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991.
Dr. Ziyu Wang Dr. Ya Zhang Dr. Cheng Chen Dr. Ruixue Zhu Dr. Jiaming Jiang Prof. Tsu-Chien Weng Prof. Quanjiang Ji Prof. Yifan Huang Prof. Chong Fang Prof. Weimin Liu 《Angewandte Chemie (International ed. in English)》2023,62(5):e202212209
Large Stokes shift (LSS) red fluorescent proteins (RFPs) are highly desirable for bioimaging advances. The RFP mKeima, with coexisting cis- and trans-isomers, holds significance as an archetypal system for LSS emission due to excited-state proton transfer (ESPT), yet the mechanisms remain elusive. We implemented femtosecond stimulated Raman spectroscopy (FSRS) and various time-resolved electronic spectroscopies, aided by quantum calculations, to dissect the cis- and trans-mKeima photocycle from ESPT, isomerization, to ground-state proton transfer in solution. This work manifests the power of FSRS with global analysis to resolve Raman fingerprints of intermediate states. Importantly, the deprotonated trans-isomer governs LSS emission at 620 nm, while the deprotonated cis-isomer's 520 nm emission is weak due to an ultrafast cis-to-trans isomerization. Complementary spectroscopic techniques as a table-top toolset are thus essential to study photochemistry in physiological environments. 相似文献
992.
Chunlin Xie Shengfang Liu Zefang Yang Huimin Ji Shuhan Zhou Hao Wu Chao Hu Yougen Tang Xiaobo Ji Qi Zhang Haiyan Wang 《Angewandte Chemie (International ed. in English)》2023,62(16):e202218612
Developing a highly stable and dendrite-free zinc anode is essential to the commercial application of zinc metal batteries. However, the understanding of zinc dendrites formation mechanism is still insufficient. Herein, for the first time, we discover that the interfacial heterogeneous deposition induced by lattice defects and epitaxial growth limited by residual stress are intrinsic and critical causes for zinc dendrite formation. Therefore, an annealing reconstruction strategy was proposed to eliminate lattice defects and stresses in zinc crystals, which achieve dense epitaxial electrodeposition of zinc anode. The as-prepared annealed zinc anodes exhibit dendrite-free morphology and enhanced electrochemical cycling stability. This work first proves that lattice defects and residual stresses are also very important factors for epitaxial electrodeposition of zinc in addition to crystal orientation, which can provide a new mechanism for future researches on zinc anode modification. 相似文献
993.
Dr. Liwei Dong Dr. Shijie Zhong Dr. Botao Yuan Dr. Yaqiang Li Dr. Jipeng Liu Dr. Yuanpeng Ji Dr. Dongjiang Chen Dr. Yuanpeng Liu Prof. Chunhui Yang Prof. Jiecai Han Prof. Weidong He 《Angewandte Chemie (International ed. in English)》2023,62(23):e202301073
Without excess Li, anode-free Li-metal batteries (AFLMBs) have been proposed as the most likely solution to realizing highly-safe and cost-effective Li-metal batteries. Nevertheless, short cyclic life puzzles conventional AFLMBs due to anodic dead Li accumulation with a local current concentration induced by irreversible electrolyte depletion, insufficient active Li reservoir and slow Li+ transfer at the solid electrolyte interphase (SEI). Herein, SrI2 is introduced into carbon paper (CP) current collector to effectively suppress dead Li through synergistic mechanisms including reversible I−/I3− redox reaction to reactivate dead Li, dielectric SEI surface with SrF2 and LiF to prevent electrolyte decomposition and highly ionic conductive (3.488 mS cm−1) inner layer of SEI with abundant LiI to enable efficient Li+ transfer inside. With the SrI2-modified current collector, the NCM532/CP cell delivers unprecedented cyclic performances with a capacity of 129.2 mAh g−1 after 200 cycles. 相似文献
994.
Chunlin Xie Shengfang Liu Wenxu Zhang Huimin Ji Shengqi Chu Qi Zhang Yougen Tang Haiyan Wang 《Angewandte Chemie (International ed. in English)》2023,62(28):e202304259
Rechargeable zinc metal batteries are promising for large-scale energy storage. However, their practical application is limited by harsh issues such as uncontrollable dendrite growth, low Coulombic efficiency, and poor temperature tolerance. Herein, a unique design strategy using γ-valerolactone-based electrolyte and nanocarbon-coated aluminum substrate was reported to solve the above problems. The electrolyte with extremely low freezing point and high thermal stability enables the symmetric cells with long cycle life over a wide temperature range (−50 °C to 80 °C) due to its ability to regulate zinc nucleation and preferential epitaxial growth. Besides, the nanocarbon-coated aluminum substrate can also promote a higher Coulombic efficiency over a wide temperature range in contrast to the low Coulombic efficiency of copper substrates with significant irreversible alloying reactions because this unique substrate with excellent chemical stabilization can homogenize the interfacial electron/ion distribution. The optimized zinc metal capacitors can operate stably under various temperature conditions (2000 cycles at 30 °C with 66 % depth of discharge and 1200 cycles at 80 °C with 50 % depth of discharge). This unique electrolyte and substrate design strategy achieves a robust zinc metal battery over a wide temperature range. 相似文献
995.
