Nanomaterials
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2022
·Vol. 12
·期 2
·209
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IF 5.719
Aiqing Ma,Hui Ran,Jiaxing Wang,Rui Ding,Chengyu Lu,Lanlan Liu,Yingmei Luo,Huaqing Chen,Ting Yin
Sonodynamic therapy (SDT), as a novel cancer therapy strategy, might be a promising approach due to the depth-penetration property in tissue. Sonosensitizers are the key element for efficient SDT. However, the development of sonosensitizers with strong sonosensitization efficacy is still a significant challenge. Herein, an urchin-shaped copper-based metalloporphyrin liposome nanosystem (FA–L–CuPP) is constructed and identified as an excellent sonosensitizer. Under ultrasound (US) irradiation, FA–L–CuPP can be highly excited to generate several reactive oxygen species (ROS), such as singlet oxygen (1O2) and free radicals (⋅OH). The molecular orbital distribution calculations reveal that a strong intramolecular charge transfer might occur in the CuPP complex under US irradiation, which could afford enough energy to the surrounding O2and H2O to concert1O2, O2−and ⋅OH. Working as “ammunitions”, the largely produced ROS can kill 4T1 tumor cells, effectively inhibiting tumor growth. This work provides an urchin-shaped nanosonosensitizer based on a copper complex, which might provide an idea to design a novel sonosensitizer for noninvasive and precise SDT antitumor applications.Keywords:sonodynamic therapy;copper-based metalloporphyrin;sonosensitizer;urchin-shaped;noninvasive therapy
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FUEL
·
2022
·
IF 8.035
Yanbin Sun,Jianfeng Zheng,Jiajia Xu,Kaixuan Yang,Zhiguo Zhu,Ting Su,Hui Ge,Wanzhong Ren,Hongying Lü
Aerobic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) is an environmentally sustainable, economically feasible, but substantially challenging conversion owing to the high energy barrier of O 2 activation. Herein, we report a catalyst with Mo 5+ connected to the oxygen vacancies (Mo 5+ -□) in Anderson-type polyoxometalate (POM) [(C 18 H 37 ) 2 N(CH 3 ) 2 ] 6 Mo 7 O 24 for oxidizing HMF to DFF. The resultant catalyst with high Mo 5+ content presents superior HMF oxidation performance, delivering a > 99% DFF selectivity with complete HMF conversion. Mechanistic studies and density functional theory (DFT) calculations reveal that the Mo 5+ -□ species in the catalyst facilitate O 2 activation and HMF oxidation. Moreover, the catalyst exhibits outstanding catalytic stability during the aerobic oxidation of HMF to DFF.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2022
·Vol. 46
·期 7
·8949-8961
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IF 4.672
Xinfei Fan,Haichao Mu,Yuanlu Xu,Chengwen Song,Yanming Liu
Summary Solar-driven interfacial evaporation is an emerging environmentally-friendly technology to produce freshwater, but the current interface evaporators are restricted by their high cost, complex fabrication processes, and low resistance to environmental conditions. Here, a low-cost and high-efficient evaporator was prepared simply by modifying natural wax gourd with polydopamine (PDA) and silver nanoparticles (AgNPs). The prepared AgNPs-PDA-wax gourd exhibited excellent light absorption (>94%) in the whole solar spectrum (300-2500 nm). Under 1 sun illumination, the prepared evaporator achieved an extraordinary evaporation rate of 1.70 kg m −2 h −1 (efficiency of 83.21%), which was 3.78 and 1.21 times higher than the rates of natural wax gourd and PDA-wax gourd, respectively. Such excellent performance was mainly attributed to the synergic light-to-heat conversion capability between localized surface plasmon resonance effect from AgNPs and enhanced light-adsorption ability from PDA. Due to the presence of AgNPs, the final evaporator also displayed a fascinating antibacterial behavior for both E. coli and S. aureus even during evaporating actual lake water. Meanwhile, the AgNPs-PDA-wax gourd presented good durability during 10-cycled experiments, seawater desalination, dye water purification and some extreme conditions (acid, alkaline and freezing). These results suggested the great potential for future practical applications of such biomass solar evaporators.
