Carbon Letters最新文献

We successfully synthesized a porous carbon material with abundant hexagonal boron nitride (h-BN) dispersed on a carbon matrix (p-BN-C) as efficient electrocatalysts for two-electron oxygen reduction reaction (2e⁻ ORR) to produce hydrogen peroxide (H₂O₂). This catalyst was fabricated via ball-milling-assisted h-BN exfoliation and subsequent growth of carbon structure. In alkaline solutions, the h-BN/carbon heterostructure exhibited superior electrocatalytic activity for H₂O₂ generation measured by a rotating ring-disk electrode (RRDE), with a remarkable selectivity of up to 90–97% in the potential range of 0.3–0.6 V vs reversible hydrogen electrode (RHE), superior to most of the reported carbon-based electrocatalysts. Density functional theory (DFT) simulations indicated that the B atoms at the h-BN heterostructure interface were crucial active sites. These results underscore the remarkable catalytic activity of heterostructure and provide a novel approach for tailoring carbon-based catalysts, enhancing the selectivity and activity in the production of H₂O₂ through heterostructure engineering.

Flexible electrodes, particularly paper electrodes modified with polypyrrole, have shown promise in energy-related applications. We have earlier demonstrated the usage of paper electrodes modified with polypyrrole as a flexible and suitable photoanode for photoelectrochemical water splitting (PEC). Further, modification of this electrode system with an appropriate tandem absorber system for solar fuel production is interesting in developing efficient photoanodes. In this study, we study the PEC performance of flexible polypyrrole-based paper photoanodes (PPy-PAs) by decorating them with rGO@Cu₂ZnSnS₄ chalcopyrites (rGO@CZTS/PPy-PAs). The lower bandgap (~ 1.5 eV) of the rGO@CZTS/PPy-PAs system allows for efficient visible light absorption, substantially improving PEC water-splitting reactions. The rGO@CZTS/PPy-PAs exhibited an enhanced current density of ~ 13.2 mA/cm² at 1.23 V vs RHE, ABPE of ~ 1.5%, and a hydrogen evolution rate of 177 μmoles/min/cm². Overall, rGO@CZTS/PPy-PAs showed 2.1-fold, 1.1-fold, and 1.4-fold enhancement in photocurrent activity over PPy-PAs, CZTS/PPy-PAs, and rGO/PPy-PAs, respectively. The usability of rGO@CZTS/PPy-PAs is established in the form of stable photocurrent for more than 200 min. These findings open new possibilities for developing modified PPy PAs as flexible PEs for efficient solar-driven PEC devices and give directions on improving flexible PEs for flexible and efficient solar-driven PEC systems.

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In this paper, the formation and characterization of Pt₂, Pt₃ as well as Pt₄ atomic clusters in cup-stacked carbon nanotubes (CSCNTs) are evaluated by DFT to examine the adsorption capacity under the clusters. The results show that the Pt clusters move toward the bottom edge or form rings in the optimized stable structure. Pt far from the carbon substrate possesses more active electrons and adsorption advantages. The three clusters can adsorb up to 17, 18, and 16 hydrogen molecules. Loading metal clusters at the bottom edge maintains a relatively good adsorption property despite the low binding energy through comparative studies. The adsorption capacity does not increase with the number of Pt for metal aggregation reducing the hydrogen adsorption area thus impacting the hydrogen storage ability and the aggregation phenomenon limiting the action of Pt metal. During adsorption, chemisorption occurs only in the Pt₂ cluster, while multiple hydrogen molecules achieve physiochemical adsorption in the Pt₃ and Pt₄ clusters. Compared with the atomic loading of the dispersion system in equal quantities, the dispersion system features higher molecular stability and can significantly reduce the energy of the carbon substrates, providing more sites for hydrogen adsorption in space.

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The electrochemical properties of a CF_X cathode were improved by defluorination of the surface with a N₂ plasma and using a silica wafer. Compared to the N₂ plasma treatment alone, when the CF_X and silica were reacted together, the C-F bonds were modified and the surface was etched efficiently, so defluorination was enhanced. An electrochemical analysis confirmed that Half-cells prepared by treating CFx and silica with nitrogen plasma exhibited a capacity of about 400 mAh/g at 5C. In addition, it was confirmed that the loss of charge transfer was reduced by up to 71% compared to that for pristine CF_X. As shown by a GITT analysis, when the CFx and silica were treated with N₂ plasma together, the ion conductivity gradually increased due to a decrease in the ion diffusion barriers and the formation of a carbon layer. Therefore, this is a simple and effective way to improve the conductivities of CF_X cathode materials with the energy of a N₂ plasma and the silica-fluorine reaction.

Because plastics are cheap and light, their use is indispensable in our daily lives. However, the extensive use of plastics causes the disposal issue. Among various disposal processes, plastic recycling is of great attention because of minimizing waste and harmful byproducts. Herein, we recycle the most popular thermoplastic materials, high-density and low-density polyethylene, producing the anode materials for the Li-ion batteries. The electrochemical properties of the as-recycled soft carbon are investigated to study the energy storage capability as the anode of Li-ion batteries. Our work demonstrates the soft carbon recycled from plastic wastes is a promising anode material.

