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Fluorescent probes and functional materials for biomedical applications
Xi-Le Hu, Hui-Qi Gan, Fan-De Meng, Hai-Hao Han, De-Tai Shi, Shu Zhang, Lei Zou, Xiao-Peng He, Tony D. James
Frontiers of Chemical Science and Engineering. 2022, 16 (10 ): 1425-1437.
https://doi.org/10.1007/s11705-022-2163-1
Due to their simplicity in preparation, sensitivity and selectivity, fluorescent probes have become the analytical tool of choice in a wide range of research and industrial fields, facilitating the rapid detection of chemical substances of interest as well as the study of important physiological and pathological processes at the cellular level. In addition, many long-wavelength fluorescent probes developed have also proven applicable for in vivo biomedical applications including fluorescence-guided disease diagnosis and theranostics (e.g., fluorogenic prodrugs). Impressive progresses have been made in the development of sensing agents and materials for the detection of ions, organic small molecules, and biomacromolecules including enzymes, DNAs/RNAs, lipids, and carbohydrates that play crucial roles in biological and disease-relevant events. Here, we highlight examples of fluorescent probes and functional materials for biological applications selected from the special issues “Fluorescent Probes” and “Molecular Sensors and Logic Gates” recently published in this journal, offering insights into the future development of powerful fluorescence-based chemical tools for basic biological studies and clinical translation.
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Theoretical and experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-based CO2 capture sorbents
Mahsa Javidi Nobarzad, Maryam Tahmasebpoor, Mohammad Heidari, Covadonga Pevida
Frontiers of Chemical Science and Engineering. 2022, 16 (10 ): 1460-1475.
https://doi.org/10.1007/s11705-022-2159-x
Carbon nanotubes-based materials have been identified as promising sorbents for efficient CO2 capture in fluidized beds, suffering from insufficient contact with CO2 for the high-level CO2 capture capacity. This study focuses on promoting the fluidizability of hard-to-fluidize pure and synthesized silica-coated amine-functionalized carbon nanotubes. The novel synthesized sorbent presents a superior sorption capacity of about 25 times higher than pure carbon nanotubes during 5 consecutive adsorption/regeneration cycles. The low-cost fluidizable-SiO2 nanoparticles are used as assistant material to improve the fluidity of carbon nanotubes-based sorbents. Results reveal that a minimum amount of 7.5 and 5 wt% SiO2 nanoparticles are required to achieve an agglomerate particulate fluidization behavior for pure and synthesized carbon nanotubes, respectively. Pure carbon nanotubes + 7.5 wt% SiO2 and synthesized carbon nanotubes + 5 wt% SiO2 indicates an agglomerate particulate fluidization characteristic, including the high-level bed expansion ratio, low minimum fluidization velocity (1.5 and 1.6 cm·s–1 ), high Richardson−Zakin index (5.2 and 5.3 > 5), and low Π value (83.2 and 84.8 < 100, respectively). Chemical modification of carbon nanotubes causes not only enhanced CO 2 uptake capacity but also decreases the required amount of silica additive to reach a homogeneous fluidization behavior for synthesized carbon nanotubes sorbent.
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NOx removal by non-thermal plasma reduction: experimental and theoretical investigations
Yue Liu, Ji-Wei Wang, Jian Zhang, Ting-Ting Qi, Guang-Wen Chu, Hai-Kui Zou, Bao-Chang Sun
Frontiers of Chemical Science and Engineering. 2022, 16 (10 ): 1476-1484.
https://doi.org/10.1007/s11705-022-2165-z
Green and efficient N O x removal at low temperature is still desired. N O x removal via non-thermal plasma (NTP) reduction is one of such technique. This work presents the experimental and theoretical study on the N O x removal via NTP reduction (NTPRD) in dielectric barrier discharge reactor (DBD). The effect of O 2 molar fraction on N O x species in the outlet of DBD, and effects of N H 3 /NO molar ratio and discharge power of DBD on N O x removal efficiency are investigated. Results indicate that anaerobic condition and higher discharge power is beneficial to direct removal of N O x , and the N O x removal efficiency can be up to 98.5% under the optimal operating conditions. It is also found that adding N H 3 is favorable for the reduction of N O x to N 2 at lower discharge power. In addition, the N O x removal mechanism and energy consumption analysis for the NTPRD process are also studied. It is found that the reduced active species ( N ∗ , N − , N+ , N 2 ∗ , N H 2 + , etc.) generated in the NTPRD process play important roles for the reduction of N O x to N 2 . Our work paves a novel pathway for N O x removal from anaerobic gas in industrial application.
