Note for: PARP1 Inhibitors: antitumor drug design_2014

Note for: PARP1 Inhibitors: antitumor drug design_2014

PMID: 26483957

Overview

PARP1

-       common nuclear protein (1-2 million molecules/cells)

-       sensor for DNA strand breaks

-       highly expression of PARP1 can be found in some cancers, treatment-resistance of tumors

-       act as chemotherapy and radio-sensitizer

-       focus on properties and feature of PARP1 inhibitors: clinical and preclinical levels

-       discuss on problems -- > application of PARP1 inhibitors, possibility of developing new PARP1 inhibitors -- > aim at DNA binding and transcriptional activity rather than catalytic domain

Introduction

-       DNA break

o   PARP1 recognize through Zn-finger

o   Transferring ADP-ribose to related protein as well as PARP1

§  Downstream effect

·         Chromatin decondensation

o   Removing H1 linker histone

·         Recruiting repair enzyme

-       Three levels of damage

o   Mild damage -- > activation of PARP1 -- > DNA repair

o   Stronger damage -- > PARP1 -- > apoptosis

o   More extensive damage -- > overreaction of PARP1 -- > cell necrosis

-       PARP1 and carcinogenesis (pro-tumor activites)

o   Loss

§  Interfere with DNA repair -- > genome shuffling and chromosomal abnormalities -- > more mutagenesis

§  Inhibiting transcription of genes related to DNA replication and cell cycle regulation

-       PARP1 and cancer state

o   Gain

§  Prognosis -- > poor survival

§  More aggressive phenotype in breast cancers

§  Tumor resistance to therapy

·         Facilitating damaged DNA repair -- > improving genetic instability -- > characteristic of transformed cells

History of PARP1 inhibitor design


-       PARP1 used to enhance conventional therapy

o   Chemosensitizer

o   Radiosensitizer

-       First generation of PARP1 inhibitors

o   Nicotinamide analogues

§  Develop ~35 years ago (count up to 2020)

§  Based on observation -- > nicotinamide (reaction’s product) -- > show moderate inhibition

§  Benzamide -- > ineffective in practice

·         Cell culture -- > used as mM concentration

·         Non-specific action

·         Based line for further PARP1 development

o   Nicotinamide/benzamide -- > pharmacophore group

o   3AB

 

-       Second generation of PARP1 inhibitor is develop based on quinazoline analogues

o   More effective and target specific

o   PJ-34 -- > further used in clinical trials

o   Crystal structure reveals carboxamide group forms several hydrogen bonds with Ser904-OG and Gly863-N in catalytic domain of PARP1 -- > improve interaction between heterocycle of 2nd inhibitor + PARP1


  

o   Significance of aromatic w-w interaction between phenolic gr. of PARP1 inhibitor + phenolic gr. of Tyr907

o   Crucial interactions which support specificity -- > hydrogen bond with Gly863, Ser904 and Glu988

-       Third generation of PARP1 inhibitor

o   Benzimidazole-based PARP1 inhibitor -- > 3rd gen








Mode of mechanism

-       PARP1 inhibition -- > failure of DNA repair

-       PARP1 binds to both SSB and DSB

-       Control several DNA repair pws

o   BER

o   NER

o   MMR

o   HR and NHEJ


HR defective which may contribute to PARP sensitivity

-       Mutation of BRCA1/2

o   Other genes in HR

§  RAD51

§  DSS1

§  RPA1

§  CHK1

-       PARP remains bound to damaged DNA -- > by the action of inhibitor

-       Make it as obstacle for PARP-dependent repair enzymes or BRCA1 to be recruited and fix the break

-       In HR defect cell, DSB -- > fix by NHEJ -- > NHEJ is controlled by PARP1 through ADP-ribosylation on Ku70/80, DNAPK

o   Prognostic markers; mutation of

§  RAD51

§  NBS1

§  ATM

§  ATR

§  Chk1

§  Chk2

§  Rad54

§  FANCD2

§  FANCA

§  53BP1

§  PALB2

§  FANCC

§  PTEN

PARP1+DNA methylation agents

-       DNA-methylating agents – dacarbazine (DTIC), temozolomide (TMZ)

PARP1+TOPOI

-       Repair of TopoI-induced damage involves BER/SSB.

-       Thus, cell lacking key BER (i.e., XECC1) -- > hypersensitive to camptothecin

-       PARP1 helps recruiting XRCC1 to TopoI-dependent DNA break -- > recruit TDP1 -- > remove TopoI from DNA

-       PARP1 can interact with Topo-I -- > repairing TopoI-dependent SSB

PARP1+Radiotherapy

-       Relied on the hypothesis -- > accumulation of SSB by PARPi -- > causing more DSB during S-phase

Prospective for new inhibitory discovery

Problems

-       Compounds inhibiting NAD+ binding -- > low specificity for PARP1 -- > blocking enzymatic pw. relating to NAD+ (which is cofactor and relates to many cellular process, thus creating higher toxicity)

-       Enzymatic PARP1 inhibitors -- > activate viral replication -- > thus this drug cannot use with patients infected with viruses, ex. Human T-cell lymphotropic virus or Kaposi’s sarcoma-associated herpes virus

-       Long-term administration of PARP1 -- > still in question on the side effects -- > example of toxicity -- > iniparib (BSI-201)

-       Since PARP1 has many functional domains -- > DNA-binding domain as well as transcriptional regulation have been proposed for another drug design

o   DNA binding domain inhibitor has been recently developed

 

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