Proton mediated spin state transition of cobalt heme analogs
Abstract
The spin state transition from low spin to high spin upon substrate addition is one of the key steps in cytochrome P450 catalysis. External perturbations such as pH and hydrogen bonding can also trigger the spin state transition of hemes through deprotonated histidine (e.g. Cytochrome c). In this work, we report the isolated 2-methylimidazole Cobalt(II) [Co(TPP)(2-MeHIm)] and [Co(TTP)(2-MeHIm)], and the corresponding 2-methylimidazolate derivatives where the N–H proton of axial 2-MeHIm is removed. Interestingly, various spectroscopies including EPR and XAFS determine a high-spin state (S = 3/2) for the imidazolate derivatives, in contrast to the low-spin state (S = 1/2) of all known imidazole analogs. DFT assisted stereoelectronic investigations are applied to understand the metal-ligand interactions, which suggest that the dramatically displaced metal center allowing a promotion eg(dπ) → b1g(dx2–y2) is crucial for the occurrence of the spin state transition.
- Authors:
-
- Univ. of Chinese Academy of Sciences, Beijing (China)
- Nankai Univ., Tianjin (China)
- Chinese Academy of Sciences (CAS), Beijing (China)
- Beijing Normal Univ., Beijing (China)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Dalian Univ. of Technology, Dalian (China)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1526720
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhao, Jianping, Peng, Qian, Wang, Zijian, Xu, Wei, Xiao, Hongyan, Wu, Qi, Sun, Hao -Ling, Ma, Fang, Zhao, Jiyong, Sun, Cheng -Jun, Zhao, Jianzhang, and Li, Jianfeng. Proton mediated spin state transition of cobalt heme analogs. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-10357-z.
Zhao, Jianping, Peng, Qian, Wang, Zijian, Xu, Wei, Xiao, Hongyan, Wu, Qi, Sun, Hao -Ling, Ma, Fang, Zhao, Jiyong, Sun, Cheng -Jun, Zhao, Jianzhang, & Li, Jianfeng. Proton mediated spin state transition of cobalt heme analogs. United States. https://doi.org/10.1038/s41467-019-10357-z
Zhao, Jianping, Peng, Qian, Wang, Zijian, Xu, Wei, Xiao, Hongyan, Wu, Qi, Sun, Hao -Ling, Ma, Fang, Zhao, Jiyong, Sun, Cheng -Jun, Zhao, Jianzhang, and Li, Jianfeng. Fri .
"Proton mediated spin state transition of cobalt heme analogs". United States. https://doi.org/10.1038/s41467-019-10357-z. https://www.osti.gov/servlets/purl/1526720.
@article{osti_1526720,
title = {Proton mediated spin state transition of cobalt heme analogs},
author = {Zhao, Jianping and Peng, Qian and Wang, Zijian and Xu, Wei and Xiao, Hongyan and Wu, Qi and Sun, Hao -Ling and Ma, Fang and Zhao, Jiyong and Sun, Cheng -Jun and Zhao, Jianzhang and Li, Jianfeng},
abstractNote = {The spin state transition from low spin to high spin upon substrate addition is one of the key steps in cytochrome P450 catalysis. External perturbations such as pH and hydrogen bonding can also trigger the spin state transition of hemes through deprotonated histidine (e.g. Cytochrome c). In this work, we report the isolated 2-methylimidazole Cobalt(II) [Co(TPP)(2-MeHIm)] and [Co(TTP)(2-MeHIm)], and the corresponding 2-methylimidazolate derivatives where the N–H proton of axial 2-MeHIm is removed. Interestingly, various spectroscopies including EPR and XAFS determine a high-spin state (S = 3/2) for the imidazolate derivatives, in contrast to the low-spin state (S = 1/2) of all known imidazole analogs. DFT assisted stereoelectronic investigations are applied to understand the metal-ligand interactions, which suggest that the dramatically displaced metal center allowing a promotion eg(dπ) → b1g(dx2–y2) is crucial for the occurrence of the spin state transition.},
doi = {10.1038/s41467-019-10357-z},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Fri May 24 00:00:00 EDT 2019},
month = {Fri May 24 00:00:00 EDT 2019}
}
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