AI Article Synopsis
Article Abstract
We have employed in situ electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) and density functional theory (DFT) calculations to study the CO reduction reaction (CORR) on Cu single-crystal surfaces under various conditions. Coadsorbed and structure-/potential-dependent surface species, including *CO, Cu-O , and Cu-OH , were identified using electrochemical spectroscopy and isotope labeling. The relative abundance of *OH follows a "volcano" trend with applied potentials in aqueous solutions, which is yet absent in absolute alcoholic solutions. Combined with DFT calculations, we propose that the surface H O can serve as a strong proton donor for the first protonation step in both the C and C pathways of CORR at various applied potentials in alkaline electrolytes, leaving adsorbed *OH on the surface. This work provides fresh insights into the initial protonation steps and identity of key interfacial intermediates formed during CORR on Cu surfaces.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1002/anie.202214210 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Electron-Donating Zr Induces Suppressed Ru Over-Oxidation and Accelerated Deprotonation Process Toward Efficient and Durable Water Electrolysis.
Small
January 2025
State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin, 130022, China.
The scarcity of cost-effective and durable iridium-free anode electrocatalysts for the oxygen evolution reaction (OER) poses a significant challenge to the widespread application of the proton exchange membrane water electrolyzer (PEMWE). To address the electrochemical oxidation and dissolution issues of Ru-based electrocatalysts, an electron-donating modification strategy is developed to stabilize WRuO under harsh oxidative conditions. The optimized catalyst with a low Zirconium doping (Zr, 1 wt.
View Article and Find Full Text PDFSupramolecularly Built Local Electric Field Microenvironment around Cobalt Phthalocyanine in Covalent Organic Frameworks for Enhanced Photocatalysis.
J Am Chem Soc
January 2025
Hefei National Research Center for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
The local electric field (LEF) plays an important role in the catalytic process; however, the precise construction and manipulation of the electric field microenvironment around the active site remains a significant challenge. Here, we have developed a supramolecular strategy for the implementation of a LEF by introducing the host macrocycle 18-crown-6 (18C6) into a cobalt phthalocyanine (CoPc)-containing covalent organic framework (COF). Utilizing the supramolecular interaction between 18C6 and potassium ion (K), a locally enhanced K concentration around CoPc can be built to generate a LEF microenvironment around the catalytically active Co site.
View Article and Find Full Text PDFPaddlewheel-type and half-paddlewheel-type diruthenium(II,II) complexes with 1,8-naphthyridine-2-carboxylate.
Dalton Trans
January 2025
Department of Chemistry, Graduate School of Natural Science and Technology, Shimane University, 1060, Nishikawatsu, Matsue, Shimane, 690-8504, Japan.
Paddlewheel-type diruthenium(II,II) complexes are paramagnetic with two unpaired electrons ( = 1) and can be utilized as versatile building blocks for higher-order structures, such as supramolecular complexes, coordination polymers, and metal-organic frameworks, although they are generally highly air-sensitive. In this study, we developed an air-stable paddlewheel-type diruthenium(II,II) complex with two electron-withdrawing 1,8-naphthyridine-2-carboxylate (npc) ligands, [Ru(μ-npc)(OCMe)] (1). The two acetate ligands in 1 can be replaced by other carboxylate ligands; the solvothermal reactions of 1 with benzoic acid (HOCPh) yields the heteroleptic [Ru(μ-npc)(OCPh)] (2), whereas its reaction with 1,8-naphthyridine-2-carboxylic acid (Hnpc) produces the homoleptic [Ru(μ-npc)(η-npc)] (3).
View Article and Find Full Text PDFEffect of the Electrolyte on the Oxygen Reduction Reaction with PCN-224(Co).
ChemSusChem
January 2025
Leiden University: Universiteit Leiden, Leiden Institute of Chemistry, Einsteinweg 55, Room number EE4.19, 2333 CC, Leiden, NETHERLANDS, KINGDOM OF THE.
Electrocatalysis in metal-organic frameworks is an interplay between the diffusion of charges, the intrinsic catalytic rate, and the mass-transport of reactants through the pores. Here a systematic study is carried out to investigate the role of the electrolyte nature and concentration on the oxygen reduction reaction (ORR) with the PCN-224(Co) MOF in aqueous electrolyte. It was found that the ORR activity is slightly influenced by the nature of the ions in solution, providing that the ionic strength is high enough to minimize the resistivity during the measurement.
View Article and Find Full Text PDFFirst-principles study of CO and HO adsorption on the anatase TiO(101) surface: effect of Au doping.
Phys Chem Chem Phys
January 2025
Shanxi Coal International Energy Group Co., Ltd., Taiyuan 030000, China.
Photocatalytic reduction of CO will play a major role in future energy and environmental crisis. To investigate the adsorption mechanisms of CO and HO molecules involved in the catalytic process on the surface of anatase titanium dioxide 101 (TiO(101)) and the influence of Au atom doping on their adsorption, first-principles density functional theory calculations were used. The results show that 1.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!