Hydrogen production by the Ruthenium(II) complex bearing a bulky PNP ligand: a catalyst for the decomposition of formic acid and/or ammonium formate
The five-coordinate complex [RuCl2(PNP)] (1) was synthesized from the binuclear [RuCl2(p-cym)]2 with a PNP-type ligand (PNP = 3,6-di-tert-butyl-1,8-bis(diisopropylphosphino)methyl)-9H-carbazole - (CbzdiphosiPr)H) in a toluene solution, within 20 h at 110 °C, producing a green solid, which was precip...
Gespeichert in:
| Hauptverfasser: | , , , , |
|---|---|
| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
24 December 2024
|
| In: |
ACS omega
Year: 2024, Jahrgang: 9, Heft: 51, Pages: 50758-50765 |
| ISSN: | 2470-1343 |
| DOI: | 10.1021/acsomega.4c09025 |
| Online-Zugang: | Verlag, kostenfrei, Volltext: https://doi.org/10.1021/acsomega.4c09025
|
| Verfasserangaben: | André L. Bogado, Leon Kambiz Paschai Darian, David Bürgy, Lucas da Silva dos Santos, and Leonardo Tsuyoshi Ueno |
MARC
| LEADER | 00000caa a2200000 c 4500 | ||
|---|---|---|---|
| 001 | 1919718818 | ||
| 003 | DE-627 | ||
| 005 | 20250717001050.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 250313s2024 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1021/acsomega.4c09025 |2 doi | |
| 035 | |a (DE-627)1919718818 | ||
| 035 | |a (DE-599)KXP1919718818 | ||
| 035 | |a (OCoLC)1528024896 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rda | ||
| 041 | |a eng | ||
| 084 | |a 30 |2 sdnb | ||
| 100 | 1 | |a Bogado, André Luiz |e VerfasserIn |0 (DE-588)1168677815 |0 (DE-627)1032445319 |0 (DE-576)511696469 |4 aut | |
| 245 | 1 | 0 | |a Hydrogen production by the Ruthenium(II) complex bearing a bulky PNP ligand |b a catalyst for the decomposition of formic acid and/or ammonium formate |c André L. Bogado, Leon Kambiz Paschai Darian, David Bürgy, Lucas da Silva dos Santos, and Leonardo Tsuyoshi Ueno |
| 246 | 3 | 0 | |a two |
| 264 | 1 | |c 24 December 2024 | |
| 300 | |b Illustrationen | ||
| 300 | |a 8 | ||
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a Computermedien |b c |2 rdamedia | ||
| 338 | |a Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Online veröffentlicht: 11. Dezember 2024 | ||
| 500 | |a Gesehen am 13.03.2025 | ||
| 520 | |a The five-coordinate complex [RuCl2(PNP)] (1) was synthesized from the binuclear [RuCl2(p-cym)]2 with a PNP-type ligand (PNP = 3,6-di-tert-butyl-1,8-bis(diisopropylphosphino)methyl)-9H-carbazole - (CbzdiphosiPr)H) in a toluene solution, within 20 h at 110 °C, producing a green solid, which was precipitated with a 1/1 mixture of n- pentane/HMDSO. The complex was characterized by NMR─1H, 13C, and 31P{1H}, mass spectroscopy─LIFDI, FTIR, UV/vis spectroscopy, and cyclic voltammetry, as well as a description of the optimized structure by DFT calculation. The reactivity of 1 was investigated in the presence of potassium triethylborohydride (KBEt3H, in THF solution of 1.0 mol L-1) and ammonium formate (NH4HCO2), producing an in situ hydride complex and a formate intermediate species coordinated to the ruthenium center. The complex 1, loaded with 0.08%, catalyzed the decomposition of ammonium formate (AF) into H2, CO2, and NH3 in THF solutions at 80 °C, with 94% of H2 and TOF = 206 h-1 (molar ratio [Ru]/AF = 1/1204). The catalytic activity increased remarkably for the decomposition of formic acid (FA) as a substrate to produce H2 and CO2. In the HMDSO solution at 80 °C, a conversion of 100% was obtained in relation to H2 and TOF = 3010 h-1 (molar ration [Ru]/FA/NEt3 = 1/1204/843). In an equimolar mixture of AF/FA in HMDSO solution at 80 °C, without additives, the complex 1 catalyzed the decomposition of both with 100% of H2 and TOF = 987 h-1 (molar ratio [Ru]/AF/FA= 1/602/602). Under the later conditions, as well as upon AF decomposition, carbamic acid [HO(C═O)NH2] was obtained as a coproduct of a secondary reaction between NH3 and CO2 (yield = 50% in relation to the amount of AF). A kinetic study for decomposing FA, in the range of 60-100 °C, provided ΔS‡ = −9.7 e.u, ΔG‡ = 13.35 kJ mol-1, and Ea = 64 kJ mol-1, suggesting that the mechanism is more associative than for the known complexes. | ||