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Nanoscale
·
2022
·Vol. 14
·期 13
·4957-4964
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IF 8.307
Tingshi Zhang,Chengkai Yang,Borong Li,Yuanming Zhang,Zanyong Zhuang,Yan Yu
Preparation of high-density and atomically-dispersed clusters is of great importance yet remains a formidable challenge, which precludes rational design of high-performance, ultrasmall heterogeneous catalysts for alleviating the energy and environmental crises. In this study, we demonstrated an appealing non-equilibrium growth model to give sub-2 nm CuO clusters not from the growth of nuclei but from the top-down growth of metastable bulk crystals. These CuO clusters have high density and intriguingly uniform orientation, and are atomically scattered on an inactive ultrathin AlOOH substrate, which has been driven by the lattice matching between the CuO clusters and the utlrathin AlOOH substrate. The catalytic activity of CuO clusters, with the hydrogenation of 4-nitrophenol as a model reaction, proved to be extremely efficient and showed a rate constant of 130.0 s−1 g−1, outperforming the commercial Pd/C catalysts and reported state-of-the-art noble-metal catalysts (1.89–117.2 s−1 g−1). These clusters have abundant interfacial oxygen vacancies (OVs) whose concentration can be regulated, and the OVs are found to be essential, according to density functional theory (DFT) calculations, in reducing the energy barrier of catalytic reduction and significantly boosting the catalytic reaction. These findings could add to the library of crystals downsized to the atomic level and demonstrate how engineering point defects on the sub-nanometer materials help design high-efficient catalysts.
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CRYSTENGCOMM
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2022
·Vol. 24
·期 11
·2100-2106
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IF 3.756
Song-Tao Dong,Zhuang Fu,Miaocheng Yu,Jia-Ling Jiang,Xiaoyun Jin,Yu-Hang Guo,Lei Wang,Ya-Mei Zhang
Self-powered photoelectric devices as a new type of sensor without an external power source have a great potential advantage in the next generation of portable and wearable personal devices. The design of those devices is normally based on three kinds of strategies: a p–n junction, the Schottky junction and ferroelectric polarization. Here, a novel solution based on ion migration induced self-powered photodetectors was explored. In this work, high quality halide perovskite FAPbBr3 crystals were grown by an inverse temperature crystallization (ITC) method. An irreversible ion migration was intentionally created using a symmetrically structured Au/FAPbBr3/Au device. The resulting built-in electric field and energy band bending were proved using electrical measurements in the dark and under light. Finally, the response of the ion migration induced self-powered FAPbBr3 detector was investigated with the values of R (∼0.18 mA W−1) and EQE (∼0.055%) under light with a power density of 1 mW cm−2 and a wavelength of 397 nm. Our investigation demonstrates that ion migration, which is normally deemed a detrimental factor for device stability, can be intentionally used for self-powered photoelectric devices.
