Department of Pharmaceutical Sciences, School of Pharmacy, University of Colorado Denver, 12700 East 19th Avenue, Box C238 P-15, Research 2, Aurora, Colorado 80045, USA.
Chem Res Toxicol. 2010 Jun 21;23(6):1034-44. doi: 10.1021/tx100038b.
Effective medical treatment and preventive measures for chemical warfare agent sulfur mustard (HD)-caused incapacitating skin toxicity are lacking, because of limited knowledge of its mechanism of action. The proliferating basal epidermal cells are primary major sites of attack during HD-caused skin injury. Therefore, employing mouse JB6 and human HaCaT epidermal cells, here, we investigated the molecular mechanism of HD analogue 2-chloroethyl ethyl sulfide (CEES)-induced skin cytotoxicity. As compared to the control, up to 1 mM CEES treatment of these cells for 2, 4, and 24 h caused dose-dependent decreases in cell viability and proliferation as measured by DNA synthesis, together with S and G2-M phase arrest in cell cycle progression. Mechanistic studies showed phosphorylation of DNA damage sensors and checkpoint kinases, ataxia telangiectasia-mutated (ATM) at ser1981 and ataxia telangiectasia-Rad3-related (ATR) at ser428 within 30 min of CEES exposure, and modulation of S and G2-M phase-associated cell cycle regulatory proteins, which are downstream targets of ATM and ATR kinases. Hoechst-propidium iodide staining demonstrated that CEES-induced cell death was both necrotic and apoptotic in nature, and the latter was induced at 4 and 24 h of CEES treatment in HaCaT and JB6 cells, respectively. An increase in caspase-3 activity and both caspase-3 and poly(ADP-ribose)polymerase (PARP) cleavage coinciding with CEES-caused apoptosis in both cell lines suggested the involvement of the caspase pathway. Together, our findings suggest a DNA-damaging effect of CEES that activates ATM/ATR cell cycle checkpoint signaling as well as caspase-PARP pathways, leading to cell cycle arrest and apoptosis/necrosis in both JB6 and HaCaT cells. The identified molecular targets, quantitative biomarkers, and epidermal cell models in this study have the potential and usefulness in rapid development of effective prophylactic and therapeutic interventions against HD-induced skin toxicity.
有效治疗和预防化学战剂芥子气(HD)引起的使人丧失能力的皮肤毒性的方法仍然缺乏,这是因为对其作用机制的了解有限。增殖的基底表皮细胞是 HD 引起皮肤损伤时的主要攻击部位。因此,在这里,我们使用小鼠 JB6 和人 HaCaT 表皮细胞研究了 HD 类似物 2-氯乙基乙基硫醚(CEES)诱导的皮肤细胞毒性的分子机制。与对照相比,高达 1mM 的 CEES 处理这些细胞 2、4 和 24 小时会导致细胞活力和增殖呈剂量依赖性下降,如 DNA 合成所示,同时细胞周期进程中的 S 和 G2-M 期停滞。机制研究表明,CEES 暴露后 30 分钟内,DNA 损伤传感器和检查点激酶的磷酸化,包括 ataxia telangiectasia-mutated (ATM) 在丝氨酸 1981 位点和 ataxia telangiectasia-Rad3-related (ATR) 在丝氨酸 428 位点,以及 S 和 G2-M 期相关的细胞周期调节蛋白的调节,这些都是 ATM 和 ATR 激酶的下游靶标。Hoechst-碘化丙啶染色表明,CEES 诱导的细胞死亡既是坏死性的,也是凋亡性的,后者在 HaCaT 和 JB6 细胞中分别在 CEES 处理 4 和 24 小时时诱导。caspase-3 活性增加以及 caspase-3 和多聚(ADP-核糖)聚合酶(PARP)切割的同时发生,与两条细胞系中的 CEES 诱导的细胞凋亡一致,表明 caspase 途径的参与。总之,我们的研究结果表明,CEES 具有 DNA 损伤作用,激活 ATM/ATR 细胞周期检查点信号通路以及 caspase-PARP 通路,导致 JB6 和 HaCaT 细胞中的细胞周期停滞和凋亡/坏死。本研究中鉴定的分子靶标、定量生物标志物和表皮细胞模型有可能并有助于快速开发针对 HD 诱导的皮肤毒性的有效预防和治疗干预措施。