| 700 | 1 | |a Paschai Darian, Leon K. |d 1997- |e VerfasserIn |0 (DE-588)1284327477 |0 (DE-627)1840028149 |4 aut | |
| 700 | 1 | |a Bürgy, David |d 1996- |e VerfasserIn |0 (DE-588)1214204112 |0 (DE-627)1725172615 |4 aut | |
| 700 | 1 | |a dos Santos, Lucas da Silva |e VerfasserIn |4 aut | |
| 700 | 1 | |a Ueno, Leonardo Tsuyoshi |e VerfasserIn |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t ACS omega |d Washington, DC : ACS Publications, 2016 |g 9(2024), 51 vom: Dez., Seite 50758-50765 |h Online-Ressource |w (DE-627)863132308 |w (DE-600)2861993-6 |w (DE-576)474097676 |x 2470-1343 |7 nnas |a Hydrogen production by the Ruthenium(II) complex bearing a bulky PNP ligand a catalyst for the decomposition of formic acid and/or ammonium formate |
| 773 | 1 | 8 | |g volume:9 |g year:2024 |g number:51 |g month:12 |g pages:50758-50765 |g extent:8 |a Hydrogen production by the Ruthenium(II) complex bearing a bulky PNP ligand a catalyst for the decomposition of formic acid and/or ammonium formate |
| 856 | 4 | 0 | |u https://doi.org/10.1021/acsomega.4c09025 |x Verlag |x Resolving-System |z kostenfrei |3 Volltext |
| 951 | |a AR | ||
| 992 | |a 20250313 | ||
| 993 | |a Article | ||
| 994 | |a 2024 | ||
| 998 | |g 1214204112 |a Bürgy, David |m 1214204112:Bürgy, David |d 120000 |d 120200 |e 120000PB1214204112 |e 120200PB1214204112 |k 0/120000/ |k 1/120000/120200/ |p 3 | ||
| 998 | |g 1284327477 |a Paschai Darian, Leon K. |m 1284327477:Paschai Darian, Leon K. |d 120000 |d 120200 |e 120000PP1284327477 |e 120200PP1284327477 |k 0/120000/ |k 1/120000/120200/ |p 2 | ||
| 999 | |a KXP-PPN1919718818 |e 4686640555 | ||
| BIB | |a Y | ||
| SER | |a journal | ||
| JSO | |a {"title":[{"title_sort":"Hydrogen production by the Ruthenium(II) complex bearing a bulky PNP ligand","subtitle":"a catalyst for the decomposition of formic acid and/or ammonium formate","title":"Hydrogen production by the Ruthenium(II) complex bearing a bulky PNP ligand"}],"person":[{"roleDisplay":"VerfasserIn","display":"Bogado, André Luiz","role":"aut","family":"Bogado","given":"André Luiz"},{"role":"aut","roleDisplay":"VerfasserIn","display":"Paschai Darian, Leon K.","given":"Leon K.","family":"Paschai Darian"},{"family":"Bürgy","given":"David","roleDisplay":"VerfasserIn","display":"Bürgy, David","role":"aut"},{"role":"aut","display":"dos Santos, Lucas da Silva","roleDisplay":"VerfasserIn","given":"Lucas da Silva","family":"dos Santos"},{"family":"Ueno","given":"Leonardo Tsuyoshi","display":"Ueno, Leonardo Tsuyoshi","roleDisplay":"VerfasserIn","role":"aut"}],"language":["eng"],"recId":"1919718818","note":["Online veröffentlicht: 11. Dezember 2024","Gesehen am 13.03.2025"],"type":{"media":"Online-Ressource","bibl":"article-journal"},"id":{"doi":["10.1021/acsomega.4c09025"],"eki":["1919718818"]},"origin":[{"dateIssuedKey":"2024","dateIssuedDisp":"24 December 2024"}],"name":{"displayForm":["André L. Bogado, Leon Kambiz Paschai Darian, David Bürgy, Lucas da Silva dos Santos, and Leonardo Tsuyoshi Ueno"]},"relHost":[{"title":[{"title":"ACS omega","title_sort":"ACS omega"}],"pubHistory":["Volume 1, issue 1 (July 2016)-"],"part":{"year":"2024","issue":"51","pages":"50758-50765","volume":"9","text":"9(2024), 51 vom: Dez., Seite 50758-50765","extent":"8"},"disp":"Hydrogen production by the Ruthenium(II) complex bearing a bulky PNP ligand a catalyst for the decomposition of formic acid and/or ammonium formateACS omega","note":["Gesehen am 25.06.2025"],"type":{"bibl":"periodical","media":"Online-Ressource"},"language":["eng"],"corporate":[{"role":"isb","roleDisplay":"Herausgebendes Organ","display":"American Chemical Society"}],"recId":"863132308","origin":[{"publisherPlace":"Washington, DC","dateIssuedDisp":"[2016]-","publisher":"ACS Publications"}],"id":{"issn":["2470-1343"],"zdb":["2861993-6"],"eki":["863132308"]},"name":{"displayForm":["American Chemical Society"]},"physDesc":[{"extent":"Online-Ressource"}]}],"physDesc":[{"noteIll":"Illustrationen","extent":"8 S."}]} | ||
| SRT | |a BOGADOANDRHYDROGENPR2420 | ||