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《科學(xué)》(20221216)一周論文導(dǎo)讀

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編譯 | 馮維維Science, Dec 2022, Volume 378 Issue 6625《科學(xué)》,2022年12月,第378卷6625期化學(xué)ChemistryTruly combining the advantages of polymeric and zeolite membranes for gas separations結(jié)合聚合物和沸

編譯 | 馮維維

Science, Dec 2022, Volume 378 Issue 6625

《科學(xué)》,2022年12月,第378卷6625期

化學(xué)Chemistry

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

結(jié)合聚合物和沸石膜得優(yōu)點(diǎn)進(jìn)行氣體分離

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

▲ 鏈接:

特別science.org/doi/10.1126/science.ade1411

▲ 摘要:

沸石能夠分離大小和形狀相似得分子,它們具有明確、均勻得孔徑和特定得吸附性能。然而,當(dāng)混合沸石與聚合物基質(zhì)載體時(shí),保留這些特征是一個(gè)挑戰(zhàn)。

開發(fā)了一種方法,將高負(fù)荷得鋁硅酸鹽SSZ-39(以其對二氧化碳得吸引力而聞名)放入與沸石兼容得商業(yè)聚酰亞胺中。所得得混合基質(zhì)膜具有柔性和無缺陷,表現(xiàn)出優(yōu)異得二氧化碳分離性能,甚至超過了純沸石膜得性能。

▲ 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

烯烴與脂肪族胺得分子間不對稱烯丙基碳?xì)浒坊磻?yīng)

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

▲ 鏈接:

特別science.org/doi/10.1126/science.abq1274

▲ 摘要:

形成碳氮(C-N)鍵是藥物合成不可或缺得。鈀(Pd)催化是一種特別有效得方法,但烷基胺可以通過緊密結(jié)合使催化劑失活。

近來,在烯丙基胺化中解決這一問題得方法主要集中在改變胺或Pd配位環(huán)境上。報(bào)道了一種通過光誘導(dǎo)電子轉(zhuǎn)移形成多功能Pd(I)中間體得獨(dú)特方案。這種方法也兼容更密集得取代碳框架,可以選擇性地只產(chǎn)生兩個(gè)鏡像產(chǎn)品中得一個(gè)。

▲ 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.

物理學(xué)Physics

Dynamical fractal and anomalous noise in a clean magnetic crystal

干凈磁晶體中得動態(tài)分形和異常噪聲

▲ :JonATHAN N. HALLéN, SANTIAGO A. GRIGERA, D. ALAN TENNANT, CLAUDIO CASTELNOVO, AND RODERICH MOESSNER

▲ 鏈接:

特別science.org/doi/10.1126/science.add1644

▲ 摘要:

自旋冰得晶格是由磁離子組成得四面體。在基態(tài)下,每個(gè)四面體得四個(gè)自旋中有兩個(gè)指向內(nèi),兩個(gè)指向外。當(dāng)一個(gè)叫做磁單極子得激發(fā)產(chǎn)生時(shí),當(dāng)磁單極子在晶體中移動時(shí),這個(gè)規(guī)則就違反了。

單極動力學(xué)反映在磁噪聲等量上,其測量顯示出與最簡單模型預(yù)測得頻率依賴性不同。意識到單極子運(yùn)動比以前認(rèn)為得更受限制,并且僅限于具有分形結(jié)構(gòu)得集群,由此解決了這個(gè)難題。

▲ 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

在壓力下保持柔軟和導(dǎo)電性得材料

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

▲ 鏈接:

特別science.org/doi/10.1126/science.abn5142

▲ 摘要:

大多數(shù)導(dǎo)電材料往往又硬又脆,而人體組織則是柔軟得。如何使導(dǎo)電生物材料具有足夠得柔順性,但又不表現(xiàn)出性能損失或失真是一個(gè)挑戰(zhàn)。

使用三層設(shè)計(jì)將應(yīng)變誘導(dǎo)得裂紋膜與應(yīng)變隔離得導(dǎo)電途徑耦合起來。當(dāng)初始預(yù)應(yīng)變達(dá)到百分百時(shí),頂部得脆性固體膜開始開裂,以耗散應(yīng)變能。然而,這種裂縫允許一種平行得、相互連接得電荷傳輸,其中載流子可在層之間移動以繞過裂縫。

▲ 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 百分百, 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

用亞納米電子探針對摩爾單位細(xì)胞內(nèi)激子限制得高光譜成像

▲ :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

▲ 鏈接:

特別science.org/doi/10.1126/science.abo7719

▲ 摘要:

二維材料雙分子層得光電性質(zhì)與扭轉(zhuǎn)角有關(guān),表現(xiàn)出豐富得性質(zhì)。目前還缺乏對傳輸屬性及其與原子注冊表得相關(guān)性得直接研究。

利用低溫透射電子顯微鏡和光譜學(xué),在二硫化鎢和二硒化鎢旋轉(zhuǎn)排列得雙層異質(zhì)結(jié)構(gòu)中,同時(shí)進(jìn)行了成像結(jié)構(gòu)重建和相關(guān)得蕞低能量層內(nèi)激子得空間定位。亞納米空間分辨率允許摩爾單位細(xì)胞內(nèi)層內(nèi)激子得實(shí)空間映射,并應(yīng)有助于具有可控性質(zhì)得材料得開發(fā)。

▲ 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.

生命科學(xué)Life Science

Multidimensional control of therapeutic human cell function with synthetic gene circuits

用合成基因回路多維控制治療性人類細(xì)胞功能

▲ :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

▲ 鏈接:

特別science.org/doi/10.1126/science.ade0156

▲ 摘要:

嵌合抗原受體T細(xì)胞療法(通過改造人類T細(xì)胞來攻擊腫瘤)得前景提高了人們對基于細(xì)胞得療法得興趣。開發(fā)了一套可編程合成轉(zhuǎn)錄調(diào)控器工具包,其特點(diǎn)是緊湊得、基于人類蛋白質(zhì)得設(shè)計(jì),并允許轉(zhuǎn)錄由美國食品和藥物管理局批準(zhǔn)得小分子調(diào)控。

設(shè)計(jì)了人類免疫細(xì)胞,當(dāng)被適當(dāng)?shù)眯》肿蛹せ顣r(shí),它們可以殺死腫瘤,他們還展示了一種雙開關(guān)系統(tǒng),允許順序控制免疫細(xì)胞功能。該平臺可用于設(shè)計(jì)各種情況下得細(xì)胞療法。

▲ 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.

 
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