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Cooperative Sulfur Transformations at a Dinickel Site: A Metal Bridging Sulfur Radical and Its H-Atom Abstraction Thermochemistry.

التفاصيل البيبلوغرافية
العنوان: Cooperative Sulfur Transformations at a Dinickel Site: A Metal Bridging Sulfur Radical and Its H-Atom Abstraction Thermochemistry.
المؤلفون: Tagliavini V; Institute of Inorganic Chemistry, University of Göttingen, Tammannstr. 4, D-37077 Göttingen, Germany., Duan PC; Institute of Inorganic Chemistry, University of Göttingen, Tammannstr. 4, D-37077 Göttingen, Germany., Chatterjee S; Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, D-45470 Mülheim an der Ruhr, Germany.; Department of Chemistry, Indian Institute of Technology Roorkee, Roorkee, Uttarakhand 247667, India., Ferretti E; Institute of Inorganic Chemistry, University of Göttingen, Tammannstr. 4, D-37077 Göttingen, Germany., Dechert S; Institute of Inorganic Chemistry, University of Göttingen, Tammannstr. 4, D-37077 Göttingen, Germany., Demeshko S; Institute of Inorganic Chemistry, University of Göttingen, Tammannstr. 4, D-37077 Göttingen, Germany., Kang L; Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, D-45470 Mülheim an der Ruhr, Germany., Peredkov S; Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, D-45470 Mülheim an der Ruhr, Germany., DeBeer S; Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, D-45470 Mülheim an der Ruhr, Germany., Meyer F; Institute of Inorganic Chemistry, University of Göttingen, Tammannstr. 4, D-37077 Göttingen, Germany.; International Center for Advanced Studies of Energy Conversion (ICASEC), University of Göttingen, Tammannstr. 6, D-37077 Göttingen, Germany.
المصدر: Journal of the American Chemical Society [J Am Chem Soc] 2024 Aug 21; Vol. 146 (33), pp. 23158-23170. Date of Electronic Publication: 2024 Aug 07.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: American Chemical Society Country of Publication: United States NLM ID: 7503056 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-5126 (Electronic) Linking ISSN: 00027863 NLM ISO Abbreviation: J Am Chem Soc Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة: Publication: Washington, DC : American Chemical Society
Original Publication: Easton, Pa. [etc.]
مستخلص: Starting from the dinickel(II) dihydride complex [ML(Ni-H) 2 ] ( 1 M ), where L 3- is a bis(tridentate) pyrazolate-bridged bis(β-diketiminato) ligand and M + is Na + or K + , a series of complexes [KLNi 2 (S 2 )] ( 2 K ), [MLNi 2 S] ( 3 M ), [LNi 2 (SMe)] ( 4 ), and [LNi 2 (SH)] ( 5 ) has been prepared. The μ-sulfido complexes 3 M can be reversibly oxidized at E 1/2 = -1.17 V (in THF; vs Fc + /Fc) to give [LNi 2 (S • )] ( 6 ) featuring a bridging S-radical. 6 has been comprehensively characterized, including by X-ray diffraction, SQUID magnetometry, EPR and XAS/XES spectroscopies, and DFT calculations. The p K a of the μ-hydrosulfido complex 5 in THF is 30.8 ± 0.4, which defines a S-H bond dissociation free energy (BDFE) of 75.1 ± 1.0 kcal mol -1 . 6 reacts with H atom donors such as TEMPO-H and xanthene to give 5 , while 5 reacts with 2,4,6-tri( tert -butyl)phenoxy radical in a reverse H atom transfer to generate 6 . These findings provide the first full characterization of a genuine M-(μ-S •- )-M complex and provide insights into its proton-coupled electron transfer (PCET) reactivity, which is of interest in view of the prominence of M-(μ-SH/μ-S)-M units in biological systems and heterogeneous catalysis.
