Author ORCID Identifier

0000-0002-1114-227X.

Defense Date

2026

Document Type

Dissertation

Degree Name

Doctor of Philosophy

Department

Pharmaceutical Sciences

First Advisor

Shijun Zhang

Abstract

NLRP3 inflammasomes are intracellular multiprotein complexes that regulate the maturation of interleukin-1β (IL-1β) and interleukin-18 (IL-18) and promote gasdermin D (GSDMD)-mediated pyroptosis. Although NLRP3 inflammasome activation protects against infection and cellular injury, persistent NLRP3/GSDMD signaling contributes to chronic inflammatory and neurodegenerative diseases. This work aimed to develop small-molecule inhibitors targeting the NLRP3 inflammasome pathway.

Starting from the glyburide-derived inhibitor JC124, structure-activity relationship studies were conducted on two lead scaffolds, YM8 and YM109. The YM8 scaffold showed limited tolerance to structural modification, whereas YM109 accommodated broader substitutions within the phenyl ring, alkoxy side chain, and tertiary amine moieties. These studies identified compounds 34, 54, and 65 as potent NLRP3 inhibitors. Compound 65 demonstrated the strongest overall profile, including potent cellular activity, improved selectivity, favorable physicochemical properties, direct NLRP3 target engagement, and suppression of LPS-induced inflammatory cytokine production in mice.

In parallel, an in-house compound library was screened to identify inhibitors of GSDMD-mediated pyroptosis. YM81 inhibited IL-1β release across NLRP3, AIM2, and NLRC4 inflammasome pathways. Mechanistic studies showed that YM81 reduced GSDMD cleavage, membrane permeabilization, LDH and HMGB1 release, and propidium iodide uptake. Biophysical studies confirmed direct nanomolar-affinity binding to GSDMD. YM81 also reduced hepatic injury and inflammation in a mouse model of acetaminophen-induced acute liver injury.

Collectively, compound 65 and YM81 represent promising inhibitors of NLRP3 and GSDMD, respectively, and support further therapeutic development for inflammasome-associated diseases.

Rights

© Jannatun Nayem Namme

Is Part Of

VCU University Archives

Is Part Of

VCU Theses and Dissertations

Date of Submission

7-30-2026

Available for download on Tuesday, July 29, 2031

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