Dr. Fangping Ren Ji Xian Zhaowei Jia Zhichun Chen Hongjun Fu Prof. Dr. Rui Wang Prof. Dr. Wen-Dao Chu Prof. Dr. Xiaobo Pan Jincai Wu 《Angewandte Chemie (International ed. in English)》2023,62(44):e202306759
To synthesize high molecular weight poly(phenolic ester) via a living ring-opening polymerization (ROP) of cyclic phenolic ester monomers remains a critical challenge due to serious transesterification and back-biting reactions. Both phenolic ester bonds in monomer and polymer chains are highly active, and it is difficult so far to distinguish them. In this work, an unprecedented selectively bifunctional catalytic system of tetra-n-butylammonium chloride (TBACl) was discovered to mediate the syntheses of high molecular weight salicylic acid-based copolyesters via a living ROP of salicylate cyclic esters (for poly(salicylic methyl glycolide) (PSMG), Mn=361.8 kg/mol, Ð<1.30). Compared to previous catalysis systems, the side reactions were suppressed remarkably in this catalysis system because phenolic ester bond in monomer can be selectively cleaved over that in polymer chains during ROP progress. Mechanistic studies reveal that the halide anion and alkyl-quaternaryammonium cation work synergistically, where the alkyl-quaternaryammonium cation moiety interacts with the carbonyl group of substrates via non-classical hydrogen bonding. Moreover, these salicylic acid-based copolyesters can be recycled to dimeric monomer under solution condition, and can be recycled to original monomeric monomers without catalyst under sublimation condition. 相似文献
996.
Yuan-Zhe Cheng Wenyan Ji Peng-Yuan Hao Xue-Han Qi Xianxin Wu Xiao-Meng Dou Xin-Yue Bian Di Jiang Prof. Dr. Fa-Tang Li Prof. Dr. Xin-Feng Liu Dr. Dong-Hui Yang Dr. Xuesong Ding Prof. Dr. Bao-Hang Han 《Angewandte Chemie (International ed. in English)》2023,62(36):e202308523
Constructing a powerful photocatalytic system that can achieve the carbon dioxide (CO2) reduction half-reaction and the water (H2O) oxidation half-reaction simultaneously is a very challenging but meaningful task. Herein, a porous material with a crystalline topological network, named viCOF-bpy-Re, was rationally synthesized by incorporating rhenium complexes as reductive sites and triazine ring structures as oxidative sites via robust −C=C− bond linkages. The charge-separation ability of viCOF-bpy-Re is promoted by low polarized π-bridges between rhenium complexes and triazine ring units, and the efficient charge-separation enables the photogenerated electron–hole pairs, followed by an intramolecular charge-transfer process, to form photogenerated electrons involved in CO2 reduction and photogenerated holes that participate in H2O oxidation simultaneously. The viCOF-bpy-Re shows the highest catalytic photocatalytic carbon monoxide (CO) production rate (190.6 μmol g−1 h−1 with about 100 % selectivity) and oxygen (O2) evolution (90.2 μmol g−1 h−1) among all the porous catalysts in CO2 reduction with H2O as sacrificial agents. Therefore, a powerful photocatalytic system was successfully achieved, and this catalytic system exhibited excellent stability in the catalysis process for 50 hours. The structure–function relationship was confirmed by femtosecond transient absorption spectroscopy and density functional theory calculations. 相似文献
997.
Dr. Lina Xie Dr. Le Shi Dr. Kai Xiong Dr. Ruilin Guan Prof. Dr. Yu Chen Prof. Dr. Jiangang Long Prof. Liangnian Ji Prof. Dr. Hui Chao 《欧洲无机化学杂志》2023,26(15):e202300001
Two novel unsymmetrical Ir(III) complexes [Ir(ppy)2(N N)Cl2] (N N=2-(pyrazin-2-yl)naphtha[1,2-e][1,2,4]triazine, Ir1 ; 2-(pyrazin-2-yl)-4b,4b’-dihydroaceanthryleno[1,2-e][1,2,4]triazine, Ir2 ) were developed as chemotherapy agents. Ir1 was mainly located in mitochondria. In contrast, Ir2 accumulated in mitochondria but subsequently migrated to the nucleus. Ir1 and Ir2 showed cytotoxicity toward cancerous cells, especially the cisplatin-resistant ones, indicating their ability to overcome cisplatin resistance. Although both Ir1 and Ir2 disrupted mitochondrial metabolism, they showed different cell death mechanisms. Ir1 induced mitochondria-mediated apoptosis in cisplatin-resistant A549R cells. Ir2 was demonstrated to cause PARP-1 activated necroptosis in A549R cells. This study provides an experimental basis for the rational design of metal-based chemotherapeutic drugs. 相似文献
998.
