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1.
《International Journal of Hydrogen Energy》2022,47(77):32928-32939
The development of efficient and stable electrocatalysts is of great significance for improving water splitting. Among them, transition metal oxyhydroxides show excellent performance in oxygen evolution reactions (OER), but there are certain difficulties in direct preparation. Recently, Metal–organic frameworks (MOFs) as precatalysts or precursors have shown promising catalytic performance in OER and can be decomposed under alkaline conditions. Therefore, using a mild and controllable way to convert MOFs into oxyhydroxides and retaining the original structural advantages is crucial for improving the catalytic activity. Herein, a rapid electrochemical strategy is used to activate well-mixed MOFs to prepare Co/Ni oxyhydroxide nanosheets for efficient OER catalysts, and the structural transformation in this process was investigated in detail by using scanning electron microscope, X-ray diffraction, Raman, X-ray photoelectron spectroscopy and electrochemical methods. It is discovered that electrochemical activation can promote ligand substitution of well-mixed MOFs to form porous oxyhydroxide nanosheets and tune the electronic structure of the metal (Co and Ni), which can lead to more active site exposure and accelerate charge transfer. In addition, the change of structure also improves hydrophilicity, as well as benefiting from the strong synergistic effect between multiple species, the optimal a-MCoNi–MOF/NF has excellent OER performance and long-term stability. More obviously, the porous CoNiOOH nanosheets are formed in situ during electrochemical activation process through structural transformation and acts as the active centers. This work provides new insights for mild synthesis of MOFs derivatives and also provides ideas for the preparation of highly efficient catalysts. 相似文献
2.
《Ceramics International》2021,47(20):28203-28209
Vanadium carbide (VC) as excellent ceramic and functional material is usually prepared by carbothermal reduction of V2O5 which must be extracted from a typical V slag by complex processes. Pollutants, such as ammonia-nitrogen wastewater, NH3 and CO2 are inevitably discharged. A novel and green method for VC preparation was proposed by one-step co-electrolysis of soluble NaVO3 and CO2 in molten salt. It was found that VC with high purity was easily obtained by reducing electrolysis temperature and CO2 flow rate to 600 °C and 10 mL min−1 at 3.0 V. Besides VC with particles and layered stacking structure in products, a small amount of carbon and oxygen elements existed. The atomic percentage contents of C, V, and O elements in VC were about 50.0%, 44.5% and 3.8%, respectively. During electrolysis, CO32− and VO3− was reduced at about −0.55 V (vs. Ag/AgCl) and −1.38 V (vs. Ag/AgCl), respectively. CO32− ions were more easily reduced than VO3−, and was firstly reduced to CO22− and then converted to C. Then, VC was prepared by two routes from CO2 and NaVO3. One route is that VO3− ions are firstly electroreduced to VO2− ions and then are further electroreduced to VC with C. Another route is that VO3− ions are electroreduced to V which in-situ reacted with C to VC. Both VO3− and CO32− ions are electroreduced by two-step process. In final, VC is in-situ deposited on cathode. It provides a novel and green way to prepare VC and also achieves the high value-added utilization of vanadium slag and CO2. 相似文献
3.
Chenhui Ding Marion Breunig Jana Timm Roland Marschall Jürgen Senker Seema Agarwal 《Advanced functional materials》2021,31(49):2106507
Covalent organic frameworks (COFs) show advantageous characteristics, such as an ordered pore structure and a large surface area for gas storage and separation, energy storage, catalysis, and molecular separation. However, COFs usually exist as difficult-to-process powders, and preparing continuous, robust, flexible, foldable, and rollable COF membranes is still a challenge. Herein, such COF membranes with fiber morphology for the first time prepared via a newly introduced template-assisted framework process are reported. This method uses electrospun porous polymer membranes as a sacrificial large dimension template for making self-standing COF membranes. The porous COF fiber membranes, besides having high crystallinity, also show a large surface area (1153 m2 g−1), good mechanical stability, excellent thermal stability, and flexibility. This study opens up the possibility of preparation of large dimension COF membranes and their derivatives in a simple way and hence shows promise in technical applications in separation, catalysis, and energy in the future. 相似文献
4.
