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Volume 24, No.4 Pages 429 - 430

4. SPring-8/SACLA通信/SPring-8/SACLA COMMUNICATIONS

2017A期 採択長期利用課題の事後評価について – 1 –
Post-Project Review of Long-term Proposals Starting in 2017A -1-

(公財)高輝度光科学研究センター 利用推進部 User Administration Division, JASRI

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SPring-8

 

 2017A期に採択された長期利用課題について、2018B期に2年間の実施期間が終了したことを受け、第64回SPring-8利用研究課題審査委員会長期利用分科会(2018年12月13日および14日開催)による事後評価が行われました。
 事後評価は、長期利用分科会が実験責任者に対しヒアリングを行った後、評価を行うという形式で実施し、SPring-8利用研究課題審査委員会で評価結果を取りまとめました。以下に評価を受けた課題の評価結果を示します。研究内容については本誌の「最近の研究から」に実験責任者による紹介記事を掲載しています。
 なお、2017A期に採択された長期利用課題4課題のうち残り2課題の評価結果は次号以降に掲載する予定です。

 

-課題1-
課題名 NRVS of mononuclear and binuclear non-heme iron enzyme intermediates and related model complexes
実験責任者(所属) Solomon Edward(Stanford University)
採択時課題番号 2017A0137
ビームライン BL09XU
利用期間/配分総シフト 2017A~2018B/93シフト

 

[評価結果]
 This program was conducted as a renewal of the long-term project performed previously in 2013B - 2016A. The applicant defined the goal of the research project as to understand the geometric and electronic structure of mononuclear and binuclear non-heme irons in enzymes. The applicant is working with general interests on the enzymes but also focuses on the interaction of oxygens with the irons, which is quite informative to understand its biologically important roles in human health, catalysis and bioremediation, and so on.
 During the period of the program, the applicant and his colleagues have established and polished the powerful combination of NRVS and DFT, and routinely collected high-quality NRVS spectra to determine and analyze accurate structures of the metal centers. In particular, they revealed the reaction intermediates of an extradiol dioxygenase, homoprotocatechuate 2,3-deoxygenase using a freeze trap method. Furthermore, its NRVS structure can correct the relevant crystal structure determined previously. These results have expanded the experimental applicability and reliability of NRVS for iron proteins, and led to 7 articles published in major journals.
 As described above, the committee concluded that this long-term project was successfully conducted.

 

[成果リスト]
(査読付き論文)

[1] SPring-8 publication ID = 37162
K. Sutherlin et al.: "NRVS Studies of the Peroxide Shunt Intermediate in a Rieske Dioxygenase and Its Relation to the Native FeII O2 Reaction" Journal of the American Chemical Society 140 (2018) 5544-5559.

[2] SPring-8 publication ID = 37163
K. Sutherlin et al.: "Nuclear Resonance Vibrational Spectroscopy Definition of O2 Intermediates in an Extradiol Dioxygenase: Correlation to Crystallography and Reactivity" Journal of the American Chemical Society 140 (2018) 16495-16513.

 

 

-課題2-
課題名 Application & Development of Nuclear Resonance Vibrational Spectroscopy (NRVS) and Synchrotron Mössbauer Spectroscopy of Iron-Hydrogen Interactions in Hydrogenases, Nitrogenases, and Model Complexes
実験責任者(所属) Stephen Cramer(University of California, Davis)
採択時課題番号 2017A0141
ビームライン BL09XU
利用期間/配分総シフト 2017A~2018B/84シフト

 

[評価結果]
 The principal investigator focused on the investigation of the chemistry of hydrogen combined with metals, especially the nature of Fe-H bonds in enzymes which are important for the future energy and environment issues. In order to analyze the active site structures of the enzymes with organometallic transition metals, he introduced the NRVS (Nuclear Resonance Vibrational Spectroscopy) technique with the DFT calculations.
 Although it is regrettable that technical developments to reduce measurement time were not carried out extensively, the committee recognizes the scientific achievements and appreciates that the PI published many high-impact original and review papers, and delivered several invited talks.

 

[成果リスト]
(査読付き論文)

[1] SPring-8 publication ID = 37054
E. Reijerse et al.: "Direct Observation of an Iron-Bound Terminal Hydride in [FeFe]-Hydrogenase by Nuclear Resonance Vibrational Spectroscopy" Journal of the American Chemical Society 139 (2017) 4306-4309.

[2] SPring-8 publication ID = 37058
V. Pelmenschikov et al.: "Reaction Coordinate Leading to H2 Production in [FeFe]-Hydrogenase Identified by Nuclear Resonance Vibrational Spectroscopy and Density Functional Theory" Journal of the American Chemical Society 139 (2017) 16894-16902.

[3] SPring-8 publication ID = 37071
M. Carlson et al.: "Sterically Stabilized Terminal Hydride of a Diiron Dithiolate" Inorganic Chemistry 57 (2018) 1988-2001.

[4] SPring-8 publication ID = 37072
L. Gee et al.: "NRVS for Fe in Biology: Experiment and Basic Interpretation" Methods in Enzymology 599 (2018) 409-425.

[5] SPring-8 publication ID = 37073
C. Pham et al.: "Terminal Hydride Species in [FeFe]-Hydrogenases Are Vibrationally Coupled to the Active Site Environment" Angewandte Chemie International Edition 57 (2018) 10605-10609.

[6] SPring-8 publication ID = 37074
V. Pelmenschikov et al.: "High-Frequency Fe-H Vibrations in a Bridging Hydride Complex Characterized by NRVS and DFT" Angewandte Chemie International Edition 57 (2018) 9367-9371.

 

 

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[ - Vol.15 No.4(2010)]
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