GRP78 Selective Inhibitors From a Direct‐to‐Biology Strategy

X Xiaoyi Zhu C Carlee A. Trindl (College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA) Q Qiu Li H Haofeng Ye (Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA) L Lewis Alexander (College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA) D Dichun Huang (Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA) Y Yongyi Wei (Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA) V Vyana Trieu (College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA) B Ben N. Stansfield (Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA) A Aikseng Ooi (Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA) Y Yang Yang‐Hartwich (Department of Obstetrics Gynecology, and Reproductive Sciences Yale School of Medicine New Haven Connecticut USA) D Donna D. Zhang E Eli Chapman (College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA)

Abstract

ABSTRACT Because cancer cells have heightened protein homeostasis (proteostasis) requirements, there is interest in targeting proteostasis machinery, including the 70 kDa heat shock proteins (HSP70s), as potential cancer therapeutics. However, studies have shown that the HSP70 family is differentially regulated across cancers, and global targeting may produce unwanted toxicities. For this reason, our lab has focused on isoform‐selective targeting of HSP70s, including the endoplasmic reticulum‐resident HSP70, GRP78 (HSPA5 or BiP). GRP78 is a central component of protein homeostasis in the secretory system and is the principal regulator of the unfolded protein response (UPR). Here, we report the use of a direct‐to‐biology (D2B) strategy to optimize a dipeptide‐based scaffold that binds selectively to GRP78, relative to the other canonical HSP70s. We show that our lead compound, 12 , potently and selectively inhibits GRP78, binds to the substrate binding pocket, kills A549 lung cancer cells in 2D (grown as a monolayer) and 3D (grown as spheroids) cultures, engages GRP78 in cells, and that GRP78 inhibition is responsible for the mode of action. This work represents the first GRP78‐selective inhibitor that inhibits substrate binding.

Article Details

Volume / Issue Vol. 65, Issue 24
Published June 08, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

X

Xiaoyi Zhu

C

Carlee A. Trindl

College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA

Q

Qiu Li

H

Haofeng Ye

Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA

L

Lewis Alexander

College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA

D

Dichun Huang

Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA

Y

Yongyi Wei

Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA

V

Vyana Trieu

College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA

B

Ben N. Stansfield

Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA

A

Aikseng Ooi

Department of Molecular Medicine Center For Inflammation Science and Systems Medicine UF Scripps Institute For Biomedical Innovation and Technology Jupiter Florida USA

Y

Yang Yang‐Hartwich

Department of Obstetrics Gynecology, and Reproductive Sciences Yale School of Medicine New Haven Connecticut USA

D

Donna D. Zhang

E

Eli Chapman

College of Medicine Department of Pharmacology and Therapeutics Center For Inflammation Science and Systems Medicine The Herbert Wertheim UF Scripps Institute For Biomedical Innovation and Technology University of Florida Jupiter Florida USA