Xiaozhen Li Chao Yin Si Si Liew Chun-Sing Lee Kanyi Pu 《Advanced functional materials》2021,31(46):2106154
Optical imaging has played a pivotal role in deciphering in vivo bioinformatics but is limited by shallow penetration depth and poor imaging performance owing to interfering tissue autofluorescence induced by concurrent photoexcitation. The emergence of near-infrared (NIR) self-luminescence imaging independent of real-time irradiation has timely addressed these problems. There are two main kinds of self-luminescent agents, namely inorganic and organic luminophores. Inorganic luminophores usually suffer from long-term biotoxicity concerns resulting from potential heavy-metal ions leakage and nonbiodegradability, which hinders their further translational application. In contrast, organic luminophores, especially organic semiconducting luminophores (OSLs) with good biodegradable potential, tunable design, and outstanding optical properties, are preferred in biological applications. This review summarizes the recent progress of OSLs used in NIR afterglow, chemiluminescence, and bioluminescence imaging. Molecular manipulation and nanoengineering approaches of OSLs are discussed, with emphasis on strategies that can extend the emission wavelength from visible to NIR range and amplify luminescence signals. This review concludes with a discussion of current challenges and possible solutions of OSLs in the self-luminescence field. 相似文献
5.
Since the discovery in 1922 of 2,2-diphenyl-1-(2,4,6-trinitrophenyl) hydrazyl stable free radical (DPPH·), the chemistry of such open-shell compounds has developed continuously, allowing for both theoretical and practical advances in the free radical chemistry area. This review presents the important, general and modern aspects of the chemistry of hydrazyl free radicals and the science behind it. 相似文献
6.
Yujie Chen Yiping Song Zhen Zhang Yali Chen Qiliang Deng Shuo Wang 《Advanced functional materials》2021,31(41):2104885
Various products, including foods and pharmaceuticals, are sensitive to temperature fluctuations. Thus, temperature monitoring during production, transportation, and storage is critical. Facile indicators are required to monitor temperature conditions via color changes in real time. This study aimed to prepare and apply thiol-functionalized covalent organic frameworks (COFs) as a novel indicator for monitoring thermal history and temperature abuse. The COFs underwent obvious color changes from bright yellow to purple after exposure to different temperatures for varying durations. The reaction kinetics are analyzed under isothermal conditions, which reveal that the order of reaction rates is k−20°C < k4°C < k20°C < k35°C < k55°C. The activation energy (Ea) of the COFs is calculated using the Arrhenius equation as 50.71 kJ moL−1. The COFs are capable of sensitive color changes and offer a broad temperature tracking range, thereby demonstrating their application potential for the monitoring of temperature and time exposure history during production, transportation, and storage. This excellent performance thermal history indicator also shows promise for expanding the application field of COFs. 相似文献
7.
Krzysztof M. Tokarz Wojciech Wesoowski Barbara Tokarz Wojciech Makowski Anna Wysocka Roman J. Jdrzejczyk Karolina Chrabaszcz Kamilla Malek Anna Kostecka-Gugaa 《International journal of molecular sciences》2021,22(2)
Grass pea (Lathyrus sativus) is a leguminous plant of outstanding tolerance to abiotic stress. The aim of the presented study was to describe the mechanism of grass pea (Lathyrus sativus L.) photosynthetic apparatus acclimatisation strategies to salinity stress. The seedlings were cultivated in a hydroponic system in media containing various concentrations of NaCl (0, 50, and 100 mM), imitating none, moderate, and severe salinity, respectively, for three weeks. In order to characterise the function and structure of the photosynthetic apparatus, Chl a fluorescence, gas exchange measurements, proteome analysis, and Fourier-transform infrared spectroscopy (FT-IR) analysis were done inter alia. Significant differences in the response of the leaf and stem photosynthetic apparatus to severe salt stress were observed. Leaves became the place of harmful ion (Na+) accumulation, and the efficiency of their carboxylation decreased sharply. In turn, in stems, the reconstruction of the photosynthetic apparatus (antenna and photosystem complexes) activated alternative electron transport pathways, leading to effective ATP synthesis, which is required for the efficient translocation of Na+ to leaves. These changes enabled efficient stem carboxylation and made them the main source of assimilates. The observed changes indicate the high plasticity of grass pea photosynthetic apparatus, providing an effective mechanism of tolerance to salinity stress. 相似文献
8.
