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971.
Meihong Zhang Yuqian Fang Shuai Yuan Liyi Shi Zhuyi Wang Yi Wang Jiefang Zhu Yin Zhao 《Surface and interface analysis : SIA》2023,55(1):63-70
The graphitic carbon nitride (g-C3N4) materials with many intriguing properties have attracted much attention in photocatalysis. The photocatalytic activity of g-C3N4 is hindered by serious aggregation and limited exposed active sites. Herein is shown that nanosized g-C3N4 can be simply obtained by a superfast high-pressure homogenization approach. The high-pressure homogenization treatment can provide strong force to cut and/or to exfoliate the bulk g-C3N4 into nanosized g-C3N4 with good dispersion. Moreover, choosing different solvents during treatment can cause a different surface structure of as-prepared nanosized g-C3N4. In addition, the narrow bandgap properties, the high photogenerated charge carrier separation, and the transport abilities are achieved in as-prepared nanosized g-C3N4 because of the retaining conjugated C3N4 system. Specifically, the photocatalytic activities of as-prepared nanosized g-C3N4 have been significantly enhanced in terms of degradation of organic dye Rhodamine B (RhB) under visible light irradiation (10 times higher than that of bulk g-C3N4). These findings can provide a promising and simple approach to the exfoliation, nanonization, and surface functionalization of 2D layered materials. 相似文献
972.
Mingxia Guo Long Fang Linlin Zhang Mingzhu Li Meiyu Cong Xiping Guan Chuanwei Shi ChunLei Gu Xia Liu Yong Wang Xin Ding 《Angewandte Chemie (International ed. in English)》2023,62(13):e202217635
Atomically dispersed Fe was designed on TiO2 and explored as a Janus electrocatalyst for both nitrogen oxidation reaction (NOR) and nitrogen reduction reaction (NRR) in a two-electrode system. Pulsed electrochemical catalysis (PE) was firstly involved to inhibit the competitive hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Excitingly, an unanticipated yield of 7055.81 μmol h−1 g−1cat. and 12 868.33 μmol h−1 g−1cat. were obtained for NOR and NRR at 3.5 V, respectively, 44.94 times and 7.8 times increase in FE than the conventional constant voltage electrocatalytic method. Experiments and density functional theory (DFT) calculations revealed that the single-atom Fe could stabilize the oxygen vacancy, lower the energy barrier for the vital rupture of N≡N, and result in enhanced N2 fixation performance. More importantly, PE could effectively enhance the N2 supply by reducing competitive O2 and H2 agglomeration, inhibit the electrocatalytic by-product formation for longstanding *OOH and *H intermediates, and promote the non-electrocatalytic process of N2 activation. 相似文献
973.
Shibing Zheng Dongjie Shi Tianjiang Sun Letian Zhang Weijia Zhang Yixin Li Zhenbo Guo Zhanliang Tao Jun Chen 《Angewandte Chemie (International ed. in English)》2023,62(9):e202217710
High-capacity small organic materials are plagued by their high solubility. Here we proposed constructing hydrogen bond networks (HBN) via intermolecular hydrogen bonds to suppress the solubility of active material. The illustrated 2, 7- diamino-4, 5, 9, 10-tetraone (PTO-NH2) molecule with intermolecular hydrogen (H) bond between O in −C=O and H in −NH2, which make PTO-NH2 presents transverse two-dimensional extension and longitudinal π–π stacking structure. In situ Fourier transform infrared spectroscopy (FTIR) has tracked the reversible evolution of H-bonds, further confirming the existence of HBN structure can stabilize the intermediate 2-electron reaction state. Therefore, PTO-NH2 with HBN structure has higher active site utilization (95 %), better cycle stability and rate performance. This study uncovers the H-bond effect and evolution during the electrochemical process and provides a strategy for materials design. 相似文献
974.
Jieshuai Xiao Prof. Dr. Minyan Wang Xuwen Yin Shuo Yang Pei Gu Xueli Lv Dr. Yue Zhao Prof. Dr. Zhuangzhi Shi 《Angewandte Chemie (International ed. in English)》2023,62(19):e202300743
Transition-metal-catalyzed enantioselective addition of aryl organometallic reagents to imines has emerged as one of the most powerful tools for the formation of optically active diarylmethylamines. Here, we report the first asymmetric reductive (hetero)arylations of imines using aryl and heteroaryl halides enabled by a chiral cobalt-bisphosphine catalyst. This approach shows good functional group compatibility and complements the reported strategy without use of organometallic reagents. Mechanistic investigations supported that aryl-cobalt, instead of an arylzinc reagent, was formed in situ in this reductive aryl-addition event. 相似文献
975.
