【最新中稿作品】 交替共轭聚合物、纳米结构加工、高能锂电池、钠离子电池正极结构等

中稿作品

解读 /April

Defect-Free Alternating Conjugated Polymers Enabled by Room- Temperature Stille Polymerization

https://doi.org/10.1002/anie.202115969

由于具有化学结构易于修饰、溶液可制备、能带及光谱可调节等优势，交替共轭聚合物在有机光电子领域具有重要的应用前景。目前，其制备方法主要为热活化Stille、Suzuki及直接芳基化等交叉偶联聚合方式。然而，该类热活化的合成方法存在合成重现性差，材料存在结构缺陷等问题，极大限制了共轭聚合物材料的性能和应用。近年来，中国科学院大学黄辉教授团队报道了一系列新型交叉偶联合成方法（Nat. Commun.,2022, 13, 144; Angew. Chem. Int. Ed.,2019, 58, 5044），在有机/高分子半导体材料的绿色高效合成中取得了重要进展。本工作中，该团队采用Buchwald预催化剂P(t-Bu)3Pd G3的高效催化体系，首次实现了室温下传统Stille聚合反应。实验结果表明，该方法不仅普适性广，更重要的是能够完全抑制均聚结构缺陷的产生，提高了共聚物的品质和重现性。

图文解读

图1：传统热活化Still聚合与室温Stille聚合反应的对比

（图片来源：Angew. Chem. Int. Ed.）

基于最优催化反应条件下，作者对亲核、亲电试剂底物进行了广泛的研究，成功合成了12个具有高分子量（11.3 kDa-77.8 kDa）、高产率和低分散度的共轭聚合物，表明了该方法具有良好的普适性。

图2：使用室温Stille聚合方法学合成的12个共轭聚合物

（图片来源：Angew. Chem. Int. Ed.）

进一步研究发现，高效的室温偶联不但可以提升交叉偶联的产率，而且能够显著抑制亲电或亲核试剂自偶联。因此，室温方法得到的聚合物（P1a）与传统高温方法获得的材料（P1b和P1c）相比，结构分析表明P1a完全无结构缺陷，而P1b和P1c含有亲核或亲电单体的均聚结构缺陷。吸收光谱的理论研究显示均聚结构缺陷的存在会导致吸收光谱的偏移，这与实验结果也保持了高度一致。

图3：缺陷研究

（图片来源：Angew. Chem. Int. Ed.）

作者使用上述三个材料分别进行了缺陷态密度及有机场效应晶体管（OFET）的研究，发现室温合成的材料表现出更低的缺陷态密度及更高的的空穴迁移率，优于传统热活化制备的材料，进一步支持了该方法的优越性。

图4：OFET器件制备与比较

（图片来源：Angew. Chem. Int. Ed.）

因此，黄辉/史钦钦团队采用一类简单高效的催化剂策略，开发了具有普适性的室温催化聚合方法。采用该方法制备的交叉聚合物无均聚结构缺陷，因而具有更高的器件性能。该方法的开发不仅为高性能共轭聚合物材料的制备提供了新方法，为开展共轭聚合物材料构效关系的研究奠定了基础，更为有机电子学发展提供了新的研究思路。

中稿作品

精选 /April

Vol.9 No.10 April 4, 2022

标题：

3-D Nanofabrication of Silicon and Nanostructure Fine-Tuning via Helium Ion Implantation (Adv. Mater. Interfaces 10/2022)

摘要：

Xiaolei Wen, Renwei Mao, and Huan Hu invent an approach for producing 3D silicon nanostructures with super small roughness based on substrate swelling caused by implantation of focused helium ion beams. Furthermore, mimicking the leaning tower of Pisa, they implant on the bottom of the readily made nanostructures to fine-tune the distance into sub 5-nm as well as the tilting angles.

论文链接：

https://doi.org/10.1002/admi.202270052

Vol.7 No.4 April 8, 2022

标题：

Anion–Diluent Pairing for Stable High-Energy Li Metal Batteries

摘要：

Rechargeable Li metal batteries (LMBs) have attracted wide attention as promising candidates for the next generation of energy-storage systems. However, limited Coulombic efficiency and unregulated dendrite growth restrict its application. Here, we report a kind of electrolyte by introducing fluorinated aromatic diluents into high-concentration electrolytes (HCEs). Unlike other localized HCEs, the fluorinated aromatic diluents pairing with anions promote the formation of a homogeneous and robust solid–electrolyte interphase (SEI), which endows Li metal with an ultrahigh Coulombic efficiency of ∼99.8%. The Li||LiNi0.8Co0.1Mn0.1O2 battery holds a capacity retention of >80% over 260 cycles even with a thin Li anode (20 μm) and a high cathode loading (3.5 mAh cm–2). A 1.8 Ah Li||NMC811 pouch cell with a lean electrolyte delivers an energy density of 340 Wh kg–1 and a stable cycling life over 200 cycles. The designed electrolytes, which benefit from the synergetic effects of anions and diluents on the SEI, pave the way for the next-generation LMBs.

