Molybdenum-mediated N2-splitting and functionalization in the presence of a coordinated alkyne
A new [PCCP]-coordinated molybdenum platform comprising a coordinated alkyne was employed for the cleavage of molecular dinitrogen. The coordinated η2-alkyne was left unaffected during this reduction. DFT calculations suggest that the reaction proceeds via an initially generated terminal N2-complex,...
Saved in:
| Main Authors: | , , |
|---|---|
| Format: | Article (Journal) |
| Language: | English |
| Published: |
07 October 2021
|
| In: |
Angewandte Chemie. International edition
Year: 2021, Volume: 60, Issue: 49, Pages: 25804-25808 |
| ISSN: | 1521-3773 |
| DOI: | 10.1002/anie.202111325 |
| Online Access: | Verlag, kostenfrei, Volltext: https://doi.org/10.1002/anie.202111325 Verlag, kostenfrei, Volltext: https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202111325 
|
| Author Notes: | Hannah K. Wagner, Hubert Wadepohl, and Joachim Ballmann |
MARC
| LEADER | 00000caa a2200000 c 4500 | ||
|---|---|---|---|
| 001 | 1815731036 | ||
| 003 | DE-627 | ||
| 005 | 20230427000539.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 220902s2021 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1002/anie.202111325 |2 doi | |
| 035 | |a (DE-627)1815731036 | ||
| 035 | |a (DE-599)KXP1815731036 | ||
| 035 | |a (OCoLC)1361714356 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rda | ||
| 041 | |a eng | ||
| 084 | |a 30 |2 sdnb | ||
| 100 | 1 | |a Wagner, Hannah |d 1993- |e VerfasserIn |0 (DE-588)1186093285 |0 (DE-627)1665407220 |4 aut | |
| 245 | 1 | 0 | |a Molybdenum-mediated N2-splitting and functionalization in the presence of a coordinated alkyne |c Hannah K. Wagner, Hubert Wadepohl, and Joachim Ballmann |
| 246 | 3 | 3 | |a Molybdenum-mediated N 2 -splitting and functionalization in the presence of a coordinated alkyne |
| 264 | 1 | |c 07 October 2021 | |
| 300 | |a 5 | ||
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a Computermedien |b c |2 rdamedia | ||
| 338 | |a Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Im Titel ist die Ziffer "2" beim Ausdruck "N2-splitting" tiefgestellt | ||
| 500 | |a Gesehen am 02.09.2022 | ||
| 520 | |a A new [PCCP]-coordinated molybdenum platform comprising a coordinated alkyne was employed for the cleavage of molecular dinitrogen. The coordinated η2-alkyne was left unaffected during this reduction. DFT calculations suggest that the reaction proceeds via an initially generated terminal N2-complex, which is converted to a dinuclear μ-(η1:η1)-N2-bridged intermediate prior to N−N bond cleavage. Protonation, alkylation and acylation of the resulting molybdenum nitrido complex led to the corresponding N-functionalized imido complexes. Upon oxidation of the N-acylated imido derivative in MeCN, a fumaronitrile fragment was built up via C−C coupling of MeCN to afford a dinuclear molybdenum complex. The key finding that the strong N≡N bond may be cleaved in the presence of a weaker, but spatially constrained C≡C bond contradicts the widespread paradigm that coordinated alkynes are in general more reactive than gaseous N2. | ||
| 650 | 4 | |a molybdenum | |
| 650 | 4 | |a N-functionalization | |
| 650 | 4 | |a nitrides | |
| 650 | 4 | |a nitrogen fixation | |
| 650 | 4 | |a phosphino alkyne ligands | |
| 700 | 1 | |a Wadepohl, Hubert |e VerfasserIn |0 (DE-588)1019812354 |0 (DE-627)691026572 |0 (DE-576)358886724 |4 aut | |
| 700 | 1 | |a Ballmann, Joachim |d 1979-2025 |e VerfasserIn |0 (DE-588)137662866 |0 (DE-627)594828848 |0 (DE-576)304830542 |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t Angewandte Chemie. International edition |d Weinheim : Wiley-VCH, 1998 |g 60(2021), 49, Seite 25804-25808 |h Online-Ressource |w (DE-627)320497879 |w (DE-600)2011836-3 |w (DE-576)111552060 |x 1521-3773 |7 nnas |a Molybdenum-mediated N2-splitting and functionalization in the presence of a coordinated alkyne |
