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• W2896581680 abstract "In this issue of Chem, Zhao and co-workers present a novel pressure-driven oriented assembly approach to synthesizing asymmetric dehiscent rutile TiO2 microparticles with single-crystal-like walls and a precisely controlled crystalline phase for photocatalytic H2 production. This versatile strategy could pave a new way for constructing mesoporous micro- and nanomaterials for diverse applications. In this issue of Chem, Zhao and co-workers present a novel pressure-driven oriented assembly approach to synthesizing asymmetric dehiscent rutile TiO2 microparticles with single-crystal-like walls and a precisely controlled crystalline phase for photocatalytic H2 production. This versatile strategy could pave a new way for constructing mesoporous micro- and nanomaterials for diverse applications. Mesoporous materials with pore diameters in the range of 2–50 nm have attracted widespread attention because of their high surface area, rich pore architectures, and diverse kinds of functional materials available in bulk and micro- and nanosized forms.1Wan Y. Zhao D. On the controllable soft-templating approach to mesoporous silicates.Chem. Rev. 2007; 107: 2821-2860Crossref PubMed Scopus (2058) Google Scholar In the past few decades, mesoporous micro- and nanoparticles have attracted significant research interest in heterogeneous catalysis, energy storage and conversion, cell imaging, disease diagnosis, and drug, gene, and protein storage or delivery.2Li W. Liu J. Zhao D. Mesoporous materials for energy conversion and storage devices.Nat. Rev. Mater. 2016; 1: 16023Crossref Scopus (886) Google Scholar, 3Guan B.Y. Yu L. Lou X.W. Formation of asymmetric bowl-like mesoporous particles via emulsion-induced interface anisotropic assembly.J. Am. Chem. Soc. 2016; 138: 11306-11311Crossref PubMed Scopus (230) Google Scholar Among various mesoporous micro- and nanomaterials, mesoporous TiO2 micro- and nanoparticles have been intensively investigated in view of their low cost, environmental benignity, and exceptionally wide range of appealing physical and chemical properties.4Zhang R. Elzatahry A.A. Al-Deyab S.S. Zhao D. Mesoporous titania: From synthesis to application.Nano Today. 2012; 7: 344-366Crossref Scopus (248) Google Scholar Up until now, most endeavors have focused on the exploration of their potentials in various applications. Further research for synthesizing mesoporous TiO2 micro- and nanoparticles in a highly controllable manner is very important for promoting their performance and potential transition from the lab bench to large-scale application. Many research groups worldwide are currently working in this field. However, the precise manipulation of the crystalline phase and micro- and/or nanostructure of mesoporous TiO2 particles remains unsolved. Now, Dongyuan Zhao and his team at Fudan University present results that could lead to new directions in the synthesis and applications of mesoporous oxide materials. Previously, the efficient approaches to preparing high-quality mesoporous TiO2 with a rutile phase remained scarce, and a single-crystal-like framework and asymmetric morphology were rarely reported. In this issue of Chem, Zhao’s team has developed a facile pressure-driven oriented assembly method for the fabrication of mesoporous rutile TiO2 microspheres with radially oriented mesochannels and a dehiscent architecture.5Lan K. Wang R. Zhang W. Zhao Z. Elzatahr A. Zhang X. Liu Y. Al-Dhayan D. Xia Y. Zhao D. Mesoporous TiO2 microspheres with precisely controlled crystallites and architectures.Chem. 2018; 4: 2436-2450Abstract Full Text Full Text PDF Scopus (48) Google Scholar The research reported by Zhao and co-workers has three remarkable advantages: (1) A truly unexpected single-crystal-like framework in a mesoporous TiO2 microsphere provides a new twist to the formation mechanism of mesoporous materials. This finding also encourages the possibility of forming novel structures for other transition-metal oxides, e.g., a similar tetrabutyl zirconate as a reaction precursor in the synthesis of mesoporous ZrO2 materials with single-crystal-like walls. (2) The facile achievement of mesoporous TiO2 with a tunable rutile/anatase phase ratio (0%–100%) comes from the precise control of acidity and oxygen content in the reaction system. High acidity and an oxygen-deficient environment favor the formation of a pure rutile phase under mild reaction condition. (3) The pressure-triggered evaporation process leads to the formation of mesoporous TiO2 microspheres with a unique dehiscent architecture. Although this is not a completely new structure, the successful synthesis of this special asymmetric hierarchically porous architecture is remarkable. It illustrates the crucial role of reaction