论文链接：

https://doi.org/10.1021/acsenergylett.2c00232

Vol.7 No.4 April 11, 2022

标题：

Challenges of layer-structured cathodes for sodium-ion batteries

摘要：

As the most promising alternative to lithium-ion batteries (LIBs), sodium-ion batteries (SIBs) still face many issues that hinder their large-scale commercialization. Layered transition metal oxide cathodes have attracted widespread attention owing to their large specific capacity, high ionic conductivity, and feasible preparation conditions. However, their electrochemical properties are usually limited by the irreversible phase transition and harsh storage conditions caused by humidity sensitivity. Recently, tremendous efforts have been devoted to solving these issues toward advanced high-performance layered oxide cathodes. Herein, we summarize these remaining challenges of layered oxide cathodes and the corresponding modification strategies such as the variations in chemical compositions, the architecture of (nano)micro-structures, surface engineering, and the regulation of phase compositions. We hope that the understanding presented in this review can provide useful guidance to developing high-performance layer-structured cathode materials for advanced SIBs.

论文链接：

https://doi.org/10.1039/D1NH00585E

Vol.2 No.1 March, 2022

标题：

Recent advances in circularly polarized luminescence generated by inorganic materials

摘要：

Circularly polarized luminescence (CPL) is an interesting phenomenon that represents the unequal emission of left- and right-handed polarized light from an emitter. CPL is promising in chirality characterization and various optical applications. Traditionally, research on CPL has been centered on organic substances. Nevertheless, in recent years, CPL based on inorganic substrates has also become a nascent topic, which is significant in exploring novel chirality- and luminescence-related properties and applications in inorganic materials. This short review summarizes the recent progress made regarding the following two aspects: 1) how to endow common inorganic luminophores with CPL activity; 2) how to use emerging chiral inorganic nanomaterials to design CPL-active systems. The general synthesis strategies, optical properties, applications and outlook of CPL-active inorganic materials are also demonstrated.

论文链接：

https://chesynjournal.com/article/view/4633

Vol.61 No.16 April 11, 2022

标题：

Grade classification of human glioma using a convolutional neural network based on mid-infrared spectroscopy mapping

摘要：

This study proposes a convolutional neural network (CNN)-based computer-aided diagnosis (CAD) system for the grade classification of human glioma by using mid-infrared (MIR) spectroscopic mappings. Through data augmentation of pixels recombination, the mappings in the training set increased almost 161 times relative to the original mappings. The pixels of the recombined mappings in the training set came from all of the one-dimensional (1D) vibrational spectroscopy of 62 (almost 80% of all 77 patients) patients at specific bands. Compared with the performance of the CNN-CAD system based on the 1D vibrational spectroscopy, we found that the mean diagnostic accuracy of the recombined MIR spectroscopic mappings at peaks of 2917 cm−1, 1539 cm−1 and 1234 cm−1 on the test set performed higher and the model also had more stable patterns. This research demonstrates that two-dimensional MIR mapping at a single frequency can be used by the CNN-CAD system for diagnosis and the research also gives a prompt that the mapping collection process can be replaced by a single-frequency IR imaging system, which is cheaper and more portable than a Fourier transform infrared microscopy and thus may be widely utilized in hospitals to provide meaningful assistance for pathologists in clinics

论文链接：

https://doi.org/10.1002/jbio.202100313

Vol.103 March 1, 2022

论文链接：

https://www.jmst.org/EN/volumn/volumn_2563.shtml

Vol.3 September 11, 2021

标题：

Alumina nanoparticles-reinforced graphene-containing waterborne polyurethane coating for enhancing corrosion and wear resistance

摘要：

To clarify the corrosion behavior of Ni-based hard facing alloy Colmonoy 56 and the preferential dissolution detail at the micrometer scale, the microstructure and the elemental distribution of a rod were analyzed, followed with the polarization measurement in aqueous solution with different pH and NaCl concentrations. This rod has Fe-, Si-, and Cr-solutioned [Ni] matrix with heterogeneously dispersed secondary phases of Cr23C6, CrB, Cr2B, and Cr5B3. The polarization curve largely changed with different pH: active in acid solution and passive in neutral and alkaline solution. The strongest passivation appeared at pH=11. Cl− promoted the corrosion attack to the [Ni] matrix. In the case of pH=11, Cl− caused the fast climb of anodic current from passivation at a less noble potential. Preferential dissolution of the [Ni] matrix occurred in most solutions, except in the case of pH=14 without NaCl, in which the secondary phases preferably dissolved.

论文链接：

https://doi.org/10.1016/j.corcom.2021.11.001

Vol.13 No.1 April 11, 2022

论文链接：

http://www.ahr-journal.com/en/default.aspx

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