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Dealloyed nanoporous gold (np-Au) has applications as oxygen reduction catalysis in Li-air batteries and fuel cells, or as actuators to convert electricity into mechanical energy. However, it faces the challenges of coarsening-induced structure instability, mechanical weakness due to low relative densities, and slow dealloying rates. Here, monolithic np-Au is dealloyed from a single-phase Au25Ni75 solid-solution at a one-order faster dealloying rate, ultra-low residual Ni content, and importantly, one-third more relative density than np-Au dealloyed from conventional Au25Ag75. The small atomic radius and low dealloying potential of the sacrificing element Ni are intrinsically beneficial to fast produce high relative density np-Au, as predicted by a general model for dealloying of binary alloys and validated by experiments. Stable, durable, and reversible actuation of np-Au takes place under cyclic potential triggering in alkaline and acidic electrolytes with negligible coarsening-induced strain-shift. The thermal and mechanical robustness of bulk np-Au is confirmed by two-order slower ligament coarsening rates during annealing at 300 °C and 45 MPa macroscopic yielding strength distinctive from the typical early onset of plastic yielding. This article opens a rich direction to achieve high relative density np-Au which is essential for porous network connectivity, mechanical strength, and nanostructure robustness for electrochemical functionality. 相似文献
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Teh C. Ho 《American Institute of Chemical Engineers》2020,66(6):e16930
Metal sulfide catalysts for ultra-deep hydrodesulfurization of diesel generally lose a fraction of their catalytically active sites during reactor startup. The underlying mechanisms are discussed. A laboratory diagnostic tool consisting of three probe molecules is developed for testing metal sulfide catalysts' start-of-run (SOR) activity maintenance. It is found that a significant fraction of the active sites on a commercial supported catalyst are deactivated permanently, but this is not the case with a bulk metal sulfide catalyst. The SOR deactivation of the bulk catalyst is completely reversible, while that of the supported catalyst is partially reversible. The diagnostic tool may provide a basis for developing a high-throughput approach for evaluating and enhancing catalyst SOR stability, thereby increasing plant productivity. 相似文献
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Polymer‐grafted inorganic particles (PGIPs) are attractive building blocks for numerous chemical and material applications. Surface‐initiated controlled radical polymerization (SI‐CRP) is the most feasible method to fabricate PGIPs. However, a conventional in‐batch reaction still suffers from several disadvantages, including time‐consuming purification processes, low grafting efficiency, and possible gelation problems. Herein, a facile method is demonstrated to synthesize block copolymer–grafted inorganic particles, that is, poly(poly(ethylene glycol) methyl ether methacrylate) (PPEGMEMA)‐b‐poly(N‐isopropylacrylamide) (PNIPAM)–grafted silica micro‐particles using continuous flow chemistry in an environmentally friendly aqueous media. Immobilizing the chain transfer agent and subsequent SI‐CRP can be accomplished sequentially in a continuous flow system, avoiding multi‐step purification processes in between. The chain length (MW) of the grafted polymers is tunable by adjusting the flow time or monomer concentration, and the narrower molar mass dispersity (Ð < 1.4) of the grafted polymers reveals the uniform polymer chains on the particles. Moreover, compared with the in‐batch reaction at the same condition, the continuous system also suppresses possible gelation problems. 相似文献
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Yasuha Watanabe Prof. Kenzo Fujimoto 《Chembiochem : a European journal of chemical biology》2020,21(22):3244-3248
The regulation of DNAzyme activity is an important problem for its in vivo applications. We achieved photochemical regulation of DNAzyme activity by using reversible DNA photo-crosslinking of 3-cyanovinylcarbazole (CNVK). The ODN containing CNVK photo-crosslinked to a pyrimidine base in the complementary strand after a few seconds of photoirradiation, and its photoadduct was split by photoirradiation of another wavelength. The activity of photo-crosslinked DNAzyme with CNVK was completely inhibited (OFF state). In contrast, after 312 nm irradiation, DNAzyme activity was recovered upon addition of a substrate strand (ON state). In addition, the photo-crosslinked DNAzyme is prone to enzymatic digestion by exonuclease. This photochemical OFF to ON switching with reversible DNA photo-crosslinking was regulated at the desired time and position; therefore, it might be possible to use it for in vivo application. 相似文献
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Natalia S Serkhacheva Nikolay I Prokopov Elena V Chernikova Elena Y Kozhunova Inna O Lebedeva Oleg V Borisov 《Polymer International》2019,68(7):1303-1314
Emulsifier‐free batch emulsion polymerization of n‐butyl acrylate and its semi‐batch copolymerization with 2,2,3,3,4,4,5,5‐octafluoropentyl acrylate and 2,2,3,4,4,4‐hexafluorobutyl acrylate both mediated by poly(acrylic acid) containing the trithiocarbonate group in the chain was employed to produce amphiphilic triblock copolymers. The polymerization‐induced self‐assembly of these copolymers in aqueous media gave rise to spherical core–shell particles. Irrespective of the experimental conditions, the polymeric product was characterized by a bimodal molecular weight distribution. The apparent violation of the reversible addition–fragmentation chain transfer polymerization mechanism may be attributed to restricted accessibility of the trithiocarbonate group in the self‐assembled block copolymers for propagating radicals that enter into the particle. Mean‐field theoretical arguments were employed to explain the exclusively spherical morphology of the particles observed in the experiment. © 2019 Society of Chemical Industry 相似文献
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