Yolk–Shell Nanoarchitectures with a Ru-Containing Core and a Radially Oriented Mesoporous Silica Shell: Facile Synthesis and Application for One-Pot Biomass Conversion by Combining with Enzyme
Abstract:In this paper, we develop a facile strategy for fabricating a yolk-shell structured catalytic system that consists of a core made of Ru supported on mesoporous carbon, which is encaged within a silica shell that has ordered radial mesochannels. A region-selective etching mechanism for the formation of the yolk-shell nanoarchitectures is proposed based on the stronger adsorption ability of the carbon core for etching agent than that of the silica shell for etching agent. By combining such material with amyloglu… Show more
“…Recently, we applied the combination of such a yolk-shell-structured catalyst and enzyme to act as a powerful platform for one-pot biomass conversion via sequential enzyme-catalyzed hydrolysis of biomass materials to glucose and the subsequent metal-catalyzed hydrogenation of glucose to sorbitol. 81,82 Preliminary studies revealed that the enzyme is easily poisoned when contacting Ru-based catalysts. Meanwhile, the metallic Ru active sites would be covered by the enzyme and the colloidal substances originated from dextrin hydrolysis, leading to a rapid deactivation for the subsequent glucose hydrogenation to sorbitol.…”
Section: Encapsulated Metal Catalystsmentioning
confidence: 99%
“…Reaction conditions: dextrin (0.6 g), amyloglucosidase (0.048 mL), a catalyst (containing 15.6 mg of Ru), water (60 mL), T = 343 K, PH 2 = 4.0 Mpa, stirring rate = 800 rpm. Each run was conducted for 6 h.Reprinted with permission from Xu et al82 (copyright 2014 American Chemical Society) and Wei et al83 (copyright 2014 American Chemical Society).…”
Metal catalysts have been widely employed in chemical production, medicine manufacture, organic synthesis, and environmental cleaning, etc. Catalyst design plays a key role in enhancing efficiencies including activity, selectivity, and durability. Both theoretical predictions and experimental research has demonstrated that besides the composition, the morphology and/or the porous structure play key roles in determining catalytic performances. This review highlights the recent progress in the controlled synthesis of new metal catalysts with hierarchical structures mainly based on our research. First, we describe the metal catalysts with unique morphologies. Second, we show the metal catalysts with different porous structures. Finally, we summarize the metal catalysts with hierarchical structures. The catalytic performances of different catalysts are also included, and their correspondence to the catalyst structure is explored. This review might supply guidance for designing new and powerful metal catalysts for industrial applications.
“…Recently, we applied the combination of such a yolk-shell-structured catalyst and enzyme to act as a powerful platform for one-pot biomass conversion via sequential enzyme-catalyzed hydrolysis of biomass materials to glucose and the subsequent metal-catalyzed hydrogenation of glucose to sorbitol. 81,82 Preliminary studies revealed that the enzyme is easily poisoned when contacting Ru-based catalysts. Meanwhile, the metallic Ru active sites would be covered by the enzyme and the colloidal substances originated from dextrin hydrolysis, leading to a rapid deactivation for the subsequent glucose hydrogenation to sorbitol.…”
Section: Encapsulated Metal Catalystsmentioning
confidence: 99%
“…Reaction conditions: dextrin (0.6 g), amyloglucosidase (0.048 mL), a catalyst (containing 15.6 mg of Ru), water (60 mL), T = 343 K, PH 2 = 4.0 Mpa, stirring rate = 800 rpm. Each run was conducted for 6 h.Reprinted with permission from Xu et al82 (copyright 2014 American Chemical Society) and Wei et al83 (copyright 2014 American Chemical Society).…”
Metal catalysts have been widely employed in chemical production, medicine manufacture, organic synthesis, and environmental cleaning, etc. Catalyst design plays a key role in enhancing efficiencies including activity, selectivity, and durability. Both theoretical predictions and experimental research has demonstrated that besides the composition, the morphology and/or the porous structure play key roles in determining catalytic performances. This review highlights the recent progress in the controlled synthesis of new metal catalysts with hierarchical structures mainly based on our research. First, we describe the metal catalysts with unique morphologies. Second, we show the metal catalysts with different porous structures. Finally, we summarize the metal catalysts with hierarchical structures. The catalytic performances of different catalysts are also included, and their correspondence to the catalyst structure is explored. This review might supply guidance for designing new and powerful metal catalysts for industrial applications.
“…For a better understanding of these structures, we would review these structures based on different fabrication approaches. The YS structure can be fabricated not only from inside to outside but also outside to inside [ 49 , 63 – 67 ]. As shown in Fig.…”
Section: Development Of Yolk–shell Structuresmentioning
confidence: 99%
“…Initial researches of YS structures concentrated on spherical structures [ 46 – 48 ]. Afterward, with the development of different synthetic methods such as selective etching [ 49 ], self-template [ 50 ], Ostwald-ripening [ 51 , 52 ] and Kirkendall effect [ 46 , 53 ], YS structures can be prepared into manifold types [ 54 – 56 ]. Fig.…”
Lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) have received much attention in energy storage system. In particular, among the great efforts on enhancing the performance of LIBs and SIBs, yolk–shell (YS) structured materials have emerged as a promising strategy toward improving lithium and sodium storage. YS structures possess unique interior void space, large surface area and short diffusion distance, which can solve the problems of volume expansion and aggregation of anode materials, thus enhancing the performance of LIBs and SIBs. In this review, we present a brief overview of recent advances in the novel YS structures of spheres, polyhedrons and rods with controllable morphology and compositions. Enhanced electrochemical performance of LIBs and SIBs based on these novel YS structured anode materials was discussed in detail.
Biocatalysis with immobilized enzymes as catalysts holds enormous promise in developing more efficient and sustainable processes for the synthesis of fine chemicals, chiral pharmaceuticals and biomass feedstocks. Despite the appealing potentials, nowadays the industrial-scale application of biocatalysts is still quite modest in comparison with that of traditional chemical catalysts. A critical issue is that the catalytic performance of enzymes, the sophisticated and vulnerable catalytic machineries, strongly depends on their intracellular working environment; however the working circumstances provided by the support matrix are radically different from those in cells. This often leads to various adverse consequences on enzyme conformation and dynamic properties, consequently decreasing the overall performance of immobilized enzymes with regard to their activity, selectivity and stability. Engineering enzyme catalysis in support nanopores by mimicking the physiological milieu of enzymes in vivo and investigating how the interior microenvironment of nanopores imposes an influence on enzyme behaviors in vitro are of paramount significance to modify and improve the catalytic functions of immobilized enzymes. In this feature article, we have summarized the recent advances in mimicking the working environment and working patterns of intracellular enzymes in nanopores of mesoporous silica-based supports. Especially, we have demonstrated that incorporation of polymers into silica nanopores could be a valuable approach to create the biomimetic microenvironment for enzymes in the immobilized state.
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