Yin-Feng Wang Meng Li Jin-Ming Teng He-Ye Zhou Chuan-Feng Chen 《Advanced functional materials》2021,31(49):2106418
Recently, circularly polarized organic light-emitting diodes (CP-OLEDs) fabricated with thermally activated delayed fluorescence (TADF) emitters are developed rapidly. However, most devices are fabricated by vacuum deposition technology, and developing efficient solution-processed CP-OLEDs, especially nondoped devices, is still a challenge. Herein, a pair of triptycene-based enantiomers, (S,S)-/(R,R)-TpAc-TRZ, are synthesized. The novel chiral triptycene scaffold of enantiomers avoids their intermolecular π–π stacking, which is conducive to their aggregation-induced emission characteristics and high photoluminescence quantum yield of 85% in the solid state. Moreover, the triptycene-based enantiomers exhibit efficient TADF activities with a small singlet-triplet energy gap (ΔEST) of 0.03 eV and delayed fluorescence lifetime of 1.1 µs, as well as intense circularly polarized luminescence with dissymmetry factors (|gPL|) of about 1.9 × 10−3. The solution-processed nondoped CP-OLEDs based on (S,S)-/(R,R)-TpAc-TRZ not only display obvious circularly polarized electroluminescence signals with gEL values of +1.5 × 10−3 and −2.0 × 10−3, respectively, but also achieve high efficiencies with external quantum, current, and power efficiency up to 25.5%, 88.6 cd A−1, and 95.9 lm W−1, respectively. 相似文献
9.
《International Journal of Hydrogen Energy》2022,47(57):23994-24003
Hydrogenation of dibenzyltoluene (DBT) is of great significance for the application in liquid organic hydrogen carriers (LOHCs). We successfully develop Mg-based metal hydrides (Mg2NiH4, MgH2, and LaH3) reactive ball-milling for the hydrogenation of DBT. Mg-based metal hydrides milled with 500 min exhibit the best catalytic activity, the hydrogen uptake of DBT can reach 4.63 wt% at the first 4 h and finally achieve 5.70 wt% through 20 h, which is the first time to use hydrogen storage material as a catalyst for the hydrogenation of DBT. The excellent catalytic hydrogenation performance of Mg-based metal hydrides mostly originates from numerous catalytic activity centers formed at the surfaces of Mg2NiH4 nanoparticles in the MgH2 matrix. Inspired by this mechanism, more general metal hydrides can be explored for catalyzing the hydrogenation of LOHCs. The new application of Mg-based metal hydrides is beneficial to developing efficient LOHC based hydrogen storage systems and offers novel insights to hydride-based catalysts. 相似文献
10.
《International Journal of Hydrogen Energy》2022,47(12):7600-7623
In this paper, a salinity gradient solar pond (SGSP) is used to harness the solar energy for hydrogen production through two cycles. The first cycle includes an absorption power cycle (APC), a proton exchange membrane (PEM) electrolyzer, and a thermoelectric generator (TEG) unit; in the second one, an organic Rankine cycle (ORC) with the zeotropic mixture is used instead of APC. The cycles are analyzed through the thermoeconomic vantage point to discover the effect of key decision variables on the cycles’ performance. Finally, NSGA-II is used to optimize both cycles. The results indicate that employing ORC with zeotropic mixture leads to a better performance in comparison to utilizing APC. For the base mode, unit cost product (UCP), exergy, and energy efficiency when APC is employed are 59.9 $/GJ, 23.73%, and 3.84%, respectively. These amounts are 47.27 $/GJ, 29.48%, and 5.86% if ORC with the zeotropic mixture is utilized. The APC and ORC generators have the highest exergy destruction rate which is equal to 6.18 and 10.91 kW. In both cycles, the highest investment cost is related to the turbine and is 0.8275 $/h and 0.976 $/h for the first and second cycles, respectively. In the optimum state the energy efficiency, exergy efficiency, UCP, and H2 production rate of the system enhances 42.44%, 27.54%,15.95%, and 38.24% when ORC with the zeotropic mixture is used. The maximum H2 production is 0.47 kg/h, and is obtained when the mass fraction of R142b, LCZ temperature, pumps pressure ratio, generator bubble point temperature are 0.603, 364.35 K, 2.12, 337.67 K, respectively. 相似文献