《自然》（20231102出版）一周论文导读

 
 
《自然》（20231102出版）一周论文导读  
 

 

编译 | 李言

Nature,  2 November 2023, Volume 623 Issue 7985

《自然》2023年11月2日，第623卷，7985期

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材料科学Materials Science

Injectable tissue prosthesis for instantaneous closed-loop rehabilitation

可以进行瞬时闭环康复的可注射组织假体

▲ 作者：Subin Jin, Heewon Choi et al.

▲ 链接：

https://www.nature.com/articles/s41586-023-06628-x

▲ 摘要：

在这里，我们提出了一种可注射的组织假体，它们在神经肌肉系统中具有瞬时双向电传导能力。这种柔软的可注射假体由具有独特的苯硼酸介导多重交联的生物相容性水凝胶组成，如不可逆但可自由重排的联苯键和可逆的配位键，通过原位交叉偶联形成导电金纳米颗粒。

在大鼠严重肌肉损伤的早期阶段，通过注射这种假体材料成功实现了机器闭环辅助康复，并在后期实现了组织的加速修复。

▲ Abstract：

Here we present an injectable tissue prosthesis with instantaneous bidirectional electrical conduction in the neuromuscular system. The soft and injectable prosthesis is composed of a biocompatible hydrogel with unique phenylborate-mediated multiple crosslinking, such as irreversible yet freely rearrangeable biphenyl bonds and reversible coordinate bonds with conductive gold nanoparticles formed in situ by cross-coupling. Closed-loop robot-assisted rehabilitation by injecting this prosthetic material is successfully demonstrated in the early stage of severe muscle injury in rats, and accelerated tissue repair is achieved in the later stage.

化学Chemistry

Quinone-mediated hydrogen anode for non-aqueous reductive electrosynthesis

醌介导的非水还原电合成氢阳极

▲ 作者：Jack Twilton, Mathew R. Johnson et al.

▲ 链接：

https://www.nature.com/articles/s41586-023-06534-2

▲ 摘要：

在此，我们报告了一种介导的H2阳极，通过将蒽醌介质的热催化加氢与蒽氢醌的电化学氧化配对，实现了H2的间接电化学氧化。这种醌介导的H2阳极用于支持镍催化的交叉亲电偶联（XEC），这种反应类别在制药工业中得到广泛采用。

我们在小规模间歇反应中对该方法进行了初步验证，随后适应了可实现百克级药物中间体合成的再循环反应器。我们的介导H2阳极技术提供了一种支持H2驱动的电合成还原的普遍策略。

▲ Abstract：

Here we report a mediated H2 anode that achieves indirect electrochemical oxidation of H2 by pairing thermal catalytic hydrogenation of an anthraquinone mediator with electrochemical oxidation of the anthrahydroquinone. This quinone-mediated H2 anode is used to support nickel-catalysed cross-electrophile coupling (XEC), a reaction class gaining widespread adoption in the pharmaceutical industry. Initial validation of this method in small-scale batch reactions is followed by adaptation to a recirculating flow reactor that enables hectogram-scale synthesis of a pharmaceutical intermediate. The mediated H2 anode technology disclosed here offers a general strategy to support H2-driven electrosynthetic reductions.

Carbon-to-nitrogen single-atom transmutation of azaarenes

氮杂芳烃的碳-氮单原子嬗变

▲ 作者：Jisoo Woo, Colin Stein, Alec H. Christian & Mark D. Levin.

▲ 链接：

https://www.nature.com/articles/s41586-023-06613-4

▲ 摘要：

在此，我们报告了一种使杂芳香碳原子直接转化为氮原子，将喹啉类转化为喹唑啉类的转化过程。母体氮杂芳烃的氧化重组得到了一个开环的中间体，带有亲电位点，为环重合和碳基离去基的排出准备了条件。

这种方法不同于现有的原子插入—删除方法，从而避免了逐步骨骼编辑中常见的骨架旋转和取代基微扰陷阱。我们展示了广泛的喹啉和相关的氮杂芳烃，所有这些都可以通过用氮原子取代C3碳转化为相应的喹唑啉。实验支持了活化中间体的关键作用，并指出了c - n嬗变反应发展的更一般策略。

▲ Abstract：

Here, we report a transformation that enables the direct conversion of a heteroaromatic carbon atom into a nitrogen atom, turning quinolines into quinazolines. Oxidative restructuring of the parent azaarene gives a ring-opened intermediate bearing electrophilic sites primed for ring reclosure and expulsion of a carbon-based leaving group. Such a ‘sticky end’ approach subverts existing atom insertion–deletion approaches and as a result avoids skeleton-rotation and substituent-perturbation pitfalls common in stepwise skeletal editing. We show a broad scope of quinolines and related azaarenes, all of which can be converted into the corresponding quinazolines by replacement of the C3 carbon with a nitrogen atom. Mechanistic experiments support the critical role of the activated intermediate and indicate a more general strategy for the development of C-to-N transmutation reactions.

气候科学Climate Science

Seasonal advance of intense tropical cyclones in a warming climate

气候变暖时强烈热带气旋的季节性推进

▲ 作者：Kaiyue Shan, Yanluan Lin, Pao-Shin Chu, Xiping Yu & Fengfei Song

▲ 链接：

https://www.nature.com/articles/s41586-023-06544-0

▲ 摘要：