It is curial to develop a high-efficient, low-cost visible-light responsive photocatalyst for the application in solar energy conversion and environment remediation. Here, a three-dimensional (3D) porous g-C3N4/graphene oxide aerogel (CNGA) has been prepared by the hydrothermal coassembly of two-dimensional g-C3N4 and graphene oxide (GO) nanosheets, in which g-C3N4 acts as an efficient photocatalyst, and GO supports the 3D framework and promotes the electron transfer simultaneously. In CNGA, the highly interconnected porous network renders numerous pathways for rapid mass transport, strong adsorption and multireflection of incident light; meanwhile, the large planar interface between g-C3N4 and GO nanosheets increases the active site and electron transfer rate. Consequently, the methyl orange removal ratio over the CNGA photocatalyst reaches up to 92% within 4 h, which is much higher than that of pure g-C3N4 (12%), 2D hybrid counterpart (30%) and most of representative g-C3N4-based photocatalysts. In addition, the dye is mostly decomposed into CO2 under natural sunlight irradiation, and the catalyst can also be easily recycled from solution. Significantly, when utilized for CO2 photoreduction, the optimized CNGA sample could reduce CO2 into CO with a high yield of 23 mmol g(-1) (within 6 h), exhibiting about 2.3-fold increment compared to pure g-C3N4. The photocatalyst exploited in this study may become an attractive material in many environmental and energy related applications.
With the continuous increase in fossil fuels consumption and the rapid growth of atmospheric CO2 concentration, the harmonious state between human and nature faces severe challenges. Exploring green and sustainable energy resources and devising efficient methods for CO2 capture, sequestration and utilization are urgently required. Converting CO2 into fuels/chemicals/materials as an indispensable element for CO2 capture, sequestration and utilization may offer a win-win strategy to both decrease the CO2 concentration and achieve the efficient exploitation of carbon resources. Among the current major methods (including chemical, photochemical, electrochemical and enzymatic methods), the enzymatic method, which is inspired by the CO2 metabolic process in cells, offers a green and potent alternative for efficient CO2 conversion due to its superior stereo-specificity and region/chemo-selectivity. Thus, in this tutorial review, we firstly provide a brief background about enzymatic conversion for CO2 capture, sequestration and utilization. Next, we depict six major routes of the CO2 metabolic process in cells, which are taken as the inspiration source for the construction of enzymatic systems in vitro. Next, we focus on the state-of-the-art routes for the catalytic conversion of CO2 by a single enzyme system and by a multienzyme system. Some emerging approaches and materials utilized for constructing single-enzyme/multienzyme systems to enhance the catalytic activity/stability will be highlighted. Finally, a summary about the current advances and the future perspectives of the enzymatic conversion of CO2 will be presented.
Activation of the NMDA subtype of glutamate receptor is required for activity-dependent structural plasticity in many areas of the young brain. Previous work has shown that NMDA receptor currents decline approximately at the time that developmental synaptic plasticity ends, and in situ hybridization studies have suggested that receptor subunit changes may be occurring during the same developmental interval. To establish a system in which the relationship between these properties of developing synapses can be explored, we have combined patch-clamp recordings with mRNA-and protein-level biochemical analyses to study the developmental regulation of NMDA receptors in the superficial layers of the rat superior colliculus. These experiments document an abrupt decrease in the NMDA receptor contribution to synaptic currents that occurs before eye opening and is closely associated with changes in NR1 protein, rapidly rising levels of the NMDA receptor subunit NR2A, and decreasing levels of NR2B. The functional and molecular changes also are correlated with the developmental decline in structural plasticity in these layers. In addition, both physiological and biochemical methods show evidence of GABA-mediated inhibition in the superficial collicular layers beginning after eye opening. This may provide an additional heterosynaptic mechanism for controlling excitation and plasticity in this neuropil by pattern vision. Thus our findings lend support to the idea that high levels of NMDA receptor function are associated with the potential for structural rearrangement in CNS neuropil and that the functional downregulation of this molecule results, at least partially, from changes in its subunit composition.