The most significant threat to the ecosystem is emerging pollutants, which are becoming worse each year and harming the planet severely and permanently. Many organic and inorganic contaminants are present and persistent due to various world events and population growth. As a result, there is a greater need for new technology and its application to address the problems caused by developing pollutants. Carbon composite nanomaterials have significant potential in the fight against numerous environmental contaminants due to their distinctive attributes. This review discusses the reports of customized carbon composite nanomaterials to meet the need for specific elimination of emerging contaminants. Physical and chemical features such as high surface area, conductivity (thermal and electrical), and vibroelectronic properties, size, shape, porosity, and composite nature are making these tailored materials of carbon-based nanomaterials an emerging and sustainable tool to remove persistent compounds like emerging contaminants in aqueous solution. Different composite materials are well discussed in this review, along with their adsorption efficiency of diverse emerging contaminants, including Bisphenol A, estradiol, metformin, etc. This review provides insight into the recent trends limited to 2017–2023. The limitations of carbon-based nanomaterials, such as regeneration and cost-effectiveness, have also been overcome in recent years by diverse modifications in the production process, which can be further improved to make these materials well suited for an extended group of emerging contaminants.

The thermal conductivity (TC) of graphene-based/metal composites is currently not satisfactory because of the existence of large interfacial thermal resistance between graphene and metal originating from the strong scattering of phonons. In this work, 6063Al-alloy-based reduced graphene oxide (rGO) composite with strong covalent bonds interface was prepared via self-assembly, reduction, and electrophoresis-deposition processes by using 3-aminopropyl triethoxysilane (APTS) as a link agent. Structural characterizations confirmed the successful construction of strong Al-O-Si-O-C covalent bonds in the as-prepared 6063Al-Ag-APTS-rGO composite, which can promote the transfer of phonons in the interface. Benefiting from the unique structure, 6063Al-Ag-APTS-rGO (214.1 W/mK) showed obviously higher cross-plane TC than 6063Al (195.6 W/mK). Comparative experiments showed that 6063Al-Ag-APTS-rGO has better cross-plane TC than 6063Al/Ag/APTS/rGO (196.6 W/mK) prepared via physical mixing of stirring process, evidencing the significance of electrophoresis-deposition (EPD) process on constructing strong covalent bonds for improving the heat dissipation performance. Besides, the effects of different rGO contents and test temperature on the TC of the composites and their corrosion resistance were also discussed. This work demonstrated a feasible strategy for the construction of metal–carbon interface composite with improved thermal performance.

Graphene-based materials modified with transition metals, and their potential utilization as hydrogen storage devices, are extensively studied in the last decades. Despite this widespread interest, a comprehensive understanding of the intricate interplay between graphene-based transition metal systems and H₂ molecules remains incomplete. Beyond fundamental H₂ adsorption, the activation of H₂ molecule, crucial for catalytic reactions and hydrogenation processes, may occur on the transition metal center. In this study, binding modes of H₂ molecules on the circumcoronene (CC) decorated with Cr or Fe atoms are investigated using the DFT methods. Side-on (η²-dihydrogen bond), end-on and dissociation modes of H₂ binding are explored for high (HS) and low (LS) spin states. Spin state energetics, reaction energies, QTAIM and DOS analysis are considered. Our findings revealed that CC decorated with Cr (CC-Cr) emerges as a promising material for H₂ storage, with the capacity to store up to three H₂ molecules on a single Cr atom. End-on interaction in HS is preferred for the first two H₂ molecules bound to CC-Cr, while the side-on LS is favored for three H₂ molecules. In contrast, CC decorated with Fe (CC-Fe) demonstrates the capability to activate H₂ through H–H bond cleavage, a process unaffected by the presence of other H₂ molecules in the vicinity of the Fe atom, exclusively favoring the HS state. In summary, our study sheds light on the intriguing binding and activation properties of H₂ molecules on graphene-based transition metal systems, offering valuable insights into their potential applications in hydrogen storage and catalysis.

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This paper explores the potential application of carbon nanotubes (CNTs) in the construction industry, as CNTs can effectively serve as nano-fillers, bridging the voids and holes in cement structures. However, the limited dispersibility of CNTs in water necessitates the use of dispersing agents for achieving uniform dispersion. In this study, two kinds of cement superplasticizers, polycarboxylate ether (PCE) and sulfonated naphthalene formaldehyde (SNF) were employed as dispersing agents to improve the interfacial affinity between CNTs and cement, and to enhance the strength of the cement nanocomposites. Contact angle experiments revealed that the utilization of PCE and SNF effectively addressed the interface issues between CNTs and cement. As a result, the cement nanocomposite with a CNT to PCE ratio of 1:2 exhibited an approximately 6.6% increase in compressive strength (73.05 MPa), while the CNT:SNF 1:2 cement composite showed a 4.7% increase (71.72 MPa) compared to plain cement (68.52 MPa). In addition, the rate of crack generation in cement nanocomposites with CNTs and dispersing agents was found to be slower than that of plain cement. The resulting cement nanocomposites, characterized by enhanced strength and durability, can be utilized as safer materials in the construction industry.

Pyrolysis of methane is a carbon-economic method to obtain valuable carbon materials and CO_x-free H₂, under the carbon peaking and carbon neutrality goals. In this work, we propose a methane pyrolysis process to produce graphite and H₂ using bubble column reactor containing NiO/Al₂O₃ and NaCl–KCl (molten salt). The process was optimized by the different amounts of NaCl–KCl, the CH₄/Ar ratio and temperature, indicating that the CH₄ conversation rate could reach 92% at 900 °C. Meanwhile, we found that the addition of molten salt could obtain pure carbon materials, even if the conversation rate of CH₄ decreases. The analysis of the carbon products revealed that graphite could be obtained.