A new PC(carbene)P pincer ligand with 2,3-benzo[b]thiophene linkers connecting the flanking dialkyl phosphine donors to the central carbene can be attached to Ir(I). The chloro derivative reacts with N2O with loss of N2 to form an iridaepoxide species by addition of an oxygen atom to the Ir═C linkage. This compound reacts with H2 to afford the oxidative addition product, in which the hydride ligands are trans to the Ir-O bond. Heating this dihydride results in slow release of H2O; kinetic and spectroscopic studies show that conversion of the dihydride to its isomer, in which the hydrides are cis to the Ir-O bond, is required for H2O elimination to take place. Together, these reactions constitute the stoichiometric conversion of N2O and H2 to N2 and H2O; further mechanistic studies suggest ways to make the system catalytic.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1021/ja512602m | DOI Listing |
J Phys Condens Matter
December 2024
Departmet of Physics(MMV), Banaras Hindu University, Varanasi, Varanasi, Uttar Pradesh, 221005, INDIA.
We report a detailed experimental study of the structural, magnetic and electrical properties of La and Ru doped (Sr1-x Lax)2Ir1-xRuxO4 (x= 0.05, 0.15).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Key Laboratory of Material Chemistry for Energy Conversion and Storage (Huazhong University of Science and Technology), Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
Low-iridium acid-stabilized electrocatalysts for efficient oxygen evolution reaction (OER) are crucial for the market deployment of proton exchange membrane (PEM) water electrolysis. Manipulating the in situ reconstruction of Ir-based catalysts with favorable kinetics is highly desirable but remains elusive. Herein, we propose an atomic ordering strategy to modulate the dynamic surface restructuring of catalysts to break the activity/stability trade-off.
View Article and Find Full Text PDFJ Am Chem Soc
November 2024
Department of Chemistry, Chemical Engineering Division, The Electrochemical Energy, Catalysis and Materials Science Laboratory, Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany.
Reducing the iridium demand in Proton Exchange Membrane Water Electrolyzers (PEM WE) is a critical priority for the green hydrogen industry. This study reports the discovery of a TiO-supported Ir@IrO(OH) core-shell nanoparticle catalyst with reduced Ir content, which exhibits superior catalytic performance for the electrochemical oxygen evolution reaction (OER) compared to a commercial reference. The TiO-supported Ir@IrO(OH) core-shell nanoparticle configuration significantly enhances the OER Ir mass activity from 8 to approximately 150 A g at 1.
View Article and Find Full Text PDFNano Lett
May 2024
Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang 325035, China.
Tuning electronic characteristics of metal-ligand bonds based on reaction pathways to achieve efficient catalytic processes has been widely studied and proven to be feasible in homogeneous catalysis, but it is scarcely investigated in heterogeneous catalysis. Herein, we demonstrate the regulation of the electronic configuration of Ir-O bonds in an Ir single-atom catalyst according to the borane activation mechanism. Ir-O bonds in Ir/Ni(OH) are found to be more electron-poor than those in Ir/NiO.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2023
State Key Laboratory of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
The construction of highly active, durable, and cost-effective catalysts is urgently needed for green hydrogen production. Herein, catalysts consisting of high-density Pt (24 atoms nm ) and Ir (32 atoms nm ) single atoms anchored on Co(OH) were constructed by a facile one-step approach. Remarkably, Pt /Co(OH) and Ir /Co(OH) only required 4 and 178 mV at 10 mA cm for hydrogen evolution reaction and oxygen evolution reaction, respectively.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!