Department of Neuroscience, Psychology, Drug Research and Child Health (NEUROFARBA), Section of Pharmacology and Toxicology, University of Florence, Viale G. Pieraccini 6, 50139, Florence, Italy.
Department of Experimental and Clinical Biomedical Sciences, "Mario Serio"-Unit of Biochemical Sciences and Molecular Biology, University of Florence, Viale GB Morgagni 50, 50134, Florence, Italy.
Neurotherapeutics. 2022 Sep;19(5):1634-1648. doi: 10.1007/s13311-022-01243-6. Epub 2022 May 2.
Despite the effort on developing new treatments, therapy for neuropathic pain is still a clinical challenge and combination therapy regimes of two or more drugs are often needed to improve efficacy. Accumulating evidence shows an altered expression and activity of histone acetylation enzymes in chronic pain conditions and restoration of these aberrant epigenetic modifications promotes pain-relieving activity. Recent studies showed a synergistic activity in neuropathic pain models by combination of histone deacetylases (HDACs) and bromodomain and extra-terminal domain (BET) inhibitors. On these premises, the present study investigated the pharmacological profile of new dual HDAC/BRD4 inhibitors, named SUM52 and SUM35, in the spared nerve injury (SNI) model in mice as innovative strategy to simultaneously inhibit HDACs and BETs. Intranasal administration of SUM52 and SUM35 attenuated thermal and mechanical hypersensitivity in the absence of locomotor side effects. Both dual inhibitors showed a preferential interaction with BRD4-BD2 domain, and SUM52 resulted the most active compound. SUM52 reduced microglia-mediated spinal neuroinflammation in spinal cord sections of SNI mice as showed by reduction of IBA1 immunostaining, inducible nitric oxide synthase (iNOS) expression, p65 nuclear factor-κB (NF-κB) and p38 MAPK over-phosphorylation. A robust decrease of the spinal proinflammatory cytokines content (IL-6, IL-1ß) was also observed after SUM52 treatment. Present results, showing the pain-relieving activity of HDAC/BRD4 dual inhibitors, indicate that the simultaneous modulation of BET and HDAC activity by a single molecule acting as multi-target agent might represent a promise for neuropathic pain relief.
尽管在开发新疗法方面付出了努力,但神经病理性疼痛的治疗仍然是一个临床挑战,通常需要联合两种或多种药物的治疗方案来提高疗效。越来越多的证据表明,在慢性疼痛情况下,组蛋白乙酰化酶的表达和活性发生改变,恢复这些异常的表观遗传修饰可促进止痛作用。最近的研究表明,组蛋白去乙酰化酶 (HDAC) 和溴结构域和末端外结构域 (BET) 抑制剂联合使用在神经病理性疼痛模型中具有协同作用。基于这些前提,本研究在 spared nerve injury (SNI) 小鼠模型中研究了新型双重 HDAC/BRD4 抑制剂 SUM52 和 SUM35 的药理学特性,作为同时抑制 HDACs 和 BETs 的创新策略。SUM52 和 SUM35 的鼻腔给药可减轻热和机械性超敏反应,而无运动副作用。两种双重抑制剂均表现出与 BRD4-BD2 结构域的优先相互作用,且 SUM52 是最活跃的化合物。SUM52 可减少 SNI 小鼠脊髓中的小胶质细胞介导的神经炎症,如减少 IBA1 免疫染色、诱导型一氧化氮合酶 (iNOS) 表达、p65 核因子-κB (NF-κB) 和 p38 MAPK 的过度磷酸化。SUM52 处理后,脊髓中促炎细胞因子的含量(IL-6、IL-1β)也明显下降。本研究结果表明,HDAC/BRD4 双重抑制剂具有止痛作用,表明通过单个多靶标分子同时调节 BET 和 HDAC 活性可能是缓解神经病理性疼痛的一种有希望的方法。