Dr. Zhao Gao Lulu Shi Fei Yan Yifei Han Wei Yuan Prof. Wei Tian 《Angewandte Chemie (International ed. in English)》2023,62(21):e202302274
Two-dimensional (2D) organic polymers have recently received considerable interest, especially those whose architectures are held together via supramolecular engineering. However, current approaches toward supramolecular 2D structures usually suffer from mutual interference of noncovalent interactions and lack of intrinsic functions. Herein, we report well-regulated 2D supramolecular polymers (2DSPs) through an aromatics-selective recognition strategy of cation-π and donor-acceptor (D-A) motifs, which are derived from C4-symmetric cationic monomers and electron-withdrawing molecules. By subtly designing the strength and direction of noncovalent driving forces, the mutual interference between cation-π and D-A interactions is effectively avoided, enabling the construction of 2DSPs in aqueous solution. On this basis, the resultant 2DSPs possess boosted photocatalytic hydrogen evolution activity at a rate of 600 μmol g−1 h−1, which is mainly ascribed to the specific stacking mode of cation-π/D-A motifs and the ordered 2D structures. 相似文献
976.
Reversible Li Plating on Graphite Anodes through Electrolyte Engineering for Fast-Charging Batteries
Xinyang Yue Jing Zhang Yongteng Dong Yuanmao Chen Zhangqin Shi Xuejiao Xu Xunlu Li Prof. Zheng Liang 《Angewandte Chemie (International ed. in English)》2023,62(19):e202302285
The difficulties to identify the rate-limiting step cause the lithium (Li) plating hard to be completely avoided on graphite anodes during fast charging. Therefore, Li plating regulation and morphology control are proposed to address this issue. Specifically, a Li plating-reversible graphite anode is achieved via a localized high-concentration electrolyte (LHCE) to successfully regulate the Li plating with high reversibility over high-rate cycling. The evolution of solid electrolyte interphase (SEI) before and after Li plating is deeply investigated to explore the interaction between the lithiation behavior and electrochemical interface polarization. Under the fact that Li plating contributes 40 % of total lithiation capacity, the stable LiF-rich SEI renders the anode a higher average Coulombic efficiency (99.9 %) throughout 240 cycles and a 99.95 % reversibility of Li plating. Consequently, a self-made 1.2-Ah LiNi0.5Mn0.3Co0.2O2 | graphite pouch cell delivers a competitive retention of 84.4 % even at 7.2 A (6 C) after 150 cycles. This work creates an ingenious bridge between the graphite anode and Li plating, for realizing the high-performance fast-charging batteries. 相似文献
977.
Dr. Huanhuan Shi Prof. Mengmeng Li Shuai Fu Dr. Christof Neumann Dr. Xiaodong Li Dr. Wenhui Niu Yunji Lee Prof. Mischa Bonn Dr. Hai I. Wang Prof. Andrey Turchanin Dr. Ali Shaygan Nia Dr. Sheng Yang Prof. Xinliang Feng 《Angewandte Chemie (International ed. in English)》2023,62(28):e202303929
Two-dimensional van der Waals heterostructures (2D vdWHs) have recently gained widespread attention because of their abundant and exotic properties, which open up many new possibilities for next-generation nanoelectronics. However, practical applications remain challenging due to the lack of high-throughput techniques for fabricating high-quality vdWHs. Here, we demonstrate a general electrochemical strategy to prepare solution-processable high-quality vdWHs, in which electrostatic forces drive the stacking of electrochemically exfoliated individual assemblies with intact structures and clean interfaces into vdWHs with strong interlayer interactions. Thanks to the excellent combination of strong light absorption, interfacial charge transfer, and decent charge transport properties in individual layers, thin-film photodetectors based on graphene/In2Se3 vdWHs exhibit great promise for near-infrared (NIR) photodetection, owing to a high responsivity (267 mA W−1), fast rise (72 ms) and decay (426 ms) times under NIR illumination. This approach enables various hybrid systems, including graphene/In2Se3, graphene/MoS2 and graphene/MoSe2 vdWHs, providing a broad avenue for exploring emerging electronic, photonic, and exotic quantum phenomena. 相似文献
978.
979.
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
980.
Ziwei Xu Hongwei Dong Dr. Wanmiao Gu Dr. Zhen He Fengming Jin Dr. Chengming Wang Dr. Qing You Prof. Dr. Jin Li Prof. Dr. Haiteng Deng Dr. Lingwen Liao Dr. Dong Chen Prof. Dr. Jun Yang Prof. Dr. Zhikun Wu 《Angewandte Chemie (International ed. in English)》2023,62(39):e202308441
Lattice tuning at the ≈1 nm scale is fascinating and challenging; for instance, lattice compression at such a minuscule scale has not been observed. The lattice compression might also bring about some unusual properties, which waits to be verified. Through ligand induction, we herein achieve the lattice compression in a ≈1 nm gold nanocluster for the first time, as detected by the single-crystal X-ray crystallography. In a freshly synthesized Au52(CHT)28 (CHT=S-c−C6H11) nanocluster, the lattice distance of the (110) facet is found to be compressed from 4.51 to 3.58 Å at the near end. However, the lattice distances of the (111) and (100) facets show no change in different positions. The lattice-compressed nanocluster exhibits superior electrocatalytic activity for the CO2 reduction reaction (CO2RR) compared to that exhibited by the same-sized Au52(TBBT)32 (TBBT=4-tert-butyl-benzenethiolate) nanocluster and larger Au nanocrystals without lattice variation, indicating that lattice tuning is an efficient method for tailoring the properties of metal nanoclusters. Further theoretical calculations explain the high CO2RR performance of the lattice-compressed Au52(CHT)28 and provide a correlation between its structure and catalytic activity. 相似文献