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101.
Haicun Yang Shuipi Cai Yu Jiang Zheng Cao Wenzhong Ma Fanghong Gong Guoliang Tao Chunlin Liu 《Journal of polymer science. Part A, Polymer chemistry》2022,60(10):1571-1587
The commonly used multi-center initiation methods always lead to the formation of quantities of homopolymer in the surface tailoring based on reverse atom transfer radical polymerization (ATRP) and reversible addition-fragmentation chain-transfer (RAFT) polymerization. In this study, a monocenter redox pair constructed of silica bearing tert-butyl hydroperoxide groups and ascorbic acid (SiO2-TBHP/AsAc) was applied to substitute the commonly used initiation method of R-supported RAFT grafting polymerization. All the propagating radicals were restricted on the surface of solid particles during the whole procedure theoretically, resulting in a higher grafting efficiency of 95.1% combined with the “controllable” feature at 10 h. This redox pair was also used to initiate the reverse ATRP in miniemulsion successfully with a grafting efficiency of 86.3% at 10 h. The grafting efficiency obtained under this monocenter initiation method was significantly higher than that of the frequently reported surface modification by reverse ATRP and RAFT polymerization. In addition, the high-efficient surface tailoring was traced and confirmed by nuclear magnetic resonance, Fourier transform infrared, X-ray photoelectron spectroscopy, thermogravimetric analysis, transmission electron microscopy, and other analysis tests. The advantage of this monocenter redox pair will open a new avenue for the potential “high-efficient” surface tailoring of various materials. 相似文献
102.
Yong Gao Dani Zhang Dr. Jingjing Li Prof. Hao Gong Dr. Cheng Jiang Dr. Hairong Xue Prof. Xianli Huang Prof. Tao Wang Prof. Jianping He 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(71):e202202410
Electrocatalysis is the most promising strategy to generate clean energy H2, and the development of catalysts with excellent hydrogen evolution reaction (HER) performance at high current density that can resist strong alkaline and acidic electrolyte environment is of great significance for practical industrial application. Therefore, a P doped MoS2@Ni3S2 nanorods array (named P-NiMoS) was successfully synthesized through successive sulfuration and phosphorization. P-NiMoS presents a core/shell structure with a heterojunction between MoS2 (shell) and Ni3S2 (core). Furthermore, the doping of P modulates the electronic structure of the P-NiMoS; the electrons transfer from the t2g orbital of Ni element to the eg empty orbital of Mo element through the Ni−S−Mo bond at the Ni3S2 and MoS2 heterojunction, facilitating the hydrogen evolution reaction. As a result, P-NiMoS exhibits excellent HER activity; the overpotential is 290 mV at high current density of 250 mA cm−2 in alkaline electrolyte, which is close to Pt/C (282 mV@250 mA cm−2), and P-NiMoS can stably evolve hydrogen for 48 h. 相似文献
103.
Mi Ouyang Dacheng Dai Xuming Hu Yuwen Li Zhangxin Chen Bowen Tao Lina Zhang Weijun Li Yujie Dong Ru Bai Xiaojing Lv Cheng Zhang 《Journal of polymer science. Part A, Polymer chemistry》2022,60(15):2269-2279
A new star-shaped structure conjugated microporous polymers, poly (2,8,14-tri[4-diphenyl-benzene]-hexaazatrinaphthylene) (PTPA-HATN), was designed and in-situ electrochemically polymerized on the surfaces of FTO electrodes with a directional alignment TiO2 nanorod array to obtain TiO2/PTPA-HATN core-shell nanocomposite films. Compared with the PTPA-HATN film, the TiO2/PTPA-HATN composite film exhibits higher optical contrast and faster response time, with contrast of 57% at 783 nm, coloring time of 3.62 s and discoloring time of 2.55 s (43%, 4.63 s and 4.77 s for PTPA-HATN film, respectively). After 400 cycles, the contrast of nanocomposite film decreased by 28%, while the PTPA-HATN film basically lost its electrochromic properties. A simple three-layer EC prototype device based on TiO2/PTPA-HATN nanocomposite film constructed with hydrogel electrolyte clearly shows color changes at different voltages. On the one hand, the formation of core-shell porous nanostructure of TiO2/PTPA-HATN composite film provides a larger ion doping/de-doping interface, shortening the average diffusion length of ions. On the other hand, the large indented polymer-nanorods contact interface makes it difficult for the polymer to detach from the electrode, thus significantly improving the cyclic stability of the composite film. 相似文献
104.
Back Cover: Spontaneous Stepwise Self‐Assembly of a Polyoxometalate–Organic Hybrid into Catalytically Active One‐Dimensional Anisotropic Structures (Chem. Eur. J. 31/2014) 下载免费PDF全文
105.
通过建立模型分析了近6年来的北京市高考试题。从试题水平来看,学生需要建立水溶液问题的基本认识角度和分析思路;从能力要求来看,部分试题实现了对关键能力的融合考查。在此基础上进行试题命制和施测,发现学生不能自主调用多个认识角度形成思路,提出了比较不同问题情境中的共同认识角度与建立“水溶液-平衡”二元分析模型的教学改进策略。 相似文献
106.
