Wellcome Trust Centre for Gene Regulation and Expression, College of Life Sciences, University of Dundee, Dundee DD1 5EH, UK.
Nature. 2012 Sep 6;489(7414):115-20. doi: 10.1038/nature11376.
Ubiquitin modification is mediated by a large family of specificity determining ubiquitin E3 ligases. To facilitate ubiquitin transfer, RING E3 ligases bind both substrate and a ubiquitin E2 conjugating enzyme linked to ubiquitin via a thioester bond, but the mechanism of transfer has remained elusive. Here we report the crystal structure of the dimeric RING domain of rat RNF4 in complex with E2 (UbcH5A) linked by an isopeptide bond to ubiquitin. While the E2 contacts a single protomer of the RING, ubiquitin is folded back onto the E2 by contacts from both RING protomers. The carboxy-terminal tail of ubiquitin is locked into an active site groove on the E2 by an intricate network of interactions, resulting in changes at the E2 active site. This arrangement is primed for catalysis as it can deprotonate the incoming substrate lysine residue and stabilize the consequent tetrahedral transition-state intermediate.
泛素修饰是由一大类特异性决定的泛素 E3 连接酶介导的。为了促进泛素转移,RING E3 连接酶通过硫酯键结合底物和与泛素连接的泛素 E2 连接酶,但转移的机制仍然难以捉摸。在这里,我们报告了与通过异肽键连接的泛素(UbcH5A)连接的大鼠 RNF4 的二聚体 RING 结构域的晶体结构。虽然 E2 与 RING 的单个单体接触,但泛素通过两个 RING 单体的接触折叠回到 E2 上。泛素的羧基末端尾巴被一个复杂的相互作用网络锁定在 E2 的活性位点槽中,导致 E2 活性位点发生变化。这种排列为催化做好了准备,因为它可以使进入的底物赖氨酸残基去质子化,并稳定随后的四面体型过渡态中间物。