Jiaying Duan Jiapeng Wang Liangpeng Hou Peixuan Ji Wusheng Zhang Jin Liu Xiaodong Zhu Zhixiang Sun Yanqing Ma Lei Ma 《Chemical record (New York, N.Y.)》2023,23(10):e202300120
Colloidal quantum dots display remarkable optical and electrical characteristics with the potential for extensive applications in contemporary nanotechnology. As an ideal instrument for examining surface topography and local density of states (LDOS) at an atomic scale, scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) has become indispensable approaches to gain better understanding of their physical properties. This article presents a comprehensive review of the research advancements in measuring the electronic orbits and corresponding energy levels of colloidal quantum dots in various systems using STM and STS. The first three sections introduce the basic principles of colloidal quantum dots synthesis and the fundamental methodology of STM research on quantum dots. The fourth section explores the latest progress in the application of STM for colloidal quantum dot studies. Finally, a summary and prospective is presented. 相似文献
999.
Dr. Dechao Zhang Dr. Yuxuan Liu Zhaoyu Sun Dr. Zhengbo Liu Dr. Xijun Xu Lei Xi Prof. Shaomin Ji Prof. Min Zhu Prof. Jun Liu 《Angewandte Chemie (International ed. in English)》2023,62(44):e202310006
The deployment of lithium metal anode in solid-state batteries with polymer electrolytes has been recognized as a promising approach to achieving high-energy-density technologies. However, the practical application of the polymer electrolytes is currently constrained by various challenges, including low ionic conductivity, inadequate electrochemical window, and poor interface stability. To address these issues, a novel eutectic-based polymer electrolyte consisting of succinonitrile (SN) and poly (ethylene glycol) methyl ether acrylate (PEGMEA) is developed. The research results demonstrate that the interactions between SN and PEGMEA promote the dissociation of the lithium difluoro(oxalato) borate (LiDFOB) salt and increase the concentration of free Li+. The well-designed eutectic-based PAN1.2-SPE (PEGMEA: SN=1: 1.2 mass ratio) exhibits high ionic conductivity of 1.30 mS cm−1 at 30 °C and superior interface stability with Li anode. The Li/Li symmetric cell based on PAN1.2-SPE enables long-term plating/stripping at 0.3 and 0.5 mA cm−2, and the Li/LiFePO4 cell achieves superior long-term cycling stability (capacity retention of 80.3 % after 1500 cycles). Moreover, Li/LiFePO4 and Li/LiNi0.6Co0.2Mn0.2O2 pouch cells employing PAN1.2-SPE demonstrate excellent cycling and safety characteristics. This study presents a new pathway for designing high-performance polymer electrolytes and promotes the practical application of high-stable lithium metal batteries. 相似文献
1000.
Jin-Jiang Zhang Kun Liu Yao Xiao Xiuling Yu Li Huang Hong-Jun Gao Ji Ma Xinliang Feng 《Angewandte Chemie (International ed. in English)》2023,62(41):e202310880
Graphene nanoribbons (GNRs) are considered promising candidates for next-generation nanoelectronics. In particular, GNR heterojunctions have received considerable attention due to their exotic topological electronic phases at the heterointerface. However, strategies for their precision synthesis remain at a nascent stage. Here, we report a novel chain-growth polymerization strategy that allows for constructing GNR heterojunction with N=9 armchair and chevron GNRs segments ( 9-AGNR/cGNR ). The synthesis involves a controlled Suzuki–Miyaura catalyst-transfer polymerization (SCTP) between 2-(6′-bromo-4,4′′-ditetradecyl-[1,1′:2′,1′′-terphenyl]-3′-yl) boronic ester ( M1 ) and 2-(7-bromo-9,12-diphenyl-10,11-bis(4-tetradecylphenyl)-triphenylene-2-yl) boronic ester ( M2 ), followed by the Scholl reaction of the obtained block copolymer ( poly-M1/M2 ) with controlled Mn (18 kDa) and narrow Đ (1.45). NMR and SEC analysis of poly-M1/M2 confirm the successful block copolymerization. The solution-mediated cyclodehydrogenation of poly-M1/M2 toward 9-AGNR/cGNR is unambiguously validated by FT-IR, Raman, and UV/Vis spectroscopies. Moreover, we also demonstrate the on-surface formation of pristine 9-AGNR/cGNR from the unsubstituted copolymer precursor, which is unambiguously characterized by scanning tunneling microscopy (STM). 相似文献