On-surface chemistry holds the potential for ultimate miniaturization of functional devices. Porphyrins are promising building-blocks in exploring advanced nanoarchitecture concepts. More stable molecular materials of practical interest with improved charge transfer properties can be achieved by covalently interconnecting molecular units. On-surface synthesis allows to construct extended covalent nanostructures at interfaces not conventionally available. Here, we address the synthesis and properties of covalent molecular network composed of interconnected constituents derived from halogenated nickel tetraphenylporphyrin on Au(111). We report that the π-extended two-dimensional material exhibits dispersive electronic features. Concomitantly, the functional Ni cores retain the same single-active site character of their single-molecule counterparts. This opens new pathways when exploiting the high robustness of transition metal cores provided by bottom-up constructed covalent nanomeshes.
Download full-text PDF |
Source |
|---|---|
| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9827996 | PMC |
| http://dx.doi.org/10.1002/anie.202210326 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Constructing atomically dispersed Ni-Mn catalysts for electrochemical CO reduction over the wide potential window.
J Colloid Interface Sci
January 2025
Henan Key Laboratory of Polyoxometalate Chemistry, College of Chemistry and Molecular Sciences, Henan University, Kaifeng 475004, PR China. Electronic address:
Single-atom catalysts (SACs), known for their high atomic utilization efficiency, are highly attractive for electrochemical CO conversion. Nevertheless, it is struggling to use a single active site to overcome the linear scaling relationship among intermediates. Herein, an isolated diatomic Ni-Mn dual-sites catalyst was anchored on nitrogenated carbon, which exhibits remarkable electrocatalytic performance towards CO reduction.
View Article and Find Full Text PDFTRAMP assembly alters the conformation and RNA binding of Mtr4 and Trf4-Air2.
Proc Natl Acad Sci U S A
January 2025
Department of Chemistry and Biochemistry, The University of Texas at Dallas, Richardson, TX 75080.
Article Synopsis
- The TRAMP complex is crucial for RNA processing and features two key enzymatic activities that involve both polyadenylation and unwinding of RNA.
- New research using hydrogen-deuterium exchange data reveals insights into how TRAMP assembles and shuffles RNA between its catalytic sites, which are not fully understood.
- Findings indicate that peripheral RNA-recognition motifs affect TRAMP assembly and that different active-site subunits interact with tRNA in ways that influence RNA transfer between TRAMP components.
Amorphous High-entropy Phosphide Nanosheets With Multi-atom Catalytic Sites for Efficient Oxygen Evolution.
Adv Mater
December 2024
School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450001, China.
Article Synopsis
- The alkaline oxygen evolution reaction (OER) involves four key reactions and poses challenges in balancing Gibbs free energies of intermediates like HO*, O*, and HOO* at active sites.
- A new high-entropy metal-organic framework using Fe, Ni, Co, Cu, and Y is developed via electrodeposition, resulting in the FeCoNiCuYP/C composite, which features an amorphous structure with several active sites.
- This composite shows enhanced OER performance in alkaline solutions, with a low overpotential of 316 mV at 100 mA/cm², attributed to the optimized electronic structure and binding strengths facilitated by Co/Ni and Fe atom interactions.
The Reaction Mechanism and Rates at Ru Single-Atom Catalysts for Hydrogenation of Biomass BHMF to Produce BHMTHF for Renewable Polymers.
J Am Chem Soc
November 2024
Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States.
Realizing high selectivity for producing biodegradable 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF) for renewable polymers from 5-hydroxymethylfurfural (HMF) biomass through ring hydrogenation on single-atom catalysts poses a considerable challenge due to the complexity of HMF functional groups and the difficulty of H dissociation. We developed a detailed reaction mechanism based on molecular dynamics (AIMD) and quantum mechanics (QM) to find that Ru single-atom catalysts can simultaneously dissociate H and perform the ring hydrogenation of biomass-derived 2,5-bis(hydroxymethyl)furan (BHMF) to produce biodegradable BHMTHF, with a free energy barrier of 0.82 eV.
View Article and Find Full Text PDFIndependent Control Over the H/OH Adsorption: Breaking the Trade-Off Between H/OH-Adsorption and HO-Dissociation of Platinum-Group Metal Electrocatalyst for Hydrogen Evolution Reaction.
Small
December 2024
School of Chemistry and Materials Science, Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Nanjing Normal University, Nanjing, 210023, China.
Platinum-group metals catalysts (such as Rh, Pd, Ir, Pt) have been the most efficient hydrogen evolution reaction (HER) electrocatalysts due to their moderate H adsorption strength, while the high HO-dissociation barrier in alkaline media restrains the catalytic performance of PGM catalysts. However, the optimization of the HO-dissociation barrier and *H/*OH binding energy toward their individual optima is limited due to the constraints of their scaling relationship on a single active site. Here, a coordinatively unsaturated "M─O─W" (M = Rh, Pd, Ir, Pt) active area is constructed, where H and OH species are anchored on Pt-group metal sites and inactive W sites for individual regulation.
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!