Tuning Spin Crossover Properties in Hofmann-Type Framework by Guest-Adaptive Deformation
Corresponding Author
Kai-Ping Xie
School of Chemistry and Materials Engineering, Huizhou University, Huizhou, Guangdong, 516007 China
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorHai-Ling Wang
School of Chemistry and Chemical Engineering, Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi Colleges and Universities Key Laboratory of Applied Chemistry Technology and Resource Development, Guangxi University, Nanning, Guangxi, 530004 China
Search for more papers by this authorZe-Yu Ruan
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorPei-Yu Liao
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorGuang Yang
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorCorresponding Author
Zi-Cheng Xiao
School of Chemistry and Materials Engineering, Huizhou University, Huizhou, Guangdong, 516007 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorCorresponding Author
Yi-Fei Deng
Department of Chemistry, Southern University of Science and Technology, Shenzhen, Guangdong, 518055 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorCorresponding Author
Si-Guo Wu
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorYan Shi
School of Chemistry and Materials Engineering, Huizhou University, Huizhou, Guangdong, 516007 China
Search for more papers by this authorMing-Liang Tong
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorCorresponding Author
Kai-Ping Xie
School of Chemistry and Materials Engineering, Huizhou University, Huizhou, Guangdong, 516007 China
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorHai-Ling Wang
School of Chemistry and Chemical Engineering, Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi Colleges and Universities Key Laboratory of Applied Chemistry Technology and Resource Development, Guangxi University, Nanning, Guangxi, 530004 China
Search for more papers by this authorZe-Yu Ruan
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorPei-Yu Liao
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorGuang Yang
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorCorresponding Author
Zi-Cheng Xiao
School of Chemistry and Materials Engineering, Huizhou University, Huizhou, Guangdong, 516007 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorCorresponding Author
Yi-Fei Deng
Department of Chemistry, Southern University of Science and Technology, Shenzhen, Guangdong, 518055 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorCorresponding Author
Si-Guo Wu
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
E-mail: [email protected]; [email protected]; [email protected]; [email protected]Search for more papers by this authorYan Shi
School of Chemistry and Materials Engineering, Huizhou University, Huizhou, Guangdong, 516007 China
Search for more papers by this authorMing-Liang Tong
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, Guangdong, 510275 China
Search for more papers by this authorComprehensive Summary
Three three-dimensional Hofmann-type metal-organic frameworks (MOFs) [Fe(bpn){Ag(CN)2}2]·Ph2S (1·Ph2S, bpn = 1,4-di(pyridin-4-yl)naphthalene, Ph2S = diphenylsulfide), [Fe(bpn){Ag(CN)2}2]·Ph2SO (1·Ph2SO, Ph2SO = diphenylsulfoxide) and [Fe(bpn){Ag(CN)2}2]·Ph2SO2 (1·Ph2SO2, Ph2SO2 = diphenylsulfone) were synthesized by employing sulfur-containing aromatic guests varying in oxidation states. 1·Ph2S performed a complete four-step spin crossover (SCO) behavior with the sequence of HS↔~LS1/3HS2/3↔~LS1/2HS1/2↔ ~LS2/3HS1/3↔LS, while an incomplete two-step SCO profile with the sequence of HS↔~LS1/3HS2/3↔~LS2/3HS1/3 and a faint SCO behavior at low temperature for 1·Ph2SO and 1·Ph2SO₂. Photomagnetic experiments indicate the light-induced excited spin-state trapping (LIESST) effect in 1·Ph2S and the bi-directional LIESST effect for 1·Ph2SO and 1·Ph2SO₂. Variable-temperature structural analyses reveal the evolution of host-guest synergy and highlight the mechanism of adaptive deformation of guests mediated by phenyl rotation amid spin transition. As the oxidation state of sulfur-containing guests increases, the host-guest cooperation within the lattice is limited by the steric effect, which stabilizes the high-spin state and consequently diminishes the SCO capability in this system. These results demonstrated herein open a new perspective on host-guest chemistry within SCO frameworks.
Supporting Information
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Appendix S1: Supporting Information |
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