Liao Jie, Hwang Sung Hee, Li Haonan, Yang Yihe, Yang Jun, Wecksler Aaron T, Liu Jun-Yan, Hammock Bruce D, Yang Guang-Yu
Department of Pathology, Feinberg School of Medicine, Northwestern University, Chicago, IL 60611, USA.
Department of Entomology and Cancer Center, University of California, One Shields Avenue, Davis, CA 95616, USA.
Cancer Lett. 2016 Feb 28;371(2):187-93. doi: 10.1016/j.canlet.2015.11.042. Epub 2015 Dec 9.
Mutant Kras and chronic pancreatitis are the most common pathological events involved in human pancreatic cancer. It has been demonstrated that c-Raf is responsible for transmitting signals from mutant Ras to its downstream signals including MEK-ERK and for initiating carcinogenesis. The soluble epoxide hydrolase (sEH), a pro-inflammatory enzyme, generally inactivates anti-inflammatory and anti-pain epoxyeicosatrienoic acids (EETs). Herein, we have synthesized a novel compound of trans-4-{4-[3-(4-chloro-3-trifluoromethyl-phenyl)-ureido]-cyclohexyloxy}-pyridine-2-carboxylic acid methylamide (t-CUPM) via modifying the central phenyl ring of sorafenib and confirmed its dual inhibition of sEH and c-Raf by recombinant kinase activity assay. Pharmacokinetic analysis revealed that oral dosing of t-CUPM resulted in higher blood levels than that of sorafenib throughout the complete time course (48 h). The effect of t-CUPM on the inhibition of mutant Kras(G12D)-initiated murine pancreatic cancer cell growth was determined using the mouse pancreatic carcinoma cell model obtained from LSL-Kras(G12D)/Pdx1-Cre mice and showed that t-CUPM significantly inhibited this murine pancreatic carcinoma cell growth both in vitro and in mice in vivo. Inhibition of mutant Kras-transmitted phosphorylations of cRAF/MEK/ERK was demonstrated in these pancreatic cancer cells using Western blot assay and immunohistochemical approach. Modulation of oxylipin profile, particularly increased EETs/DHET ratio by sEH inhibition, was observed in mice treated with t-CUPM. These results indicate that t-CUPM is a highly potential agent to treat pancreatic cancer via simultaneously targeting c-Raf and sEH.
突变型Kras和慢性胰腺炎是人类胰腺癌中最常见的病理事件。已经证明,c-Raf负责将信号从突变型Ras传递到其下游信号,包括MEK-ERK,并启动致癌作用。可溶性环氧化物水解酶(sEH)是一种促炎酶,通常会使抗炎和抗疼痛的环氧二十碳三烯酸(EETs)失活。在此,我们通过修饰索拉非尼的中心苯环合成了一种新型化合物反式-4-{4-[3-(4-氯-3-三氟甲基苯基)-脲基]-环己氧基}-吡啶-2-羧酸甲酰胺(t-CUPM),并通过重组激酶活性测定证实了其对sEH和c-Raf的双重抑制作用。药代动力学分析表明,在整个完整的时间过程(48小时)中,口服t-CUPM导致的血药浓度高于索拉非尼。使用从LSL-Kras(G12D)/Pdx1-Cre小鼠获得的小鼠胰腺癌细胞模型,确定了t-CUPM对突变型Kras(G12D)启动的小鼠胰腺癌细胞生长的抑制作用,结果表明t-CUPM在体外和体内小鼠中均显著抑制了这种小鼠胰腺癌细胞的生长。使用蛋白质印迹分析和免疫组织化学方法在这些胰腺癌细胞中证实了对突变型Kras传递的cRAF/MEK/ERK磷酸化的抑制作用。在用t-CUPM处理的小鼠中观察到氧化脂质谱的调节,特别是通过抑制sEH使EETs/DHET比值增加。这些结果表明,t-CUPM是一种通过同时靶向c-Raf和sEH来治疗胰腺癌的极具潜力的药物。