We propose a unique experimental technique in which isotopically labeled ethanol, e.g., 12CH3-13CH2-OH, is used to trace the carbon atoms during the formation of single-walled carbon nanotubes (SWNTs) by chemical vapor deposition (CVD). The proportion of 13C is determined from Raman spectra of the obtained SWNTs, yielding the respective contribution of ethanol's two different carbon atoms to SWNT formation. Surprisingly, the carbon away from the hydroxyl group is preferably incorporated into the SWNT structure, and this preference is significantly affected by growth temperature, presence of secondary catalyst metal species such as Mo, and even by the substrate material. These experiments provide solid evidence confirming that the active carbon source is not limited to products of gas-phase decomposition such as ethylene and acetylene, but ethanol itself is arriving at and reacting with the metal catalyst particles. Furthermore, even the substrate or other catalytically inactive species directly influences the formation of SWNTs, possibly by changing the local environment around the catalyst or even the reaction pathway of SWNT formation. These unexpected effects, which are inaccessible by conventional techniques, paint a clearer picture regarding the decomposition and bond breaking process of the ethanol precursor during the entire CVD process and how this might influence the quality of the obtained SWNTs.
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http://dx.doi.org/10.1021/nn305180g | DOI Listing |
J Am Chem Soc
January 2025
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, Kowloon 999077, China.
Heterogeneous ice nucleation is a widespread phenomenon in nature. Despite extensive research on ice nucleation near biological antifreeze proteins, a probe for ice nucleation and growth processes at the atomic level is still lacking. Herein, we present simulation evidence of the heterogeneous ice nucleation process on the ice-binding surface (IBS) of the antifreeze protein (TmAFP).
View Article and Find Full Text PDFSmall
January 2025
College of Materials Science and Engineering, Sichuan University, Chengdu, 610065, China.
The transition metal single atoms (SAs)-based catalysts with M-N coordination environment have shown excellent performance in electrocatalytic reduction of CO, and they have received extensive attention in recent years. However, the presence of SAs makes it very difficult to efficiently improve the coordination environment. In this paper, a method of direct high-temperature pyrolysis carbonization of ZIF-8 adsorbed with Ni and Fe ions is reported for the synthesis of Ni SAs and FeN nanoparticles (NPs) supported by the N-doped carbon (NC) hollow nanododecahedras (HNDs) with nanotubes (NTs) on the surface (Ni SAs/FeN NPs@NC-HNDs-NTs).
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January 2025
College of Ecology and Environment, Co-Innovation Center for the Sustainable Forestry in Southern China, Nanjing Forestry University, Nanjing, 210037, P. R. China.
Constructing heterojunctions between phase interfaces represents a crucial strategy for achieving excellent photocatalytic performance, but the absence of sufficient interface driving force and limited charge transfer pathway leads to unsatisfactory charge separation processes. Herein, a doping-engineering strategy is introduced to construct a In─N bond-bridged InS nanocluster modified S doped carbon nitride (CN) nanosheets Z-Scheme van der Waals (VDW) heterojunctions (InS/CNS) photocatalyst, and the preparation process just by one-step pyrolysis using the pre-coordination confinement method. Specifically, S atoms doping enhances the bond strength of In─N and forms high-quality interfacial In─N linkage which serves as the atomic-level interfacial "highway" for improving the interfacial electrons migration, decreasing the charge recombination probability.
View Article and Find Full Text PDFAdv Mater
January 2025
Department of Mechanical & Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, M5S 3G8, Canada.
Nanoarchitected materials are at the frontier of metamaterial design and have set the benchmark for mechanical performance in several contemporary applications. However, traditional nanoarchitected designs with conventional topologies exhibit poor stress distributions and induce premature nodal failure. Here, using multi-objective Bayesian optimization and two-photon polymerization, optimized carbon nanolattices with an exceptional specific strength of 2.
View Article and Find Full Text PDFChem Sci
January 2025
Interdisciplinary Research Center for Sustainable Energy Science and Engineering (IRC4SE2), School of Chemical Engineering, Zhengzhou University Henan 450001 China
The exceptional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performances of core-shell catalysts are well documented, yet their activity and durability origins have been interpreted only based on the static structures. Herein we employ a NiFe alloy coated with a nitrogen-doped graphene-based carbon shell (NiFe@NC) as a model system to elucidate the active structure and stability mechanism for the ORR and OER by combining constant potential computations, molecular dynamic simulations, and experiments. The results reveal that the synergistic effects between the alloy core and carbon shell facilitate the formation of Fe-N-C active sites and replenish metal sites when central metal atoms detach.
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