Vol.11 no.3 2019

Research paper : Challenge towards synthesis of non-silica-based hybrid mesoporous materials (T. KIMURA)−122−Synthesiology - English edition Vol.11 No.3 (2018) Fig. 1, the elemental technologies that must be considered can be categorized into (1) to (6). Excluding elemental technology (6), it is correct in understanding that mesoporous silica is synthesized by their integration. The importance becomes more apparent in materials like non-silica-based materials in which obtaining mesoporosity is difficult. The mesoporous materials cannot be synthesized just by improving individual elemental technologies. Therefore, particularly important technology is how to control bond formation of inorganic species in solution, as stated in elemental technology (1). This is explained in the section about the difficulties of synthesizing non-silica-based mesoporous materials. Moreover, in elemental technology (5) that seems to have low relationship with others, the results are affected by the integrity of the periodic structure (high symmetry) and the degree of condensation of the silicate framework in the mesoporous silica precursor. As a result, it is reported that the mesoporous structure disintegrates during the process of removing amphiphilic organic molecules.The precursors of mesoporous materials is invariably formed by either the liquid crystal template route or the concerted organization route. In this research a new formation route was not developed. Therefore, I corrected Fig. 4 and Fig. 5 so the details of the synthesis route would correspond to the numbering of elemental technologies. In this research, new composition design technology was proposed and demonstrated using the reaction of organic bridged phosphonate compounds and metal sources to achieve non-silica-based inorganic-organic composites with the ingredients that surround the assembly of amphiphilic organic molecules.Comment (Motoyuki Akamatsu)In the first two paragraphs of Chapter 2, you describe the silica-based synthesis route and that synthesis occurs through a concerted organization route. Based on this, you identify six elemental technologies, and your claim is that these six elemental technologies must be integrated for non-silica-based materials. Then you describe the development of non-silica-based mesoporous materials in Chapter 3 in which you state the selection of materials in Subchapter 3.0 and reactivity control in Subchapter 3.2. However, non-specialist readers cannot easily understand which of the six elemental technologies corresponds to which part of the description. Can you make the corresponding relation easier to understand? I think it will make things clear if explanations of the elemental technologies follow the subchapters of Chapter 3.Answer (Tatsuo Kimura)I thought I clearly showed the important elemental technologies in the figure for formation mechanism of Fig. 4 (silica-based hybrid materials) and Fig. 5 (non-silica-based hybrid materials). However, it seems that it was difcult to understand for non-specialist readers, so I decided to use the numbering of the six elemental technologies.3 Research strategyComment & Question (Motoyuki Akamatsu)In Paragraph 5, Chapter 1, you explain that while a study of hybrid mesoporous materials by silica-based materials is R&D that “specializes on functional design,” this research (= non-silica-based hybrid mesoporous materials) took a research strategy (= research policy?) of “designing the pore environment.” What is the essential difference between the two? While silica-based materials followed a goal-oriented approach (of developing a material to realize a certain function), why didn’t you take such a goal-oriented approach here? Please explain your views behind this.Answer (Tatsuo Kimura)The essential difference of the research strategies of “specializing in functional design” and “designing the pore environment” is as follows.Silica-based mesoporous material is made to express functions (acidity, oxidizing function, etc.) that are not expressed with silica alone by introducing different element species into the silicate framework, and at times organic groups are incorporated into the silica framework as in mesoporous organosilica. In any case, design is specific such as for catalyst function or photoresponsivity, and components that are necessary for functional expression (goal oriented) are introduced. However, since there is no option other than using the pore environment provided by the final product, the design of the environment inside the pore is essential for efcient functional expression.In this research, I discuss the difculty of synthesis research for hybrid mesoporous materials and the level I have achieved so far. In other words, the discussion is about the methodology for designing the pore environment. Ultimately, if I utilize the ndings necessary for functional design that had been claried for silica-based materials, I believe I can design a nanoscale chemical reaction eld where functions can be expressed efciently.For the question why I did not take a goal-oriented approach for non-silica-based hybrid mesoporous materials that is the target of this research, that is because I have not reached the stage in which I can freely synthesize with a goal in mind. Even for a silica-based mesoporous material, it cannot be synthesized on demand. Because there are overwhelming number of reports and the selection range has expanded, it merely looks like there are lots of accomplishments in “specializing on functional design” that is actually the next phase of research. In non-silica-based materials, as described in this paper, the reactivity of raw materials is fast, and an enormous amount of experimental samples are needed to synthesize just one type of mesoporous material with a certain inorganic composition. Therefore, I think there is great significance that I opened a path toward diversification of non-silica-based hybrid mesoporous materials through an approach of continuous control of reactivity of the raw materials, as shown in this study.4 New properties of materials and expanded usageComment (Toshimi Shimizu)By extending the composition of mesoporous materials from the current silica to organosilica, or from silica to alumina and then to titania, and from organosilica to non-silica hybrids, I can expect the expansion of structure, function, and property value of mesoporous materials. To strengthen the significance of this paper, how about adding specic new properties and advantages I can expect through the development of a universal synthesis method for non-silica-based hybrid mesoporous materials? Also, if possible, I think it will help the readers understand the research objective if you add the potential and expectations on how such development will contribute to industrial and social demands. There is a section at the bottom of Fig. 1 that points to this. However, it is organized by items “silica and alumina,” “transition metal oxides,” “carbon,” “metals,” and “hybrid materials,” and they do not correspond to the terminology used in this paper like “non-silica-based” or “non-silica-based hybrid.”Answer (Tatsuo Kimura)For the point that you indicated, I added a text to Paragraph 3, Chapter 1 of the nal draft. Also, for the section at the bottom of Fig. 1, I added a simple explanation to Paragraph 3, Chapter 1.Comment & Question (Motoyuki Akamatsu)In Chapter 1, you write, “the primary research strategy of this research is the design of pore environment,” and after that you write, “I set the goal as the design of hydrophilic surface structure.” Does this mean the specific goal of “designing the pore environment” is the “designing of the hydrophilic surface

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