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51.
Yaqin Wang Xibo Zhang Kuan Chang Zhiying Zhao Jiayu Huang Prof. Qin Kuang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(16):e202104514
Exploring new catalytic strategies for achieving efficient CO2 hydrogenation under mild conditions is of great significance for environmental remediation. Herein, a composite photocatalyst Zr-based MOF encapsulated plasmonic AuPt alloy nanoparticles (AuPt@UiO-66-NH2) was successfully constructed for the efficient photothermal catalysis of CO2 hydrogenation. Under light irradiation at 150 °C, AuPt@UiO-66-NH2 achieved a CO production rate of 1451 μmol gmetal−1 h−1 with 91 % selectivity, which far exceeded those obtained by Au@Pt@UiO-66-NH2 with Pt shell on Au (599 μmol gmetal−1 h−1) and Au@UiO-66-NH2 (218 μmol gmetal−1 h−1). The outstanding performances of AuPt@UiO-66-NH2 were attributed to the synergetic effect originating from the plasmonic metal Au, doped active metal Pt, and encapsulation structure of UiO-66-NH2 shell. This work provides a new way for photothermal catalysis of CO2 and a reference for the design of high-performance plasmonic catalysts. 相似文献
52.
Guoxiu Qin Chen Xilin Xu Youning Li Fan Zhou Wenping Li Weizhe 《Journal of Radioanalytical and Nuclear Chemistry》2022,331(9):3545-3550
Journal of Radioanalytical and Nuclear Chemistry - When monitoring radioactive aerosol in the atmosphere, choosing a filter membrane with better surface collection characteristics and filtering... 相似文献
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54.
The chemical nature of the DNA bases is an important factor in sequence-mediated association of DNA molecules. Nucleotides are the fundamental DNA elements and the base identity impacts the molecular properties of nucleotide fragments. It is interesting to study the fundamental nature of nucleotides in DNA, on the basis of base-specific interactions, association, and modes of standard atomic or molecular interactions. With all-atom molecular dynamics simulations of model dinucleotide and tetranucleotide systems having single-stranded dinucleotide or tetranucleotide fragments of varying sequences, we show how the base identity and interactions between the different bases as well as water may affect the clustering properties of nucleotides fragments in an ionic solution. Sequence-dependent differential interactions between the nucleotide fragments, ionic concentration, and elevated temperature are found to influence the clustering properties and dynamics of association. Well-known epigenetic modification of DNA, that is, cytosine methylation also promotes dinucleotide clustering in solution. These observations point to one possible chemical nature of the DNA bases, as well as the importance of the base pairing, base stacking, and ionic interactions in DNA structure formation, and DNA sequence-mediated association. Sequence- and the ionic environment-mediated self-association properties of the dinucleotides indicate its great potential to develop biological nanomaterials for desired applications. 相似文献
55.
Miao Zhu Qin Zhou He Cheng Prof. Dr. Ye Sha Prof. Dr. Vladimir I. Bregadze Prof. Dr. Hong Yan Prof. Dr. Zhe Sun Prof. Dr. Xiang Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(1):e202213470
The combination of carbon-based nanohoops with other functional organic molecular structures should lead to the design of new molecular configurations with interesting properties. Here, necklace-like nanohoops embedded with carborane were synthesized for the first time. The unique deboronization of o-carborane has led to the facile preparation of ionic nanohoop compounds. Nanohoops functionalized by nido-o-carborane show excellent fluorescence emission, with a solution quantum yield of up to 90.0 % in THF and a solid-state quantum efficiency of 87.3 %, which opens an avenue for the applications of the nanohoops in OLEDs and bioimaging. 相似文献
56.
Haojie Zhu Fangcheng Wang Lu Peng Tingting Qin Prof. Feiyu Kang Prof. Cheng Yang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(2):e202212439
Rechargeable aqueous sodium ion batteries (ASIBs) are rising as an important alternative to lithium ion batteries, owing to their safety and low cost. Metal anodes show a high theoretical capacity and nonselective hydrated ion insertion for ASIBs, yet their large volume expansion and sluggish reaction kinetics resulted in poor electrochemical stability. Herein, we demonstrate an electrode cyclability enhancement mechanism by inlaying bismuth (Bi) nanoparticles on graphene nanosheets through chemical bond, which is achieved by a unique laser induced compounding method. This anchored metal-graphene heterostructure can effectively mitigate volume variation, and accelerate the kinetic capability as the active Bi can be exposed to the electrolyte. Our method can achieve a reversible capacity of 122 mAh g−1 at a large current density of 4 A g−1 for over 9500 cycles. This finding offers a desirable structural design of other metal anodes for aqueous energy storage systems. 相似文献
57.
