Vol.11 no.3 2019

Research paper : Challenge towards synthesis of non-silica-based hybrid mesoporous materials (T. KIMURA)−121−Synthesiology - English edition Vol.11 No.3 (2018) AuthorTatsuo KIMURAGraduated from the Department of Applied Chemistry, School of Science and Engineering, Waseda University in March 1994. Completed courses at the Department of Applied Chemistry, Graduate School of Science and Engineering, Waseda University in March 1999; obtained doctorate (Engineering). Research Associate, Department of Applied Chemistry, School of Science and Engineering, Waseda University from April 1998. Joined the National Industrial Research Institute of Nagoya (currently, AIST Chubu) in October 2000; dispatched to the Nonferrous Metals Division and Metal Industries Division, Manufacturing Industries Bureau, the Ministry of Economy, Trade and industry (METI); and Group Leader, Materials for Chemical Transformation Group, Inorganic Functional Materials Research Institute, AIST from October 2016. Specialty is the inorganic materials chemistry. Engages mostly in researches on the precise synthesis of porous materials.[13]T. Kimura: Evaporation-induced self-assembly processcontrolled for obtaining highly ordered mesoporousmaterials with demanded morphologies, Chem. Rec., 16 (1),445–457 (2016).[14]H. Elhamzaoui, B. Jousseaume, H. Riague, T. Toupance,P.Dieudonné, C. Zakri, M. Maugey and H. Allouchi: Self- assembled tin-based bridged hybrid materials, J. Am. Chem.Soc., 126 (26), 8130–8131 (2004).[15]T. Kimura: Synthesis of novel mesoporous aluminumorganophosphonate by using organically bridgeddiphosphonic acid, Chem. Mater., 15 (20), 3742–3744 (2003).[16]T. Kimura: Synthesis of mesostructured and mesoporousaluminum organophosphonates prepared by usingdiphosphonic acids with alkylene groups, Chem. Mater., 17(2), 337–344 (2005).[17]T. Kimura: Oligomeric surfactant and triblock copolymersyntheses of aluminum organophosphonates with highlyordered mesoporous structures, Chem. Mater., 17 (22),5521–5528 (2005).[18]T. Kimura and K. Kato: Simple removal of oligomericsurfactants and triblock copolymers from mesostructuredprecursors of ordered mesoporous aluminumorganophosphonates, Microporous Mesoporous Mater., 101(1-2), 207–213 (2007).[19]T. Kimura and K. Kato: Synthesis of ordered mesoporousaluminum alkylenediphosphonates with integratedinorganic-organic hybrid frameworks, J. Mater. Chem., 17(6), 559–566 (2007).[20]T. Kimura: Advance in the synthetic strategy of mesoporousaluminum phosphonates, Phosphorus Letter, 91, 20–27(2018) (in Japanese).[21]B. Tian, X. Liu, B. Tu, C. Yu, J. Fan, L. Wang, S. Xie, G.D.Stucky and D. Zhao: Self-adjusted synthesis of orderedstable mesoporous minerals by acid-base pairs, NatureMater., 2 (3), 159–163 (2003).[22]T. Kimura: Molecular design of bisphosphonates to adjusttheir reactivity toward metal sources for the surfactant- assisted synthesis of mesoporous lms, Angew. Chem. Int.Ed., 56 (43), 13459–13463 (2017).[23]T. Kimura, K. Kato and Y. Yamauchi: Temperature-controlled and aerosol-assisted synthesis of aluminumorganophosphonate spherical particles with uniformmesopores, Chem. Commun., 33, 4938–4940 (2009).[24]T. Kimura, N. Suzuki, P. Gupta and Y. Yamauchi: Effectivemesopore tuning using aromatic compounds in the aerosol-assisted system of aluminum organophosphonate sphericalparticles, Dalton Trans., 39 (21), 5139–5144 (2010).[25]T. Kimura and Y. Yamauchi: General information to obtainspherical particles with ordered mesoporous structures,Chem. Asian J., 8 (1), 160–167 (2013).[26]TY. Ma and ZY. Yuan: Metal phosphonate hybridmesostructures: environmentally friendly multifunctionalmaterials for clean energy and other applications,ChemSusChem, 4 (10), 1407–1419 (2011).[27]YP. Zhu, TZ. Ren and ZY. Yuan: Mesoporous non-siliceousinorganic-organic hybrids: a promising platform fordesigning multifunctional materials, New J. Chem., 38 (5),1905–1922 (2014).[28]YP. Zhu, TY. Ma, YL. Liu, TZ. Ren and ZY. Yuan: Metalphosphonate hybrid materials: From densely layered tohierarchically nanoporous structures, Inorg. Chem. Front., 1(5), 360–383 (2014).[29]T. Kimura: A new family of nonsiliceous porous hybridsfrom bisphosphonates, J. Nanosci. Nanotechnol., 13 (4),2461–2470 (2013).Discussions with Reviewers1 OverallComment (Toshimi Shimizu and Motoyuki Akamatsu, AIST)This paper describes, in scenario style, the details of the course by which synthesis of a non-silica-based hybrid mesoporous material, which was considered difficult, was achieved. The challenging strategies and tactics involve selection of new starting materials and utilization of unconventional synthesis routes. I think it is significant that you were able to extend the composition and structure of mesoporous materials as a result of this research. The paper demonstrates that the integration of cumulative elemental technologies is important, using tools of sub-nanometer scale chemical species such as organic and metal species. Hence, the paper is suitable for publication in Synthesiology.2 Synthesis and integration of elemental technologiesComment & Question (Toshimi Shimizu)The author uses Fig. 3 to show individual items (1) to (6) as elemental technologies for the synthesis research for mesoporous materials, and emphasizes that their integration is essential in composition design control of advanced mesoporous materials. However, looking at the subchapter titles of the rst draft of this paper, rather than explanations of elemental technologies from (1) to (6), you provide explanations of new chemical materials and synthesis routes from silica to organosilica, alumina and titania, and then non-silica-based hybrid mesoporous materials. In other words, there is no specific explanation about the integration of elemental technologies. To deepen the readers’ understanding, I think you should clearly state what correlation exists between newly developed chemical materials and synthesis routes and the elemental technologies (1) to (6), as well as specic contents about the integration of elemental technologies. Also, here is a question: Is the route newly developed by the author (Fig. 4 and Fig. 5) neither the liquid crystal template route shown in Fig. 3 nor the concerted organization route?Answer (Tatsuo Kimura)In the process of synthesizing mesoporous silica shown in

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