kinetics in the formation of reaction products, as highlighted below. Figure 1 summarizes the formation process of mesoporous rutile TiO2 microspheres with a single-crystal-like framework and dehiscent morphology according to the results of Zhao and co-workers. The shown reaction process mainly involves two steps: (1) Mesoporous TiO2 microspheres are assembled by spherical composite micelles formed by the preferential evaporation of tetrahydrofuran (THF) solvent. Continuous evaporation of the residual THF and hydrolyzed solvents drives the oriented growth of both mesochannels and nanocrystal building blocks along the radial direction within the rutile TiO2 microspheres. (2) The vapor pressure generated from low-boiling-point solvent inside the microspheres ultimately exceeds the exterior hydrothermal pressure, thus forming splits on the surface of the microspheres. In the first step, the authors showed that high-temperature thermal treatment is not necessary for preparing mesoporous TiO2 in the rutile phase. In this regard, the relatively mild reaction condition constitutes a clear advantage given that the annealing process and use of specific protective templates can be avoided. Moreover, the authors carefully investigated rutile-to-anatase phase transition in this reaction system, which is attributed to two chemical processes occurring at the surface of nanosized TiO2 particles. First, the arrangement and growth of TiO6 octahedra through edge sharing initiate the rutile phase, whereas face sharing results in the anatase phase.6Yanagisawa K. Ovenstone J. Crystallization of anatase from amorphous titania using the hydrothermal technique: Effects of starting material and temperature.J. Phys. Chem. B. 1999; 103: 7781-7787Crossref Scopus (472) Google Scholar Highly concentrated HCl enables dispersion of TiO6 octahedra into discrete ones by protonating the surface Ti-OH groups, which is beneficial to the edge-sharing polycondensation between TiO6 octahedra, giving rise to the formation of the rutile phase.7Yin H. Wada Y. Kitamura T. Kambe S. Murasawa S. Mori H. Sakata T. Yanagida S. Hydrothermal synthesis of nanosized anatase and rutile TiO2 using amorphous phase tio2.J. Mater. Chem. 2001; 11: 1694-1703Crossref Scopus (526) Google Scholar Second, the oxygen-deficient environment favors the formation of high-activity TiO6 octahedra with oxygen vacancies at the surface,8Ricci P.C. Carbonaro C.M. Stagi L. Salis M. Casu A. Enzo S. Delogu F. Anatase-to-rutile phase transition in TiO2 nanoparticles irradiated by visible light.J. Phys. Chem. C. 2013; 117: 7850-7857Crossref Scopus (106) Google Scholar and the monomers prefer to form linear chains by sharing equatorial edges. Therefore, the nuclei grow to crystallinity with a high rutile-to-anatase phase ratio. This strategy is particularly remarkable because it overcomes the main limitation of the formation of mesoporous rutile TiO2. Additionally, these mesoporous rutile TiO2 particles show a single-crystal-like framework, making them ideal as mesoscopic photocatalysts. In this regard, there might be different attempts to synthesize other mesoporous oxide particles with single-crystal-like frameworks and controlled crystalline structures for various applications. In the second step, the formation of the unique dehiscent architecture is mainly due to the pressure-triggered evaporation process. The spherical composite precursors contain low-boiling-point solvents (THF and water). The increased hydrothermal temperature can cause intensive hydrolysis and higher vapor pressure inside microspheres. The vapor pressure ultimately exceeds the exterior hydrothermal pressure, and the solvents inside prefer to evaporate from certain regions, forming splits on the surface of microspheres. The application of dehiscent rutile TiO2 microspheres to photocatalytic H2 production is quite promising. There are several advantages with respect to photocatalysis, the most relevant of which are the ultrafast wettability and excellent capability of mass transport through the hierarchical pore systems. The rutile TiO2 catalyst exhibits higher photocatalytic activity and stability than conventional Ti-based materials and commercial P25. The potential of this type of TiO2 catalyst in other photocatalytic reactions deserves further investigations that could provide inspirations in the design of novel structured photocatalysts, and the simple approach reported in this work is expected to be applicable to the construction of numerous delicate nanostructures with diverse compositions under moderate conditions." @default.
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• W2896581680 title "Asymmetric Mesoporous Rutile TiO2 Microspheres with Single-Crystal-like Frameworks" @default.
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