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Materials
·
2022
·Vol. 15
·期 5
·1719
·
IF 3.748
Jingjing Wang,Junjie Ren,Qinglin Tang,Xinzhi Wang,Yao Wang,Yanxin Wang,Zhonglin Du,Wei Wang,Linjun Huang,Laurence A. Belfiore,Jianguo Tang
Copper (II) complexes containing mixed ligands were synthesized in dimethyl formamide (DMF). The intense cyan emission at an ambient temperature is observed for solid copper (II) complexes with salicylic acid and a 12% quantum yield with a fluorescent lifetime of approximately 10 ms. Hence, copper (II) complexes with salicylic acid are excellent candidates for photoactive materials. Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) reveal that the divalent copper metal centers coordinate with the nitrogen and oxygen lone pairs of conjugate ligands. XPS binding energy trends for core electrons in lower-lying orbitals are similar for all three copper (II) complexes: nitrogen 1s and oxygen 1s binding energies increase relative to those for undiluted ligands, and copper 2p3/2binding energies decrease relative to that for CuCl2. The thermal behavior of these copper complexes reveals that the thermal stability is characterized by the following pattern: Cu(1,10-phenanthroline)(salicylic acid) > Cu(1,10-phenanthroline)(2,2’-bipyridine) > Cu(1,10-phenanthroline)(1-benzylimidazole)2.Keywords:copper (II) complex;luminescent materials;benzylimidazole;bipyridine;salicylic acid;spectroscopy
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2022
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IF 4.52
Mi Wei,Huiyin Liu,Zhilin Zhang,Xuemin Chen,Zhenhua Guo,Xiangxia Yang
As a specialty food that is medicinal and edible, Anoectochilus roxburghii contains many active ingredients. Herein, optimal conditions to preserve A. roxburghii samples and obtain high physiological activity have been studied. The contents of polysaccharides , kinsenoside, and flavonoids of A. roxburghii were monitored during post-harvest storage for a period of eight months at 25 °C with different packaging methods such as stacking, multilayer pocket and vacuum. The results indicated that packaging method and storage time have significant influences on the preservation of active compounds. Polysaccharides, kinsenoside and flavonoids exhibited a general descending trend during storage for a period of eight months in all packaging conditions. However, the vacuum method is more effective in preservation of polysaccharides and flavonoids than stacking and multilayer pockets methods due to the lower activity of microbial community under vacuum condition. Interestingly, kinsenoside, a characteristic compound of A. roxburghii , responsive for the hypoglycemic function, was not affected by packaging methods. This is because kinsenoside was mainly affected by plant endogenous enzymes instead of microbial community. Two-factor variance analysis showed that packaging method and storage time have significant interactions in preservation. It was further disclosed that the changes of active components were closely related to the plant endogenous enzymes, microbial community and their functions. The findings in this study will shed some light on the storage of A. roxburghii and other herb products.
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JOURNAL OF CHEMICAL PHYSICS
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2023
·Vol. 158
·期 20
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IF 4.4
Zhang Qin,Zhou Zhongneng,Deng Bodan,Wang Bingyao,Kang Xiu-Wen,Chen Jinquan,Ding Bei,Zhong Dongping
Phototriggers are useful molecular tools to initiate reactions in enzymes by light for the purpose of photoenzymatic design and mechanistic investigations. Here, we incorporated the non-natural amino acid 5-cyanotryptophan (W 5CN ) in a polypeptide scaffold and resolved the photochemical reaction of the W 5CN –W motif using femtosecond transient UV/Vis and mid-IR spectroscopy. We identified a marker band of ∼2037 cm −1 from the CN stretch of the electron transfer intermediate W 5CN ·− in the transient IR measurement and found UV/Vis spectroscopic evidence for the W ·+ radical at 580 nm. Through kinetic analysis, we characterized that the charge separation between the excited W 5CN and W occurs in 253 ps, with a charge-recombination lifetime of 862 ps. Our study highlights the potential use of the W 5CN –W pair as an ultrafast phototrigger to initiate reactions in enzymes that are not light-sensitive, making downstream reactions accessible to femtosecond spectroscopic detection.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2023
·
IF 3.8
Fuhua Wei,Haiyan Liu,Qinhui Ren,Lu Yang,Lan Qin,Hongliang Chen,Yufu Ma,Zhao Liang,Siyuan Wang
