I am working on mechanistic understandings of chemical reactions and developing concepts for heterogeneous catalysis based on systematic structural calculations. The past work can be summarized to be (a) Investigations of the catalytic activity of metal clusters based on systematic structural exploration. (b)Theoretical prediction of activities of surface catalysts based on systematic calculations of active sites.
Surface catalysis
Functionalization of inert material to be catalytic active opens a new route to designing novel catalytic material. I am interested in theoretical modifications of insulator materials, hexagonal boron nitride material (h-BN) and did a series of theoretical works to predict the activity of h-BN by introducing defects, metal support or heteroatoms. In particular, h-BN surface shows an unexpected catalytic property for supported metal clusters with experimental proof.
[1] M. Gao, A. Lyalin*, and T. Taketsugu J. Phys. Chem. C, 116, 9054-9062 (2012)
[2] M. Gao, A. Lyalin*, and T. Taketsugu J. Phys. Conference Series. 438, 012003 (2013)
[3] M. Gao, A. Lyalin*, and T. Taketsugu Int. J. Quantum Chem., 113, 443-452 (2013).
[4] M. Gao, A. Lyalin*, and T. Taketsugu J. Chem. Phys., 138, 034701 (2013)
[5] M. Gao, M. Adachi, A. Lyalin*, and T. Taketsugu* J. Phys. Chem. C, 120, 159993-16001 (2016)
[6] Y. Cao, P. Maitarad, M. Gao*, T. Taketsugu, H. Li, T. Yan, L. Shi, and D. Zhang* Appl. Catal. B-environ, 238,51-60, (2018)
[6] W. Qu, P. Wang, M. Gao, J. Hasegawa, Z. Shen, Q. Wang, R. Li, D. Zhang* Environ. Sci. Technol., 54, 9693-9701, (2020)
[7] M. Gao*, B. Wang, T. Tsuneda, A. Lyalin, T. Taketsugu* J. Phys. Chem. C, 125, 19219-19228 (2021)
[8] M. Gao*, M. Nakahara, A. Lyalin*, T. Taketsugu*, J. Phys. Chem. C,125, 1334-1344 (2021)
[9] S. Kuboon, J. Deng, M. Gao, K. Faungnawakij, J. Hasegawa, X. Zhang, L. Shi, and D. Zhang* Catal. Today, In press (2022)
2. Metal cluster catalysis
Catalysis by metal nanoparticles has been widely used in the chemical industry and environmental applications. Metal nanoparticles composed of tens of atoms (metal cluster) are very flexible, and possess various structures and active sites. Therefore, a metal cluster with high symmetry or high stability is chosen as a model for computational investigations.
We proposed a theoretical approach based on systematic exploration using GRRM to investigate the activation of small molecules on metal clusters. A systematic investigation was done to analyze the structure-activity relationship of gold clusters for H2 activation. It was shown that the most stable isomer is not always the most active one and several isomeric structures must be taken into account for an adequate description of the reaction rates at finite temperatures. It was the first example to show the importance of metal clusters geometry by systematic reaction pathways exploration. This approach and idea proposed were also applied to investigate fundamental reactions on metal clusters, such as H2 activation , O2 activation , CO2 adsorption and surface-supported metal clusters .
[1] M. Gao, A. Lyalin, S. Maeda*, and T. Taketsugu* J. Chem. Theo. Comp., 10, 1623-1630 (2014)
[2] M. Gao, A. Lyalin*, M. Takagi, S. Maeda*, and T. Taketsugu* J. Phys. Chem. C 119, 11120-11130 (2015)
[3] M. Gao, D. Horita, Y. Ono, A. Lyalin*, S. Maeda*, and T. Taketsugu* J. Phys. Chem. C, 121, 2661-2668 (2017)
[4] X. Song, M. R. Fagiani, S. Debnath, M. Gao, S. Maeda, T. Taketsugu, S. Gewinner, W. Schollkopf, K. R. Asmis*, and A. Lyalin* Phys. Chem. Chem. Phys., 19, 23154-23161 (2017)
[5] T. Iwasa*, T. Sato, M. Takagi, M. Gao, A. Lyalin, M. Kobayashi, K. Shimizu, S. Maeda, and T. Taketsugu* J. Phys. Chem. A, 123, 210-217 (2019)
[6] S. Debnath, X. Song, M. Fagiani, M. Weichman, M. Gao, S. Maeda, T. Taketsugu, W. Schollkopf, A. Lyalin*, D. Neumark, and K. Asmis* J. Phys. Chem. C, 123, 8439-8446 (2019)
[1] B. Wang, M. Gao, K. Uosaki, T. Taketsugu, Phys. Chem. Chem. Phys., 22, 12200-12208, (2020)
[2] B. Wang, M. Ito, M. Gao, H. Noguchi, K. Uosaki, and T. Taketsugu J. Phys. Chem. C, in press.
3. Enantioselective photoinduced Reaction Mechanism
[1] Y. Ueda, Y. Masuda, T. Iwai, K. Imaeda, H. Takeuchi, K.i Ueno, M. Gao, J. Hasegawa*, M. Sawamura* J. Am. Chem. Soc. 114, 2218-2224 (2022)
4. ·Cooperation works with experimental groups to reveal catalytic activity