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A density functional theory study of methane activation on MgO supported Ni9 M1 cluster: role of M on C–H activation
Juntian Niu, Haiyu Liu, Yan Jin, Baoguo Fan, Wenjie Qi, Jingyu Ran
Frontiers of Chemical Science and Engineering. 2022, 16 (10 ): 1485-1492.
https://doi.org/10.1007/s11705-022-2169-8
Methane activation is a pivotal step in the application of natural gas converting into high-value added chemicals via methane steam/dry reforming reactions. Ni element was found to be the most widely used catalyst. In present work, methane activation on MgO supported Ni–M (M = Fe, Co, Cu, Pd, Pt) cluster was explored through detailed density functional theory calculations, compared to pure Ni cluster. CH4 adsorption on Cu promoted Ni cluster requires overcoming an energy of 0.07 eV, indicating that it is slightly endothermic and unfavored to occur, while the adsorption energies of other promoters M (M = Fe, Co, Pd and Pt) are all higher than that of pure Ni cluster. The role of M on the first C–H bond cleavage of CH4 was investigated. Doping elements of the same period in Ni cluster, such as Fe, Co and Cu, for C–H bond activation follows the trend of the decrease of metal atom radius. As a result, Ni–Fe shows the best ability for C–H bond cleavage. In addition, doping the elements of the same family, like Pd and Pt, for CH4 activation is according to the increase of metal atom radius. Consequently, C–H bond activation demands a lower energy barrier on Ni–Pt cluster. To illustrate the adsorptive dissociation behaviors of CH4 at different Ni–M clusters, the Mulliken atomic charge was analyzed. In general, the electron gain of CH4 binding at different Ni–M clusters follows the sequence of Ni–Cu (–0.02 e) < Ni (–0.04 e) < Ni–Pd (–0.08 e) < Ni–Pt (–0.09 e) < Ni–Co (–0.10 e) < Ni–Fe (–0.12 e), and the binding strength between catalysts and CH 4 raises with the CH4 electron gain increasing. This work provides insights into understanding the role of promoter metal M on thermal-catalytic activation of CH4 over Ni/MgO catalysts, and is useful to interpret the reaction at an atomic scale.
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Nickel-based metal−organic framework-derived whisker-shaped nickel phyllosilicate toward efficiently enhanced mechanical, flammable and tribological properties of epoxy nanocomposites
Yuxuan Xu, Guanglong Dai, Shibin Nie, Jinian Yang, Song Liu, Hong Zhang, Xiang Dong
Frontiers of Chemical Science and Engineering. 2022, 16 (10 ): 1493-1504.
https://doi.org/10.1007/s11705-022-2168-9
Metal−organic framework-derived materials have attracted significant attention in the applications of functional materials. In this work, the rod-like nickel-based metal−organic frameworks were first synthesized and subsequently employed as the hard templates and nickel sources to prepare the whisker-shaped nickel phyllosilicate using a facile hydrothermal technology. Then, the nickel phyllosilicate whiskers were evaluated to enhance the mechanical, thermal, flammable, and tribological properties of epoxy resin. The results show that adequate nickel phyllosilicate whiskers can disperse well in the matrix, improving the tensile strength and elastic modulus by 13.6% and 56.4%, respectively. Although the addition of nickel phyllosilicate whiskers could not obtain any UL-94 ratings, it enhanced the difficulty in burning the resulted epoxy resin nanocomposites and considerably enhanced thermal stabilities. Additionally, it was demonstrated that such nickel phyllosilicate whiskers preferred to improve the wear resistance instead of the antifriction feature. Moreover, the wear rate of epoxy resin nanocomposites was reduced significantly by 80% for pure epoxy resin by adding 1 phr whiskers. The as-prepared nickel phyllosilicate whiskers proved to be promising reinforcements in preparing of high-performance epoxy resin nanocomposites.
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Pd/Fe3 O4 supported on bio-waste derived cellulosic-carbon as a nanocatalyst for C–C coupling and electrocatalytic application
Vishal Kandathil, Akshay Moolakkil, Pranav Kulkarni, Alaap Kumizhi Veetil, Manjunatha Kempasiddaiah, Sasidhar Balappa Somappa, R. Geetha Balakrishna, Siddappa A. Patil
Frontiers of Chemical Science and Engineering. 2022, 16 (10 ): 1514-1525.
https://doi.org/10.1007/s11705-022-2158-y
The current work describes the synthesis of a new bio-waste derived cellulosic-carbon supported-palladium nanoparticles enriched magnetic nanocatalyst (Pd/Fe3 O4 @C) using a simple multi-step process under aerobic conditions. Under mild reaction conditions, the Pd/Fe3 O4 @C magnetic nanocatalyst demonstrated excellent catalytic activity in the Hiyama cross-coupling reaction for a variety of substrates. Also, the Pd/Fe3 O4 @C magnetic nanocatalyst exhibited excellent catalytic activity up to five recycles without significant catalytic activity loss in the Hiyama cross-coupling reaction. Also, we explored the use of Pd/Fe3 O4 @C magnetic nanocatalyst as an electrocatalyst for hydrogen evolution reaction. Interestingly, the Pd/Fe3 O4 @C magnetic nanocatalyst exhibited better electrochemical activity compared to bare carbon and magnetite (Fe3 O4 nanoparticles) with an overpotential of 293 mV at a current density of 10 mA·cm–2 .
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