Zr-MOF was prepared under solvothermal conditions using zirconium acetate as the metal ion and 2,5-dihydroxyterephthalic acid as the organic ligand. It was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and thermogravimetry (TG). Zr-MOF was used as an adsorbent to remove norfloxacin from aqueous solutions. The experimental results were fitted, and the results showed that the pseudo-second-order kinetics model was appropriate for studying the removal of norfloxacin. We investigated the adsorption capacity of Zr-MOF under different masses, concentrations, and pH values. At pH 10, the maximum adsorption capacity after 5 h was 134.5 mg/g.Compared with another adsorbent,the adsorption capacity of Zr-MOF was higher.The removal of norfloxacin from an aqueous solution using Zr-MOF was feasible, inexpensive, and effective. Our findings indicate that Zr-MOF has broad application prospects for the purification of an aqueous solution.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
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IF 16.6
Deng Rongyu,He Zhenjiang,Chu Fulu,Lei Jie,Cheng Yi,Zhou You,Wu Feixiang
The conventional weak acidic electrolyte for aqueous zinc-ion batteries breeds many challenges, such as undesirable side reactions, and inhomogeneous zinc dendrite growth, leading to low Coulombic efficiency, low specific capacity, and poor cycle stability. Here, an aqueous densified electrolyte, namely, a conventional aqueous electrolyte with addition of perovskite SrTiO 3 powder, is developed to achieve high-performance aqueous zinc-ion batteries. The densified electrolyte demonstrates unique properties of reducing water molecule activity, improving Zn 2+ transference number, and inducing homogeneous and preferential deposition of Zn (002). As a result, the densified electrolyte exhibits an ultra-long cycle stability over 1000 cycles in Zn/Ti half cells. In addition, the densified electrolyte enables Zn/MnO 2 cells with a high specific capacity of 328.2 mAh g −1 at 1 A g −1 after 500 cycles under an extended voltage range. This work provides a simple strategy to induce dendrite-free deposition characteristics and high performance in high-voltage aqueous zinc-ion batteries.
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MOLECULES
·
2023
·Vol. 28
·期 17
·6233
·
IF 4.6
Mengran Tang,Long Zhang,Xiaoxue Song,Long Zhao
Gold nanoparticles (AuNPs) possess remarkable optical properties and electrical conductivity, making them highly relevant in various fields such as medical diagnoses, biological imaging, and electronic sensors. However, the existing methods for modulating the optical properties of AuNPs are often under limitations such as a high cost, the complexity of detection, a narrow range of application settings, and irreversibility. In this study, we propose a novel approach to address these challenges by constructing a reversible electrochemical switch. The switch (ITO-OMAD) involves covalently linking nitroxide radicals and AuNPs (AuNPs-NO•), followed by tethering this nanocomposite to a siloxane-derived indium tin oxide (ITO) electrode. By simply electrochemically oxidizing/reducing the nitroxide units, one is able to reversibly modulate the optical properties of AuNPs at will. The surface morphology and structure of the as-prepared ITO-OMAD electrode were characterized through scanning electron microscopy (SEM) and cyclic voltammetry (CV). SEM imaging confirmed the successful anchoring of AuNPs on the ITO electrode. Electrochemical tests performed in the three-electrode system demonstrated that the local surface plasmon resonance (LSPR) of AuNPs can be reversibly regulated by alternatively imposing ± 0.5V (vs. Ag/AgCl) to the modified electrode. The development of this electrochemical switch presents a novel approach to effectively control the optical properties of AuNPs. The further exploration and utilization of this reversible electrochemical switch could significantly enhance the versatility and practicality of AuNPs in numerous applications.Keywords:gold nanoparticles;nitroxide radicals;electrochemical switch;optical regulation
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Journal of Flow Chemistry
·
2023
·Vol. 13
·期 4
·375-383
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IF 2.7
Lai Liangchuan,Gao Liang,Liu Minjie,Guo Yongxing,Cheng Dang,Jiang Meifen,Chen Fener
Continuous flow technology has been widely adopted in manufacturing active pharmaceutical ingredients (APIs). Herein, we report an expeditious multi-step continuous-flow strategy for an efficient and highly productive flow synthesis of 7-methoxy-1-tetralone, which is an essential intermediate for the opioid analgesic drug (-)-dezocine. Compared with the traditional batch operation, this work presents significant advantages of continuous-flow chemistry with dramatically reduced reaction time, highly improved reaction efficiency, good controls over reaction optimizing conditions, etc. The flow protocol in this work provided the desired product in an overall yield of up to 76.6% with 99% purity, much higher than those from batch process (i.e., 50% yield, 92% purity). Moreover, reaction efficiency is highly improved with a throughput of 0.49 g/h, the total reaction time is markedly reduced from hours in batch to minutes in flow process. Graphical abstract
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