Carbon Letters最新文献

Complex structure constituting of several layers of heteroatom-doped N-CDs are used as a main sensing film along with aluminum electrodes in conductometric gas sensing system for sensitive and selective monitoring of CO₂ and CO gases diluted with normal air, which are extensively prevalent in the atmosphere primarily due to the industrial revolution, locomotives, and numerous natural phenomena’s and the limit of detection (LOD) turned out to be 400 ppm and 30 ppm, respectively, with 20% relative humidity at 30 °C and pressure 1 (atm) which are good for healthy air quality checks. The sensor performance was satisfactory and bidirectional at ambient room temperature (30 °C) and pressure (1 atm) conditions but the relative humidity (50%) at 30 °C had a detrimental impact on the sensing responses, therefore intermittent heating at 80 °C for several minutes between the sensing responses was provided to the sensing chip or one should use gas filter membranes to block humidity, thereby maintaining its constant performance with great ease and accuracy. The cyclic voltammetry revealed well-defined oxidation and reduction peaks, with excellent stability and reversibility. In a nutshell, heteroatom-doped N-CDs’ nanocomposite material can revolutionize in a better environmental pollution monitoring by sensing gases in an extensively lesser response and recovery times.

Graphical Abstract

This study delves into the potential application of whisker carbon nanotube (w-CNT) in terms of electrical heating performance, with a particular emphasis on its significance in high-efficiency electrothermal conversion applications. Meanwhile, a comparative study was conducted on traditional carbon nanotubes (T1 and T3) with different aspect ratios. A uniform and dense carbon nanotube paper (BP) was prepared using a vacuum filtration method, including single-layer (T1, T3 and w-CNT BP), double-layer gradient composite (T1/T3-g, w-CNT/T3-g), and mixed composite (T1/T3-m and w-CNT/T3-m). The thickness of each type of BP is approximately 100 µm. The results demonstrated that electrical conductivity and electrical heating performance of single-layer BPs follow the order of T1 > T3 > w-CNT. While, mixed composite BPs are superior to double-layer gradient composite BPs in electrical conductivity and thermal performance. Notably, w-CNT/T3-m BP exhibits excellent electrothermal performance. Under an applied voltage of 5 V, the surface temperature of w-CNT/T3-m BP reaches 190 ℃. When the voltage is increased to 6 V, the surface temperature rises by 150℃ within 10 s, reaching a steady-state temperature of 318 ℃. This excellent electrothermal performance can be attributed to the introduction of w-CNT, which has a perfect and defect free structure according to Raman analysis. In-depth analysis using X-ray diffraction (XRD) indicated a more complete and higher degree of crystallinity in the w-CNT structure. In summary, this study not only provides experimental and theoretical basis for the application of high-performance electrothermal materials based on carbon nanotubes, but also foreshadows their broad application prospects in the field of macroscopic materials.

Crystalline heptazine carbon nitride (HCN) is an ideal photocatalyst for photocatalytic ammonia synthesis. However, the limited response to visible light has hindered its further development. As a noble metal, Au nanoparticles (NPs) can enhance the light absorption capability of photocatalysts by the surface plasmon resonance (SPR) effect. Therefore, a series of Au NPs-loaded crystalline carbon nitride materials (AH) were prepared for photocatalytic nitrogen fixation. The results showed that the AH displayed significantly improved light absorption and decreased recombination rate of photo-generated carriers owing to the introduction of Au NPs. The optimal 2AH (loaded with 2 wt% Au) sample demonstrated the best photocatalytic performance for ammonia production with a yield of 70.3 μmol g⁻¹ h⁻¹, which outperformed that of HCN. This can be attributed to the SPR effect of Au NPs and alkali metal of HCN structure. These findings provide a theoretical basis for studying noble metal-enhanced photocatalytic activity for nitrogen fixation and offer new insights into advances in efficient photocatalysts.

In recent years, the search on fabrication of highly efficient, stable, and cost-effective alternative to Pt for the hydrogen evolution reaction (HER) has led to the development of new catalysts. In this study, we investigated the electrocatalytic HER activity of the Toray carbon substrate by creating defect sites in its graphitic layer through ultrasonication and anodization process. A series of Toray carbon substrates with active sites are prepared by modifying its surface through ultrasonication, anodization, and ultrasonication followed by anodization procedures at different time periods. The anodization process significantly enhances the surface wettability, consequently resulting in a substantial increase in proton flux at the reaction sites. As an implication, the overpotential for HER is notably reduced for the Toray carbon (TC-3U-10A), subjected to 3 min of ultrasonification followed by 10 min of anodization, which exhibits a significantly lower Tafel slope value of 60 mV/dec. Furthermore, the reactivity of the anodized surface for HER is significantly elevated, especially at higher concentrations of sulfuric acid, owing to the enhanced wettability of the substrate. The lowest Tafel slope value recorded in this study stands at 60 mV/dec underscoring the substantial improvements achieved in catalytic efficiency of the defect-rich carbon materials. These findings hold promise for the advancement of electrocatalytic applications of carbon materials and may have significant implications for various technological and industrial processes.

