Vacancies in graphene present sites of altered chemical reactivity and open possibilities to tune graphene properties by defect engineering. The understanding of chemical reactivity of such defects is essential for successful implementation of carbon materials in advanced technologies. We report the results of a systematic DFT study of atomic adsorption on graphene with a single vacancy for the elements of rows 1-6 of the periodic table of elements (PTE), excluding lanthanides. The calculations have been performed using the PBE, long-range dispersion interaction-corrected PBE (PBE+D2 and PBE+D3) and non-local vdW-DF2 functionals. We find that most elements strongly bind to the vacancy, except for the elements of groups 11 and 12, and noble gases, for which the contribution of dispersion interaction to bonding is most significant. The strength of the interaction with the vacancy correlates with the cohesive energy of the elements in their stable phases: the higher the cohesive energy is, the stronger bonding to the vacancy can be expected. As most atoms can be trapped at the SV site we have calculated the potentials of dissolution and found that in most cases the metals adsorbed at the vacancy are more "noble" than they are in their corresponding stable phases.
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Ecotoxicol Environ Saf
January 2025
School of Eco-Environment, Hebei Key Laboratory of Close-to-Nature Restoration Technology of Wetlands, Hebei University, Baoding 071002, China. Electronic address:
Imidacloprid (IMI), as an emerging pollutant, is frequently detected in pesticide wastewater. Cobalt-based single-atom catalysts (Co-SACs) doped with sulfur atoms can serve as an efficient strategy to activate peroxymonosulfate (PMS) and degrade organic pollutants. The paper employed density functional theory and computational toxicology to deeply explore the mechanism and ecotoxicity of IMI when S atoms were introduced into Co-SACs for PMS activation.
View Article and Find Full Text PDFJ Control Release
January 2025
Dipartimento di Scienza dei Materiali, Università degli Studi di Milano-Bicocca, via R. Cozzi 55, 20125 Milano, Italy; BioNanoMedicine Center NANOMIB, Università degli Studi di Milano-Bicocca, Italy. Electronic address:
Graphene oxide (GO) is an amphiphilic and versatile graphene-based nanomaterial that is extremely promising for targeted drug delivery, which aims to administer drugs in a spatially and temporally controlled manner. A typical GO nanocarrier features a polyethylene glycol coating and conjugation to an active targeting ligand. However, it is challenging to accurately model GO dots, because of their intrinsically complex and not unique structure.
View Article and Find Full Text PDFEnviron Res
January 2025
Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China; CAS Key Laboratory of Renewable Energy, Guangzhou 510640, China; Guangdong Provincial Key Laboratory of High-Quality Recycling of End-of-Life New Energy Devices, Guangzhou 510640, China. Electronic address:
Hydrogen sulfide (HS) is a major air pollutant posing a serious threat to both the environment and public health. In this study, a novel nitrogen-rich biocarbon that effectively removes HS was produced from a mixture of sewage sludge and pine sawdust using melamine as nitrogen source. Compared with pristine biocarbons, nitrogen (N)-doped biocarbons possessed an adjustable porosity, e.
View Article and Find Full Text PDFACS Nano
January 2025
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore.
Transition-metal dichalcogenides (TMDs), such as molybdenum disulfide (MoS), have emerged as a generation of nonprecious catalysts for the hydrogen evolution reaction (HER), largely due to their theoretical hydrogen adsorption energy close to that of platinum. However, efforts to activate the basal planes of TMDs have primarily centered around strategies such as introducing numerous atomic vacancies, creating vacancy-heteroatom complexes, or applying significant strain, especially for acidic media. These approaches, while potentially effective, present substantial challenges in practical large-scale deployment.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
State Key Laboratory of Fine Chemicals, Research and Development Center of Membrane Science and Technology, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
The electrocatalytic nitrogen reduction reaction (eNRR) is an attractive strategy for the green and distributed production of ammonia (NH); however, it suffers from weak N adsorption and a high energy barrier of hydrogenation. Atomically dispersed metal dual-site catalysts with an optimized electronic structure and exceptional catalytic activity are expected to be competent for knotty hydrogenation reactions including the eNRR. Inspired by the bimetallic FeMo cofactor in biological nitrogenase, herein, an atomically dispersed FeMo dual site anchored in nitrogen-doped carbon is proposed to induce a favorable electronic structure and binding energy.
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