Are There Really Low-Barrier Hydrogen Bonds in Proteins? The Case of Photoactive Yellow Protein
详细信息 查看全文
- 作者：Marc Nadal-Ferret ; Ricard Gelabert ; Miquel Moreno ; Jos茅 M. Lluch
- 刊名：Journal of the American Chemical Society
- 出版年：2014
- 出版时间：March 5, 2014
- 年：2014
- 卷：136
- 期：9
- 页码：3542-3552
- 全文大小：489K
- 年卷期：v.136,no.9(March 5, 2014)
- ISSN：1520-5126
文摘
For a long time, low-barrier hydrogen bonds (LBHBs) have been proposed to exist in many enzymes and to play an important role in their catalytic function, but the proof of their existence has been elusive. The transient formation of an LBHB in a protein system has been detected for the first time using neutron diffraction techniques on a photoactive yellow protein (PYP) crystal in a study published in 2009 (Yamaguchi, S.; et al. Proc. Natl. Acad. Sci. U.S.A. 2009, 106, 440鈥?44). However, very recent theoretical studies based on electronic structure calculations and NMR resonance experiments on PYP in solution (Saito, K.; et al. Proc. Natl. Acad. Sci. U.S.A. 2012, 109, 167鈥?72) strongly indicate that there is not such an LBHB. By means of electronic structure calculations combined with the solution of the nuclear Schr枚dinger equation, we analyze here under which conditions an LBHB can exist in PYP, thus leading to a more reasonable and conciliating understanding of the above-mentioned studies.