Enzyme catalysis, as a green, efficient process, displays exceptional functionality, adaptivity and sustainability. Multi-enzyme catalysis, which can accomplish the tandem synthesis of valuable materials/chemicals from renewable feedstocks, establishes a bridge between single-enzyme catalysis and whole-cell catalysis. Multi-enzyme catalysis occupies a unique and indispensable position in the realm of biological reactions for energy and environmental applications. Two complementary strategies, i.e., compartmentalization and substrate channeling, have been evolved by living organisms for implementing the complex in vivo multi-enzyme reactions (MERs), which have been applied to construct multi-enzyme catalytic systems (MECSs) with superior catalytic activity and stabilities in practical biocatalysis. This tutorial review aims to present the recent advances and future prospects in this burgeoning research area, stressing the features and applications of the two strategies for constructing MECSs and implementing in vitro MERs. The concluding remarks are presented with a perspective on the construction of MECSs through rational combination of compartmentalization and substrate channeling.
Graphitic carbon nitride (g-C 3 N 4 ) is an emergent metal-free photocatalyst because of its band position, natural abundance, and facile preparation. Synergetic intensification of charge generation and charge transfer of g-C 3 N 4 to increase solar-to-chemical efficiency remains a hot yet challenging issue. Herein, a nanoshell with two moieties of α-Fe 2 O 3 and carbon (C) is in situ formed on the surface of a g-C 3 N 4 core through calcination of Fe 3+ /polyphenol-coated melamine, thus acquiring g-C 3 N 4 @α-Fe 2 O 3 /C core@shell photocatalysts. The α-Fe 2 O 3 moiety acts as an additional photosensitizer, offering more photogenerated electrons, whereas the C moiety bridges a "highway" to facilitate the electron transfer either from α-Fe 2 O 3 moiety to g-C 3 N 4 or from g-C 3 N 4 to C moiety. By tuning the proportion of these two moieties in the nanoshell, a photocurrent density of 3.26 times higher than pristine g-C 3 N 4 is obtained. When utilized for photocatalytic regeneration of reduced nicotinamide adenine dinucleotide (NADH, a dominant cofactor in biohydrogenation reaction), g-C 3 N 4 @α-Fe 2 O 3 /C exhibits an equilibrium NADH yield of 76.3% with an initial reaction rate (r) of 7.7 mmol h −1 g −1 , among the highest r for photocatalytic NADH regeneration ever reported. Manipulating the coupling between charge generation and charge transfer may offer a facile, generic strategy to improve the catalytic efficiency of a broad range of photocatalysts other than g-C 3 N 4 .
Organic-inorganic hybrid capsules, which typically possess a hollow lumen and a hybrid wall, have emerged as a novel and promising class of hybrid materials and have attracted enormous attention. In comparison to polymeric capsules or inorganic capsules, the hybrid capsules combine the intrinsic physical/chemical properties of the organic and inorganic moieties, acquire more degrees of freedom to manipulate multiple interactions, create hierarchical structures and integrate multiple functionalities. Thus, the hybrid capsules exhibit superior mechanical strength (vs. polymeric capsules) and diverse functionalities (vs. inorganic capsules), which may give new opportunities to produce high-performance materials. Much effort has been devoted to exploring innovative and effective methods for the synthesis of hybrid capsules that exhibit desirable performance in target applications. This tutorial review firstly presents a brief description of the capsular structure and hybrid materials in nature, then classifies the hybrid capsules into molecule-hybrid capsules and nano-hybrid capsules based upon the size of the organic and inorganic moieties in the capsule wall, followed by a detailed discussion of the design and synthesis of the hybrid capsules. For each kind of hybrid capsule, the state-of-the-art synthesis methods are described in detail and a critical comment is embedded. The applications of these hybrid capsules in biotechnological areas (biocatalysis, drug delivery, etc.) have also been summarized. Hopefully, this review will offer a perspective and guidelines for the future research and development of hybrid capsules.
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