Zhang, Shiyu - The Ohio State University - Department of Chemistry & Biochemistry

个人简介

Shiyu Zhang obtained B.S. in Chemistry and Biology from Jilin University, China (2010) and Ph.D. in Chemistry from Georgetown University (2015). As a graduate student, he worked in the group of Prof. Timothy Warren where he was awarded the ACS DIC Young Investigator Award in recognition of his work in the bioinorganic chemistry of nitric oxide. From 2015 to 2017, Shiyu conducted postdoctoral research under the joint supervision of Prof. Christopher Cummins at MIT and Prof. Daniel Nocera at Harvard, where he had the opportunity to develop novel electrolytes for electrochemical energy storage systems, such as Li-ion, Li-Air and redox flow batteries.

研究领域

Cooperative Reactivity of Bimetallic Complexes Metalloenzymes play a crucial role in multi-electron transfer reactions that are fundamental to all domains of life. These challenging cellular reactions, such as hydrocarbon oxidation and CO2 reduction, are driven by the cooperative reactivity of bimetallic protein sites composed of Earth-abundant transition metals. The Zhang group aims to synthetically model biological centers with high reactivities that have yet to be replicated by synthetic systems. We aim to (1) understand the fundamental bioinorganic chemistry underlying the bimetallic synergy, (2) mimic the enzymatic reactivities with synthetic bimetallic or trimetallic catalysts, and (3) develop new reactions that are beyond the scope of what biology accomplishes itself. C-H Functionalization Despite the growing interest in the synthesis of fluorinated organic compounds, few methods can incorporate fluoride ion directly into alkyl C−H bonds. We are developing C(sp3)−H fluorination methods with formally copper(III) fluoride complexes. Quantum chemical calculations reveal significant fluorine radical character for copper(III) fluoride, suggesting their ability to initiate and terminate a C(sp3)-H fluorination sequence. The capability of copper(III) fluoride to perform both hydrogen atom abstraction and radical capture was leveraged to enable fluorination of allylic and benzylic C−H bonds and α-C−H bonds of ethers at room temperature. Sustainable Organic Battery Materials Conversion and storage of renewable energy to electrical power are key challenges across the world for realizing net zero carbon emission. Further breakthroughs of secondary batteries are required to fulfill the future desires for electric vehicles. With the driving range of commercial EV now approaches 300 miles, the slow charging rate of the current lithium-ion battery technology has become one of the most pressing issues that the electric vehicle industry faces today. The Zhang lab seeks to develop a general approach to prepare sustainable organic battery materials for energy storage. Our goal is to synthesize redox-active molecules with multiple reversible redox couples and systematically optimize their performance in batteries.

近期论文

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“Nitrogen Oxides Catholyte for Rechargeable Battery” Zhang, W., Yang, X., and Zhang S.* Angew. Chem. Int. Ed. 2023, ASAP. Link “C(sp3)-H Cyanation by a Formal Copper(III) Cyanide Complex” Bower, J. K.,‡ Reese, M.,‡, Mazina, I. M., Zarnitsa, L. M., Cypcar, A. D., Moore, C. E., Sokolov, A. Y.,* and Zhang S.* Chem. Sci. 2023, Accepted. Link “Copper-catalyzed electrochemical C-H fluorination” Hintz, H., Bower, J., Tang, J., LaLama, M., Sevov, C.*, and Zhang S.* Chem. Catalysis, 2023, ASAP. Link “Reductive NO Coupling at Dicopper Center via a [Cu2(NO)2]2+ Diamond-Core Intermediate” Tao, W., Carter, S., Trevino, R., Zhang W., Shafaat, H. S.*, and Zhang S.* J. Am. Chem. Soc. 2022, 144, 22633–22640. Link “Controlling the direction of S-nitrosation vs. denitrosation: reversible cleavage and formation of S-N bond within a dicopper center” Tao, W., Yerbulekova, A., Moore, C. E., Shafaat, H. S.*, and Zhang S.* J. Am. Chem. Soc. 2022, 144, 2867–2872 Link “Multiple proton-coupled electron transfers at a tricopper cluster: modeling the reductive regeneration process in multicopper oxidases” Zhang, W., Moore, C. E., and Zhang, S.* J. Am. Chem. Soc. 2022, 144, 1709–1717. Link “Redox-active zinc thiolates for low-cost rechargeable aqueous Zn-ion batteries” Tuttle, M. R., Walter, C., Brackman, E., Moore, C. E., Espe, M., Rasik, C., Adams, P., and Zhang, S.* Chem. Sci. 2021, 12, 15253-15262. ‡ equal contribution. Link “Direct NO reduction by a biomimetic iron(II) pyrazolate MOF” Cai, Z., Tao, Q., Moore, C. E., Zhang, S. Wade, C. R.*, Angew. Chem. Int. Ed. 2021, 60, 21221-21225. Link “Redox-neutral S-nitrosation Mediated by a Dicopper Center” Tao, W. , Moore, C. E., Zhang, S.* Angew. Chem. Int. Ed. 2021, 60, 2-10. Link “Iron (II/III) Halide Complexes Promote the Interconversion of Nitric Oxide and S-nitrosothiols through Reversible Fe-S Interaction” Poptic, A. L., Zhang, S.* Inorg. Chem. 2021, 60, 7, 5190–5197. Link “Synergistic Effect of Hydrogen Bonding and π–π Stacking Enables Long Cycle Life in Organic Electrode Materials” Tuttle M. R., Davis, S. T., Zhang, S.* ACS. Energy Lett. 2021, 6, 643–649. Link “Encapsulation of tricopper cluster in a protein-like cavitand enables facile redox processes from CuICuICuI to CuIICuIICuII states” Zhang W., Moore, C. E., Zhang, S.* Chem. Sci. 2021,12, 2986-2992. Link “C(sp3)-H Fluorination with a Copper(II)/(III) Redox Couple” Bower J. K., Cypcar, A. D., Henriquez, B., Stieber, S. C. E.,* Zhang, S.* J. Am. Chem. Soc., 2020, 142, 8514–8521. Link “Bisthiazolyl Quinones: Stabilizing Organic Electrode Materials with Sulfur-Rich Thiazyl Motifs” Tuttle, M. R., Zhang, S.* Chem. Mater., 2020, 32, 255-261. Link “Dicopper µ-Oxo, µ-Nitrosyl complex from the activation of NO or nitrite at a dicopper center” Tao, W., Bower, J. K., Moore, C. E., Zhang, S.* J. Am. Chem. Soc. 2019, 141, 10159-10164. Link “Four‐Coordinate Copper Halonitrosyl {CuNO}¹⁰ Complexes.” Bower, J. K., Sokolov, A. Yu., Zhang, S.* Angew. Chem., Int. Ed., 2019, 58, 10225-10229. Link