Lewis Acid Activation of the Ferrous Heme–NO Fragment Towards the N–N Coupling Reaction with NO to Generate N2O,Journal of the American Chemical Society

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Lewis Acid Activation of the Ferrous Heme–NO Fragment Towards the N–N Coupling Reaction with NO to Generate N2O
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-03-04 , DOI: 10.1021/jacs.7b13681
Erwin G. Abucayon ₁ , Rahul L. Khade ₂ , Douglas R. Powell ₁ , Yong Zhang ₂ , George B. Richter-Addo ₁

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Bacterial NO reductase (bacNOR) enzymes utilize a heme/non-heme active site to couple two NO molecules to N2O. We show that BF3 coordination to the nitrosyl O-atom in (OEP)Fe(NO) activates it toward N-N bond formation with NO to generate N2O. 15N-isotopic labeling reveals a reversible nitrosyl exchange reaction and follow-up N-O bond cleavage in the N2O formation step. Other Lewis acids (B(C6F5)3 and K+) also promote the NO coupling reaction with (OEP)Fe(NO). These results, complemented by DFT calculations, provide experimental support for the cis: b3 pathway in bacNOR.

中文翻译：

亚铁血红素-NO 片段的路易斯酸活化朝向与 NO 的 N-N 偶联反应生成 N2O

细菌 NO 还原酶 (bacNOR) 酶利用血红素/非血红素活性位点将两个 NO 分子与 N2O 偶联。我们表明，BF3 与 (OEP)Fe(NO) 中亚硝酰基 O 原子的配位将其激活，使其与 NO 形成 NN 键以生成 N2O。15N 同位素标记揭示了在 N2O 形成步骤中可逆的亚硝酰基交换反应和后续的 NO 键断裂。其他路易斯酸（B(C6F5)3 和 K+）也促进 NO 与 (OEP)Fe(NO) 的偶联反应。这些结果与 DFT 计算相辅相成，为 bacNOR 中的 cis: b3 通路提供了实验支持。

更新日期：2018-03-04

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