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71.
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
72.
Dr. Wenhui Niu Dr. Yubin Fu Gianluca Serra Kun Liu Jörn Droste Yeonju Lee Zhitian Ling Dr. Fugui Xu Dr. José D. Cojal González Dr. Andrea Lucotti Prof. Dr. Jürgen P. Rabe Prof. Dr. Michael Ryan Hansen Prof. Dr. Wojciech Pisula Prof. Dr. Paul W. M. Blom Prof. Dr. Carlos-Andres Palma Prof. Dr. Matteo Tommasini Prof. Dr. Yiyong Mai Dr. Ji Ma Prof. Dr. Xinliang Feng 《Angewandte Chemie (International ed. in English)》2023,62(35):e202305737
The incorporation of nanopores into graphene nanostructures has been demonstrated as an efficient tool in tuning their band gaps and electronic structures. However, precisely embedding the uniform nanopores into graphene nanoribbons (GNRs) at the atomic level remains underdeveloped especially for in-solution synthesis due to the lack of efficient synthetic strategies. Herein we report the first case of solution-synthesized porous GNR ( pGNR ) with a fully conjugated backbone via the efficient Scholl reaction of tailor-made polyphenylene precursor ( P1 ) bearing pre-installed hexagonal nanopores. The resultant pGNR features periodic subnanometer pores with a uniform diameter of 0.6 nm and an adjacent-pores-distance of 1.7 nm. To solidify our design strategy, two porous model compounds ( 1 a , 1 b ) containing the same pore size as the shortcuts of pGNR , are successfully synthesized. The chemical structure and photophysical properties of pGNR are investigated by various spectroscopic analyses. Notably, the embedded periodic nanopores largely reduce the π-conjugation degree and alleviate the inter-ribbon π–π interactions, compared to the nonporous GNRs with similar widths, affording pGNR with a notably enlarged band gap and enhanced liquid-phase processability. 相似文献
73.
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
74.
Hui Liang Manlin Lu Zafar Mahmood Zheng Li Zeduan Chen Guowei Chen Prof. Ming-De Li Prof. Yanping Huo Prof. Shaomin Ji 《Angewandte Chemie (International ed. in English)》2023,62(44):e202312600
The design of efficient heavy atom-free triplet photosensitizers (PSs) based on through bond charge transfer (TBCT) features is a formidable challenge due to the criteria of orthogonal donor-acceptor geometry. Herein, we propose using parallel (face-to-face) conformation carbazole-bodipy donor-acceptor dyads (BCZ-1 and BCZ-2) featuring through space intramolecular charge transfer (TSCT) process as efficient triplet PS. Efficient intersystem crossing (ΦΔ=61 %) and long-lived triplet excited state (τT=186 μs) were observed in the TSCT dyad BCZ-1 compared to BCZ-3 (ΦΔ=0.4 %), the dyad involving TBCT, demonstrating the superiority of the TSCT approach over conventional donor-acceptor system. Moreover, the transient absorption study revealed that TSCT dyads have a faster charge separation and slower intersystem crossing process induced by charge recombination compared to TBCT dyad. A long-lived charge-separated state (CSS) was observed in the BCZ-1 (τCSS=24 ns). For the first time, the TSCT dyad was explored for the triplet-triplet annihilation upconversion, and a high upconversion quantum yield of 11 % was observed. Our results demonstrate a new avenue for designing efficient PSs and open up exciting opportunities for future research in this field. 相似文献
75.
Dr. Ying-Jie Sun Wen-Da Chen Dr. Ji Liu Jun-Jin Li Yu Zhang Wei-Qi Cai Prof. Li Liu Xin-Jing Tang Jian Hou Prof. Ming Wang Prof. Liang Cheng 《Angewandte Chemie (International ed. in English)》2023,62(5):e202212413
The CRISPR/Cas system is one of the most powerful tools for gene editing. However, approaches for precise control of genome editing and regulatory events are still desirable. Here, we report the spatiotemporal and efficient control of CRISPR/Cas9- and Cas12a-mediated editing with conformationally restricted guide RNAs (gRNAs). This approach relied on only two or three pre-installed photo-labile substituents followed by an intramolecular cyclization, representing a robust synthetic method in comparison to the heavily modified linear gRNAs that often require extensive screening and time-consuming optimization. This tactic could direct the precise cleavage of the genes encoding green fluorescent protein (GFP) and the vascular endothelial growth factor A (VEGFA) protein within a predefined cutting region without notable editing leakage in live cells. We also achieved light-mediated myostatin (MSTN) gene editing in embryos, wherein a new bow-knot-type gRNA was constructed with excellent OFF/ON switch efficiency. Overall, our work provides a significant new strategy in CRISPR/Cas editing with modified circular gRNAs to precisely manipulate where and when genes are edited. 相似文献
76.
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
77.
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
78.
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
79.
Tuoya Naren Gui-Chao Kuang Ruheng Jiang Piao Qing Hao Yang Jialin Lin Yuejiao Chen Weifeng Wei Xiaobo Ji Libao Chen 《Angewandte Chemie (International ed. in English)》2023,62(26):e202305287
Lithium (Li) metal anodes have the highest theoretical capacity and lowest electrochemical potential making them ideal for Li metal batteries (LMBs). However, Li dendrite formation on the anode impedes the proper discharge capacity and practical cycle life of LMBs, particularly in carbonate electrolytes. Herein, we developed a reactive alternative polymer named P(St-MaI) containing carboxylic acid and cyclic ether moieties which would in situ form artificial polymeric solid electrolyte interface (SEI) with Li. This SEI can accommodate volume changes and maintain good interfacial contact. The presence of carboxylic acid and cyclic ether pendant groups greatly contribute to the induction of uniform Li ion deposition. In addition, the presence of benzyl rings makes the polymer have a certain mechanical strength and plays a key role in inhibiting the growth of Li dendrites. As a result, the symmetric Li||Li cell with P(St-MaI)@Li layer can stably cycle for over 900 h under 1 mA cm−2 without polarization voltage increasing, while their Li||LiFePO4 full batteries maintain high capacity retention of 96 % after 930 cycles at 1C in carbonate electrolytes. The innovative strategy of artificial SEI is broadly applicable in designing new materials to inhibit Li dendrite growth on Li metal anodes. 相似文献
80.
Xiaoyang Cheng Xiaotian Jiang Shuhu Yin Lifei Ji Yani Yan Guang Li Rui Huang Prof. Chongtai Wang Prof. Honggang Liao Prof. Yanxia Jiang Prof. Shigang Sun 《Angewandte Chemie (International ed. in English)》2023,62(34):e202306166
To achieve the Fe−N−C materials with both high activity and durability in proton exchange membrane fuel cells, the attack of free radicals on Fe−N4 sites must be overcome. Herein, we report a strategy to effectively eliminate radicals at the source to mitigate the degradation by anchoring CeO2 nanoparticles as radicals scavengers adjacent (Scaad-CeO2) to the Fe−N4 sites. Radicals such as ⋅OH and HO2⋅ that form at Fe−N4 sites can be instantaneously eliminated by adjacent CeO2, which shortens the survival time of radicals and the regional space of their damage. As a result, the CeO2 scavengers in Fe−NC/Scaad-CeO2 achieved ∼80 % elimination of the radicals generated at the Fe−N4 sites. A fuel cell prepared with the Fe−NC/Scaad-CeO2 showed a smaller peak power density decay after 30,000 cycles determined with US DOE PGM-relevant AST, increasing the decay of Fe−NCPhen from 69 % to 28 % decay. 相似文献