| 773 | 1 | 8 | |g volume:60 |g year:2021 |g number:49 |g pages:25804-25808 |g extent:5 |a Molybdenum-mediated N2-splitting and functionalization in the presence of a coordinated alkyne |
| 775 | 0 | 8 | |i Parallele Sprachausgabe |n deutsch |a Wagner, Hannah, 1993 - |t Molybdän-vermittelte N2-Spaltung und Funktionalisierung in Gegenwart eines koordinierten Alkins |d 2021 |w (DE-627)1815713771 |
| 856 | 4 | 0 | |u https://doi.org/10.1002/anie.202111325 |x Verlag |x Resolving-System |z kostenfrei |3 Volltext |
| 856 | 4 | 0 | |u https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202111325 |x Verlag |z kostenfrei |3 Volltext |
| 951 | |a AR | ||
| 992 | |a 20220902 | ||
| 993 | |a Article | ||
| 994 | |a 2021 | ||
| 998 | |g 137662866 |a Ballmann, Joachim |m 137662866:Ballmann, Joachim |d 120000 |d 120200 |d 120000 |e 120000PB137662866 |e 120200PB137662866 |e 120000PB137662866 |k 0/120000/ |k 1/120000/120200/ |k 0/120000/ |p 3 |y j | ||
| 998 | |g 1019812354 |a Wadepohl, Hubert |m 1019812354:Wadepohl, Hubert |d 120000 |d 120200 |e 120000PW1019812354 |e 120200PW1019812354 |k 0/120000/ |k 1/120000/120200/ |p 2 | ||
| 998 | |g 1186093285 |a Wagner, Hannah |m 1186093285:Wagner, Hannah |d 120000 |d 120200 |e 120000PW1186093285 |e 120200PW1186093285 |k 0/120000/ |k 1/120000/120200/ |p 1 |x j | ||
| 999 | |a KXP-PPN1815731036 |e 4184428126 | ||
| BIB | |a Y | ||
| SER | |a journal | ||
| JSO | |a {"title":[{"title_sort":"Molybdenum-mediated N2-splitting and functionalization in the presence of a coordinated alkyne","title":"Molybdenum-mediated N2-splitting and functionalization in the presence of a coordinated alkyne"}],"person":[{"roleDisplay":"VerfasserIn","display":"Wagner, Hannah","role":"aut","family":"Wagner","given":"Hannah"},{"role":"aut","roleDisplay":"VerfasserIn","display":"Wadepohl, Hubert","given":"Hubert","family":"Wadepohl"},{"role":"aut","display":"Ballmann, Joachim","roleDisplay":"VerfasserIn","given":"Joachim","family":"Ballmann"}],"titleAlt":[{"title":"Molybdenum-mediated N 2 -splitting and functionalization in the presence of a coordinated alkyne"}],"language":["eng"],"recId":"1815731036","note":["Im Titel ist die Ziffer \"2\" beim Ausdruck \"N2-splitting\" tiefgestellt","Gesehen am 02.09.2022"],"type":{"media":"Online-Ressource","bibl":"article-journal"},"id":{"eki":["1815731036"],"doi":["10.1002/anie.202111325"]},"origin":[{"dateIssuedDisp":"07 October 2021","dateIssuedKey":"2021"}],"name":{"displayForm":["Hannah K. Wagner, Hubert Wadepohl, and Joachim Ballmann"]},"relHost":[{"physDesc":[{"extent":"Online-Ressource"}],"id":{"issn":["1521-3773"],"doi":["10.1002/(ISSN)1521-3773"],"eki":["320497879"],"zdb":["2011836-3"]},"origin":[{"dateIssuedDisp":"1998-","publisher":"Wiley-VCH","dateIssuedKey":"1998","publisherPlace":"Weinheim"}],"corporate":[{"roleDisplay":"Herausgebendes Organ","display":"Gesellschaft Deutscher Chemiker","role":"isb"}],"language":["eng"],"recId":"320497879","disp":"Molybdenum-mediated N2-splitting and functionalization in the presence of a coordinated alkyneAngewandte Chemie. International edition","type":{"bibl":"periodical","media":"Online-Ressource"},"note":["Gesehen am 20.12.2022","Fortsetzung der Druck-Ausgabe"],"titleAlt":[{"title":"Angewandte Chemie / International edition"}],"part":{"pages":"25804-25808","issue":"49","year":"2021","extent":"5","text":"60(2021), 49, Seite 25804-25808","volume":"60"},"pubHistory":["37.1998 -"],"title":[{"title_sort":"Angewandte Chemie","title":"Angewandte Chemie","subtitle":"a journal of the Gesellschaft Deutscher Chemiker","partname":"International edition"}]}],"physDesc":[{"extent":"5 S."}]} | ||
| SRT | |a WAGNERHANNMOLYBDENUM0720 | ||