crystal structure will be discussed. However, even when the overall structure is reliable, this is not necessarily true for each and every detail. Particularly relevant in this respect are the protein residues that interact with substrates or inhibitors and the interacting molecules themselves. A few examples will be used to demonstrate that the structures of ligands etc. are often less reliable than those of their proteinaceous hosts.

Obviously, for users of protein structures these observations have important implications. First and foremost, crystal structures should be treated with healthy scepticism rather than reverence. The best way to assess the reliability of critical aspects of a structure (ligands, active-site residues, metal-binding sites, interface residues, etc.) is to inspect the experimental electron density maps. Our efforts to provide such maps, and information derived from them, for all crystal structures for which structure factors have been deposited with the wwPDB will be discussed. They have resulted in EDS - the Uppsala Electron Density Server (http://eds.bmc.uu.se/).

Assignment of Protonation States and Geometries to Macromolecular Structures using Unary Quadratic Optimization
Paul Labute, CCG

Many computational methodologies relating to macromolecular structures depend significantly on the assigment of protonation states and proton coordinates. The complexity of hydrogen bond networks, tautomers, ionization states and metal ligands often make automated protonation assignment quite difficult. A method based upon Unary Quadratic Optiimization is presented to address this problem. The algorithm and theormodynamic theory is described along with some validation results on high resolution crystal structures.


Structure-based prediction of small-molecule druggability
Alan C. Cheng, Amgen

Over half of drug discovery efforts fail in lead identification or in optimization of leads for drug-like properties. We set out to reduce the failure rate by identifying the more druggable targets early on, and discovered that a model based on basic biophysical principles does this very well. The basic idea is to quantitatively estimate the maximal affinity achievable at a given binding site by a small molecule with certain ‘drug-like’ properties. These estimates turn out to correlate reasonably well with drug discovery outcomes and are useful in the prioritization of small-molecule drug targets. Computer-aided approaches that have potential in tackling difficult druggability targets will also be presented.

Drug Target Modeling: Ligands Tell Us More Than We Think
Ajay N. Jain, Ph.D., Professor, Cancer Research Institute and Depts. of Biopharmaceutical Sciences and Laboratory Medicine; Director, Informatics Core, UCSF Cancer Center

There are just over 1000 small molecule therapeutics approved for human use in the United States. Systematic annotation of their primary targets reveals that over 700 of these modulate approximately 85 biological targets. The results of multiple analyses, based exclusively on ligand-focused modeling, will be discussed. Drug/drug similarities and target/target similarities were computed on the basis of three-dimensional ligand structures. Drug pairs sharing a target had significantly higher similarity than drug pairs sharing no target. Also, target pairs with no overlap in annotated drug specificity shared lower similarity than target pairs with increasing overlap. Clustering analysis suggested that side effects and drug-drug interactions might be revealed by modeling many targets. Ligand-based models of diverse targets were constructed and tested in virtual screening protocols. Excellent enrichment was possible against backgrounds of screening molecules. More interesting, however, was that by crossing all drugs against all targets, it becomes possible to identify a number of known side effects, drug specificities, and drug-drug interactions that have a rational basis in molecular structure.
 

 

Barry Hardy
eCheminfo Community of Practice

 

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