《科学》（20221216）一周论文导读

编译 | 冯维维

Science, Dec 2022, Volume 378 Issue 6625

《科学》，2022年12月，第378卷6625期

化学Chemistry

Truly combining the advantages of polymeric and zeolite membranes for gas separations

结合聚合物和沸石膜的优点进行气体分离

▲ 作者：XIAOYU TAN, SVEN ROBIJNS, RAYMOND THÜR, QUANLI K, NIELS DE WITTE, ARAN LAMAIRE, YUN LI, IMRAN ASLAM, DAAN VAN HAVERE, AND IVO VANKELECOM

▲ 链接：

https://www.science.org/doi/10.1126/science.ade1411

▲ 摘要：

沸石能够分离大小和形状相似的分子，它们具有明确、均匀的孔径和特定的吸附性能。然而，当混合沸石与聚合物基质载体时，保留这些特征是一个挑战。

作者开发了一种方法，将高负荷的铝硅酸盐SSZ-39（以其对二氧化碳的吸引力而闻名）放入与沸石兼容的商业聚酰亚胺中。所得的混合基质膜具有柔性和无缺陷，表现出优异的二氧化碳分离性能，甚至超过了纯沸石膜的性能。

▲ Abstract：

Zeolites are able to separate molecules with similar size and shape because of their well-defined, uniform pore size and specific adsorption properties. However, it has been a challenge to retain these features when blending a zeolite with a polymeric matrix support. Tan et al. developed a method to put high loadings of the aluminosilicate SSZ-39, which is known for its attraction of carbon dioxide, into a commercial polyimide selected for its compatibility with the zeolite. The resulting mixed matrix membranes were flexible and defect free, showing excellent separation of carbon dioxide that even exceeded the performance of pure zeolite membranes.

Asymmetric intermolecular allylic C–H amination of alkenes with aliphatic amines

烯烃与脂肪族胺的分子间不对称烯丙基碳氢胺化反应

▲ 作者：KELVIN PAK, SHING CHEUNG, JIAN FANG, KALLOL MUKHERJEE, ANDRANIK MIHRANYAN, AND VLADIMIR GEVORGYAN

▲ 链接：

https://www.science.org/doi/10.1126/science.abq1274

▲ 摘要：

形成碳氮（C-N）键是药物合成不可或缺的。钯（Pd）催化是一种特别有效的方法，但烷基胺可以通过紧密结合使催化剂失活。

近来，在烯丙基胺化中解决这一问题的方法主要集中在改变胺或Pd配位环境上。作者报道了一种通过光诱导电子转移形成多功能Pd(I)中间体的独特方案。这种方法也兼容更密集的取代碳框架，可以选择性地只产生两个镜像产品中的一个。

▲ Abstract：

Forming carbon–nitrogen (C–N) bonds is integral to pharmaceutical synthesis. Palladium (Pd) catalysis is an especially efficient means to this end, but alkyl amines can deactivate the catalyst by tight binding. Several recent approaches to circumventing this problem in allylic amination have focused on modifying either the amines or the Pd coordination environment. Cheung et al. report a distinct protocol that operates through photoinduced electron transfer to form versatile Pd(I) intermediates. This method is also compatible with more densely substituted carbon frameworks and can selectively produce just one of two mirror image products.

物理学Physics

Dynamical fractal and anomalous noise in a clean magnetic crystal

干净磁晶体中的动态分形和异常噪声

▲ 作者：JONATHAN N. HALLÉN, SANTIAGO A. GRIGERA, D. ALAN TENNANT, CLAUDIO CASTELNOVO, AND RODERICH MOESSNER

▲ 链接：

https://www.science.org/doi/10.1126/science.add1644

▲ 摘要：

自旋冰的晶格是由磁离子组成的四面体。在基态下，每个四面体的四个自旋中有两个指向内，两个指向外。当一个叫做磁单极子的激发产生时，当磁单极子在晶体中移动时，这个规则就违反了。

单极动力学反映在磁噪声等量上，其测量显示出与最简单模型预测的频率依赖性不同。作者意识到单极子运动比以前认为的更受限制，并且仅限于具有分形结构的集群，由此解决了这个难题。

▲ Abstract：

Spin ices have crystal lattices that consist of tetrahedra of magnetic ions. In a ground state, two of the four spins on each tetrahedron point in and two point out. When an excitation called the magnetic monopole is created, this rule is violated as the monopole moves through the crystal. Monopole dynamics are reflected in quantities such as magnetic noise, the measurements of which have shown a different frequency dependence from the one that the simplest model predicts. Hallén et al. solved this puzzle by realizing that the monopole motion is more restricted than previously thought and is limited to a cluster with a fractal structure.