Shang Li Yuxing Xu Dr. Hengwei Wang Prof. Botao Teng Dr. Qin Liu Dr. Qiuhua Li Lulu Xu Xinyu Liu Prof. Junling Lu 《Angewandte Chemie (International ed. in English)》2023,62(8):e202218167
Tuning the coordination environments of metal single atoms (M1) in single-atom catalysts has shown large impacts on catalytic activity and stability but often barely on selectivity in thermocatalysis. Here, we report that simultaneously regulating both Rh1 atoms and ZrO2 support with alkali ions (e.g., Na) enables efficient switching of the reaction products from nearly 100 % CH4 to above 99 % CO in CO2 hydrogenation in a wide temperature range (240–440 °C) along with a record high activity of 9.4 molCO gRh−1 h−1 at 300 °C and long-term stability. In situ spectroscopic characterization and theoretical calculations unveil that alkali ions on ZrO2 change the surface intermediate from formate to carboxy species during CO2 activation, thus leading to exclusive CO formation. Meanwhile, alkali ions also reinforce the electronic Rh1-support interactions, endowing the Rh1 atoms more electron deficient, which improves the stability against sintering and inhibits deep hydrogenation of CO to CH4. 相似文献
58.
Shuai Zhang Hancheng Qin Shuwen Cheng Yue Zhang Nan Gao Prof. Meining Zhang 《Angewandte Chemie (International ed. in English)》2023,62(16):e202300083
Reactive oxygen species (ROS)-based therapeutic strategies play an important role in cancer treatment. However, in situ, real-time and quantitative analysis of intracellular ROS in cancer treatment for drug screening is still a challenge. Herein we report one selective hydrogen peroxide (H2O2) electrochemical nanosensor, which is prepared by electrodeposition of Prussian blue (PB) and polyethylenedioxythiophene (PEDOT) onto carbon fiber nanoelectrode. With the nanosensor, we find that the level of intracellular H2O2 increases with NADH treatment and that increase is dose-dependent to the concentration of NADH. High-dose of NADH (above 10 mM) can induce cell death and intratumoral injection of NADH is validated for inhibiting tumor growth in mice. This study highlights the potential of electrochemical nanosensor for tracking and understanding the role of H2O2 in screening new anticancer drug. 相似文献
59.
Wenbo Dong Zhiying Qin Kuixing Wang Yueyuan Xiao Xiangyang Liu Shijie Ren Longyu Li 《Angewandte Chemie (International ed. in English)》2023,62(5):e202216073
Imine-linked covalent organic frameworks (COFs) have been extensively studied in photocatalysis because of their easy synthesis and excellent crystallinity. The effect of imine-bond orientation on the photocatalytic properties of COFs, however, is still rarely studied. Herein, we report two novel COFs with different orientations of imine bonds using oligo(phenylenevinylene) moieties. The COFs showed similar structures but great differences in their photoelectric properties. COF-932 demonstrated a superior hydrogen evolution performance compared to COF-923 when triethanolamine was used as the sacrificial agent. Interestingly, the use of ascorbic acid led to the protonation of the COFs, further altering the direction of electron transfer. The photocatalytic performances were increased to 23.4 and 0.73 mmol g−1 h−1 for protonated COF-923 and COF-932, respectively. This study provides a clear strategy for the design of imine-linked COF-based photocatalysts and advances the development of COFs. 相似文献
60.
Bing Qin Zhi-Long Yu Jin Huang Yu-Feng Meng Rui Chen Zhi Chen Shu-Hong Yu 《Angewandte Chemie (International ed. in English)》2023,62(5):e202214809
Cellulose aerogels are plagued by intermolecular hydrogen bond-induced structural plasticity, otherwise rely on chemicals modification to extend service life. Here, we demonstrate a petrochemical-free strategy to fabricate superelastic cellulose aerogels by designing hierarchical structures at multi scales. Oriented channels consolidate the whole architecture. Porous walls of dehydrated cellulose derived from thermal etching not only exhibit decreased rigidity and stickiness, but also guide the microscopic deformation and mitigate localized large strain, preventing structural collapse. The aerogels show exceptional stability, including temperature-invariant elasticity, fatigue resistance (∼5 % plastic deformation after 105 cycles), high angular recovery speed (1475.4° s−1), outperforming most cellulose-based aerogels. This benign strategy retains the biosafety of biomass and provides an alternative filter material for health-related applications, such as face masks and air purification. 相似文献