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首页> 外文期刊>Chemistry: A European journal >How does Cu~(II) convert into Cu~I? An unexpected ring-mediated single-electron reduction
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How does Cu~(II) convert into Cu~I? An unexpected ring-mediated single-electron reduction

机译：Cu〜（II）如何转化为Cu〜I？意外的环介导的单电子还原

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摘要

Cu_xO (x=1,2) nanomaterials with tailored composition and properties-a hot topic in sustainable technologies-may be fabricated from molecular sources through bottom-up processes that involve unexpected changes in the metal oxidation state and open intriguing challenges on the copper redox chemistry. How copper(II) sources may lead to copper(I) species in spite of the absence of any explicit reducing agent, and even in the presence of oxygen, is one such question-to date unanswered. Herein, we study copper "reduction without reductants" within one molecule and reveal that the actual reducing agent is abstracted atomic hydrogen. By investigating the fragmentation of a copper(II) precursor for copper oxide nanostructures by combined ESI-MS with multiple collisional experiments (ESI/MS~n) and theoretical calculations, we highlight a copper-promoted C-H bond activation, leading to reduction of the metal center and formation of a Cu~I-C-NCCN six-membered ring. Such a novel ring system is the structural motif for a new family of cyclic copper(I) adducts, which show a bonding scheme, herein reported for the first time, that may shed unprecedented light on copper chemistry. Beyond the relevance for the preparation of copper oxide nanostructures, the hydrogen-abstraction/proton-delivery/electron-gain mechanism of copper(II) reduction disclosed herein appears to be a general property of copper and might help to understand its redox reactivity.
机译：具有定制的成分和性能的Cu_xO（x = 1,2）纳米材料-可持续技术中的热门话题-可以通过自下而上的过程由分子来源制造，该过程涉及金属氧化态的意外变化并给铜氧化还原带来了有趣的挑战化学。尽管没有任何明确的还原剂，甚至在有氧的情况下，铜（II）源如何导致形成铜（I）物种，也是迄今尚未解决的一个问题。在本文中，我们研究了一个分子内的铜“没有还原剂的还原”，并揭示了实际的还原剂是抽象的原子氢。通过结合多种碰撞实验（ESI / MS〜n）和理论计算研究ESI-MS对氧化铜纳米结构的铜（II）前体的裂解，我们强调了铜促进的CH键活化，从而降低了金属中心并形成Cu〜IC-NCCN六元环。这样的新型环系统是环状铜（I）加合物新家族的结构基序，该家族显示出本文首次报道的键合方案，该方案可能对铜化学产生前所未有的启示。除了制备氧化铜纳米结构的重要性以外，本文公开的铜（II）还原的氢吸收/质子传递/电子增益机理似乎是铜的一般性质，并且可能有助于理解其氧化还原反应性。

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