References: J Am Chem Soc. 2004 Nov 10;126(44):14600-10. (PMID: 15521780)
J Am Chem Soc. 2001 Jun 27;123(25):6025-39. (PMID: 11414836)
Acta Crystallogr C Struct Chem. 2015 Jan;71(Pt 1):3-8. (PMID: 25567568)
Inorg Chem. 2020 Oct 5;59(19):14207-14217. (PMID: 32960575)
J Am Chem Soc. 2020 Apr 8;142(14):6717-6728. (PMID: 32163715)
Acc Chem Res. 2015 Nov 17;48(11):2967-75. (PMID: 26401686)
Inorg Chem. 2018 Aug 20;57(16):9670-9682. (PMID: 29561154)
J Am Chem Soc. 2018 Apr 11;140(14):4929-4939. (PMID: 29595258)
Chem Rev. 2022 Jan 12;122(1):1-49. (PMID: 34928136)
Acc Chem Res. 2020 Nov 17;53(11):2753-2761. (PMID: 33074643)
J Am Chem Soc. 2021 Jan 13;143(1):481-487. (PMID: 33356206)
Chem Commun (Camb). 2021 Jun 24;57(51):6264-6267. (PMID: 34075955)
Chem Rev. 2014 Apr 23;114(8):4149-74. (PMID: 24521136)
J Am Chem Soc. 2009 Apr 15;131(14):5224-32. (PMID: 19309157)
J Am Chem Soc. 1973 Jan 10;95(1):273-4. (PMID: 4682896)
Chem. 2023 Sep 14;9(9):2601-2609. (PMID: 39021493)
Chem Rev. 2004 Feb;104(2):527-59. (PMID: 14871134)
Inorg Chem. 2015 Oct 19;54(20):9770-6. (PMID: 26445295)
Angew Chem Int Ed Engl. 2019 Feb 4;58(6):1705-1709. (PMID: 30516873)
Inorg Chem. 2008 May 19;47(10):3931-3. (PMID: 18410087)
Coord Chem Rev. 2021 Feb 15;429:. (PMID: 33692589)
J Org Chem. 2016 Sep 2;81(17):7349-61. (PMID: 27392255)
J Am Chem Soc. 2023 Aug 23;145(33):18477-18486. (PMID: 37565682)
J Am Chem Soc. 2020 Jun 17;142(24):10681-10691. (PMID: 32432468)
Chem Commun (Camb). 2014 Jul 7;50(53):7014-6. (PMID: 24849692)
J Am Chem Soc. 2009 Jan 14;131(1):64-5. (PMID: 19072280)
J Am Chem Soc. 2008 Oct 15;130(41):13536-7. (PMID: 18803388)
Inorg Chem. 2007 Jan 22;46(2):486-96. (PMID: 17279827)
J Am Chem Soc. 2016 Sep 28;138(38):12352-5. (PMID: 27606792)
J Am Chem Soc. 2009 Oct 28;131(42):15212-24. (PMID: 19795866)
J Org Chem. 2006 Nov 24;71(24):9062-7. (PMID: 17109531)
Angew Chem Int Ed Engl. 2015 Dec 1;54(49):14956-9. (PMID: 26457792)
Chemphyschem. 2012 Feb;13(3):695-8. (PMID: 22262374)
Angew Chem Int Ed Engl. 2006 Feb 6;45(7):1138-41. (PMID: 16385608)
Chem Rev. 2020 Jun 24;120(12):5082-5106. (PMID: 32176472)
Acta Crystallogr A Found Adv. 2015 Jan;71(Pt 1):3-8. (PMID: 25537383)
Angew Chem Int Ed Engl. 2005 Dec 2;44(47):7745-8. (PMID: 16267877)
Chem Soc Rev. 2020 Jun 21;49(12):4070-4134. (PMID: 32420562)
Dalton Trans. 2021 Aug 28;50(32):11300-11306. (PMID: 34342320)
Met Ions Life Sci. 2020 Mar 23;20:. (PMID: 32851832)
Inorg Chem. 2019 Apr 15;58(8):5154-5162. (PMID: 30907585)
Proc Natl Acad Sci U S A. 2002 Dec 10;99(25):15971-6. (PMID: 12475995)
J Am Chem Soc. 2017 Nov 22;139(46):16720-16731. (PMID: 29037034)
Met Ions Life Sci. 2020 Mar 23;20:. (PMID: 32851828)
J Am Chem Soc. 2019 Aug 14;141(32):12682-12696. (PMID: 31299154)
Angew Chem Int Ed Engl. 2022 Sep 26;61(39):e202208544. (PMID: 35920055)
Inorg Chem. 2015 Apr 20;54(8):3815-28. (PMID: 25835183)
Chem Rev. 2020 Jun 24;120(12):5194-5251. (PMID: 32459087)
J Am Chem Soc. 2009 Jan 21;131(2):440-1. (PMID: 19099477)
Dalton Trans. 2009 Nov 21;(43):9410-7. (PMID: 19859595)
J Am Chem Soc. 2004 Jun 2;126(21):6522-3. (PMID: 15161258)
Inorg Chem. 2010 Apr 5;49(7):3104-12. (PMID: 20199095)
Angew Chem Int Ed Engl. 2021 Jan 25;60(4):1891-1896. (PMID: 33026170)
J Magn Reson. 2006 Jan;178(1):42-55. (PMID: 16188474)
Angew Chem Int Ed Engl. 2014 Mar 3;53(10):2750-3. (PMID: 24481669)
Science. 1997 Aug 1;277(5326):653-9. (PMID: 9235882)
J Am Chem Soc. 2008 Jul 16;130(28):8940-51. (PMID: 18564842)
Inorg Chem. 2015 Mar 16;54(6):2705-12. (PMID: 25742125)
Dalton Trans. 2016 Oct 7;45(37):14508-10. (PMID: 27139714)
Phys Chem Chem Phys. 2016 Apr 28;18(16):10688-99. (PMID: 26924248)
Inorg Chem. 2010 Aug 2;49(15):6817-9. (PMID: 20586478)
تواريخ الأحداث: Date Created: 20240807 Latest Revision: 20240828
رمز التحديث: 20240828
مُعرف محوري في PubMed: PMC11345757
DOI: 10.1021/jacs.4c05113
PMID: 39110481
قاعدة البيانات: MEDLINE
الوصف
تدمد:1520-5126
DOI:10.1021/jacs.4c05113