Soft strain-insensitive bioelectronics featuring brittle materials

在压力下保持柔软和导电性的材料

▲ 作者：YICHAO ZHAO, BO WANG, JIAWEI TAN, HEXING YIN, RUYI HUANG, JIALUN ZHU, SHUYU LIN, YAN ZHOU, DAVID JELINEK, AND SAM EMAMINEJAD

▲ 链接：

https://www.science.org/doi/10.1126/science.abn5142

▲ 摘要：

大多数导电材料往往又硬又脆，而人体组织则是柔软的。如何使导电生物材料具有足够的柔顺性，但又不表现出性能损失或失真是一个挑战。

作者使用三层设计将应变诱导的裂纹膜与应变隔离的导电途径耦合起来。当初始预应变达到100%时，顶部的脆性固体膜开始开裂，以耗散应变能。然而，这种裂缝允许一种平行的、相互连接的电荷传输，其中载流子可在层之间移动以绕过裂缝。

▲ Abstract：

Most electrically conductive materials tend to be stiff and brittle, whereas human tissue is soft and compliant. It is thus a challenge to make conductive biomaterials that are sufficiently compliant but do not show a loss or distortion in performance. Zhao et al. used a three-layer design to couple strain-induced cracked films with a strain-isolated conductive pathway. Upon an initial prestrain to 100%, the brittle solid film on top cracks to dissipate the strain energy. However, this cracking permits a type of parallel, interconnected charge transport in which the charge carriers move between the layers to circumvent the cracks.

Hyperspectral imaging of exciton confinement within a moiré unit cell with a subnanometer electron probe

用亚纳米电子探针对摩尔单位细胞内激子限制的高光谱成像

▲ 作者：SANDHYA SUSARLA, MIT H. NAIK, DARIA D. BLACH, JONAS ZIPFEL, TAKASHI TANIGUCHI, KENJI WATANABE, LIBAI HUANG, RAMAMOORTHY RAMESH, FELIPE H. DA JORNADA, AND ARCHANA RAJA

▲ 链接：

https://www.science.org/doi/10.1126/science.abo7719

▲ 摘要：

二维材料双分子层的光电性质与扭转角有关，表现出丰富的性质。目前还缺乏对传输属性及其与原子注册表的相关性的直接研究。

作者利用低温透射电子显微镜和光谱学，在二硫化钨和二硒化钨旋转排列的双层异质结构中，同时进行了成像结构重建和相关的最低能量层内激子的空间定位。亚纳米空间分辨率允许摩尔单位细胞内层内激子的实空间映射，并应有助于具有可控性质的材料的开发。

▲ Abstract：

The optoelectronic properties of bilayers of two-dimensional materials exhibit a wealth of properties dependent on the twist angle. A direct probe of the transport properties and their correlation with the atomic registry has been lacking. Susarla et al. used cryogenic transmission electron microscopy and spectroscopy to simultaneously image the structural reconstruction and the associated spatial localization of the lowest-energy intralayer exciton in a rotationally aligned bilayer heterostructure of tungsten disulfide and tungsten diselenide. The subnanometer spatial resolution allows the real-space mapping of intralayer excitons within a Moiré unit cell and should aid in the development of materials with controlled properties.

生命科学Life Science

Multidimensional control of therapeutic human cell function with synthetic gene circuits

用合成基因回路多维控制治疗性人类细胞功能

▲ 作者：HUI-SHAN LI, DIVYA V. ISRANI, KEITH A. GAGNON, KOK ANN GAN, MICHAEL H. RAYMOND, JEFFRY D. SANDER, KOLE T. ROYBAL, J. KEITH JOUNG, WILSON W. WONG, AND AHMAD S. KHALIL

▲ 链接：

https://www.science.org/doi/10.1126/science.ade0156

▲ 摘要：

嵌合抗原受体T细胞疗法（通过改造人类T细胞来攻击肿瘤）的前景提高了人们对基于细胞的疗法的兴趣。作者开发了一套可编程合成转录调控器工具包，其特点是紧凑的、基于人类蛋白质的设计，并允许转录由美国食品和药物管理局批准的小分子调控。

作者设计了人类免疫细胞，当被适当的小分子激活时，它们可以杀死肿瘤，他们还展示了一种双开关系统，允许顺序控制免疫细胞功能。该平台可用于设计各种情况下的细胞疗法。

▲ Abstract：

The promise of chimeric antigen receptor T cell therapy, in which human T cells are engineered to attack tumors, has heightened interest in cell-based therapies. Li et al. developed a toolkit of programmable synthetic transcription regulators that feature a compact, human protein–based design and allow transcription to be regulated by US Food & Drug Administration–approved small molecules. The authors engineered human immune cells that kill tumors when activated by the appropriate small molecule, and they also demonstrated a dual-switch system that allows sequential control of immune cell function. This platform could be adapted to design cell therapies in a variety of contexts.