Dr. Yuting Li Prof. Dr. Yu Tang Prof. Dr. Franklin Tao 《Angewandte Chemie (International ed. in English)》2023,62(15):e202214332
C−N coupling is significant for the synthesis of fine chemicals toward various applications. Hydroaminoalkylation of olefins is a tandem reaction of C−N coupling involving first the formation of an aldehyde through hydroformylation of an olefin and then the production of amine through reductive amination of the aldehyde. Here we report a stable, supported catalyst of singly dispersed Rh1 atoms anchored on TiO2 (P25) nanoparticles designated as Rh1/P25. Its high activity for C−N coupling was demonstrated by six hydroaminoalkylations of olefins and amines with selectivity of higher than 90% for producing tertiary amines. The singly dispersed Rh1O4 on P25 exhibit activity and selectivity for hydroaminoalkylation comparable or even higher than some reported molecular catalysts. In contrast to molecular catalysts, the Rh-based single-atom Rh heterogeneous catalysis (Rh1/P25) can be readily separated from reactants and products, reused for multiple runs of hydroaminoalkylation, and recycled with a low cost. 相似文献
107.
Zheng Zhou Xin Pei Tao Zhang Liting Wang Jianhe Hong Yu Lu Gang He 《Electroanalysis》2023,35(4):e202200306
Gel polymer electrolytes (GPEs) incorporate both the high ionic conductivity of organic liquid electrolyte and the high safety performance of all-solid-state electrolytes (ASSEs), greatly improving the electrochemical performance of solid polymer electrolytes (SPEs). However, the practical application of GPEs is still limited by inferior interface compatibility, lithium dendrites, etc. Herein, we prepared GPEs based on poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) further co-blended the two-dimensional sheet inorganic filler hectorite and poly(methyl methacrylate) (PMMA) to improve the mechanical and electrochemical properties of the GPEs. When the content of PMMA and hectorite is optimal, this GPEs have an ionic conductivity of 1.06×10−3 S cm−1 and outstanding lithium symmetric cells cycle time of more than 3000 h, indicating that the introduction of filler effectively inhibits the growth of lithium dendrites at room temperature. Moreover, the GPEs adopt a relatively simple solution casting method to provide a fresh idea for the synthesis of high-performance GPEs. 相似文献
108.
Jiehao Du Banggui Cheng Huiqing Yuan Yuan Tao Ya Chen Mei Ming Zhiji Han Richard Eisenberg 《Angewandte Chemie (International ed. in English)》2023,62(9):e202211804
We report the unprecedented electrocatalytic activity of a series of molecular nickel thiolate complexes ( 1 – 5 ) in reducing CO2 to C1–3 hydrocarbons on carbon paper in pH-neutral aqueous solutions. Ni(mpo)2 ( 3 , mpo=2-mercaptopyridyl-N-oxide), Ni(pyS)3− ( 4 , pyS=2-mercaptopyridine), and Ni(mp)2− ( 5 , mp=2-mercaptophenolate) were found to generate C3 products from CO2 for the first time in molecular complex. Compound 5 exhibits Faradaic efficiencies (FEs) of 10.6 %, 7.2 %, 8.2 % for C1, C2, C3 hydrocarbons respectively at −1.0 V versus the reversible hydrogen electrode. Addition of CO to the system significantly promotes the FEC1–C3 to 41.1 %, suggesting that a key Ni−CO intermediate is associated with catalysis. A variety of spectroscopies have been performed to show that the structures of nickel complexes remain intact during CO2 reduction. 相似文献
109.
Asma Mani Tao Feng Albert Gandioso Robin Vinck Anna Notaro Lisa Gourdon Pierre Burckel Bruno Saubaméa Olivier Blacque Kevin Cariou Jamel-Eddine Belgaied Hui Chao Gilles Gasser 《Angewandte Chemie (International ed. in English)》2023,62(20):e202218347
Five osmium(II) polypyridyl complexes of the general formula [Os(4,7-diphenyl-1,10-phenanthroline)2 L ]2+ were synthesized as photosensitizers for photodynamic therapy by varying the nature of the ligand L . Thanks to the pronounced π-extended structure of the ligands and the heavy atom effect provided by the osmium center, these complexes exhibit a high absorption in the near-infrared (NIR) region (up to 740 nm), unlike related ruthenium complexes. This led to a promising phototoxicity in vitro against cancer cells cultured as 2D cell layers but also in multicellular tumor spheroids upon irradiation at 740 nm. The complex [Os(4,7-diphenyl-1,10-phenanthroline)2(2,2′-bipyridine)]2+ was found to be the most efficient against various cancer cell lines, with high phototoxicity indexes. Experiments on CT26 tumor-bearing BALB/c mice also indicate that the OsII complexes could significantly reduce tumor growth following 740 nm laser irradiation. The high phototoxicity in the biological window of this structurally simple complex makes it a promising photosensitizer for cancer treatment. 相似文献
110.
Shuang Qiu Wannan Li Tao Deng Angzhi Bi Yang Yang Xi Jiang Dr. Jie P. Li 《Angewandte Chemie (International ed. in English)》2023,62(28):e202303014
Intercellular proximity labeling has emerged as a promising approach to enable the study of cell-cell interactions (CCIs), but the efficiency of current platforms is limited. Here, we use Ru(bpy)32+ to construct an efficient photocatalytic proximity labeling (PPL) system on the cell surface that allows the highly discriminative CCI detection with spatiotemporal resolution. Through the mechanism study and quantitative characterization on living cells, we demonstrate that the singlet-oxygen (1O2) mechanism is more efficient and specific than the single electron transfer (SET) mechanism in Ru-mediated PPL. Ru(bpy)32+ catalysts with different cell-anchoring moieties are prepared to facilitate the catalyst loading on primary cells. Finally, based on this system, we develop a “live” T cell receptor (TCR) multimer with TCR-T cells that could sensitively identify and discriminate cells presenting antigens of different affinity, providing a powerful tool to better understand the heterogeneity of antigen presenting cells. 相似文献