Coal tar pitch is a raw material that can be made from various carbon materials such as activated carbon, carbon fiber, and artificial graphite through heat treatment. In particular, it is an important raw material used as a binder and impregnated pitch when manufacturing carbon composite materials. In order to improve the physical properties of such a carbon composite material, the content of β-resin is an important factor. Although β-resin plays the role of a binder, it also corresponds to fixed carbon, so it can determine the physical properties after carbonization. In this study, we compared the physical properties of coal tar pitch various temperature ramping rate, and found through Py-GC/MS analysis that intermediate materials were generated by heteroatoms such as oxygen and nitrogen. MALDI-TOF/MS analysis revealed that these intermediate materials overlapped with the molecular weight region of β-resin. Therefore, the content of β-resin is in the following order: 430–5 (12.8 wt%), 430–10 (10.2 wt%), and 430–2 (6.3 wt%), and when 430–5 is used as a binder, the highest density appeared at 1.75 g/cm³. However, such intermediate materials undergo thermal decomposition even at temperatures above 900 °C. As a result, after carbonization, 430–5 had a density of 1.60 g/cm³, which was similar or lower than that of 430–2 (1.72 → 1.63 g/cm³) and 430–10 (1.73 → 1.61 g/cm³). From these results, it is expected that if the heteroatom content is distributed in an appropriate amount and the heating rate is well controlled, it will be possible to maintain a high density even after carbonization while ensuring a high beta-resin content.

In this study, ester co-solvents and fluoroethylene carbonate (FEC) were used as low-temperature electrolyte additives to improve the formation of the solid electrolyte interface (SEI) on graphite anodes in lithium-ion batteries (LIBs). Four ester co-solvents, namely methyl acetate (MA), ethyl acetate, methyl propionate, and ethyl propionate, were mixed with 1.0 M LiPF₆ ethylene carbonate:diethyl carbonate:dimethyl carbonate (1:1:1 by vol%) as the base electrolyte (BE). Different concentrations were used to compare the electrochemical performance of the LiCoO₂/graphite full cells. Among various ester co-solvents, the cell employing BE mixed with 30 vol% MA (BE/MA30) achieved the highest discharge capacity at − 20 °C. In contrast, mixing esters with low-molecular-weight degraded the cell performance owing to the unstable SEI formation on the graphite anodes. Therefore, FEC was added to BE/MA30 (BE/MA30-FEC5) to form a stable SEI layer on the graphite anode surface. The LiCoO₂/graphite cell using BE/MA30-FEC5 exhibited an excellent capacity of 127.3 mAh g⁻¹ at − 20 °C with a capacity retention of 80.6% after 100 cycles owing to the synergistic effect of MA and formation of a stable and uniform inorganic SEI layer by FEC decomposition reaction. The low-temperature electrolyte designed in this study may provide new guidelines for resolving low-temperature issues related to LIBs, graphite anodes, and SEI layers.

Graphical abstract

Graphitic nitrogen-doped carbon film/nanoparticle composite, in which the films were wrapped and separated by the nanoparticles, was prepared through a simple co-calcination route. Due to its unique porous structure and improved nitrogen content, the as-prepared electrode material could exhibit high specific capacitances of 317.5 F g⁻¹ at 0.5 A g⁻¹ and 200.0 F g⁻¹ at 20 A g⁻¹, and stable cycling behavior with no capacitance decline after 10,000 cycles in three-electrode system. When assembled in two-electrode capacitor, its specific capacitance could be well kept at 265.5 F g⁻¹ at 0.5 A g⁻¹, and thus the supercapacitor with a high energy density of 9.22 Wh kg⁻¹ was obtained. The superior energy storage properties of the as-prepared material indicate its promising application as high-performance carbon-based electrode for supercapacitors.

Silicon carbide (β-SiC) was synthesized through an improved sol–gel method, then Ni/SiC catalysts were prepared using a hydrothermal method. The catalysts were characterized using TEM, H₂-TPR, CO₂-TPD and N₂-TPD, etc. The results showed that the synthesized β-SiC had a large specific surface area, promoting the dispersion of Ni species and thus exposing more active sites. The interaction between Ni species and β-SiC contributed significantly to catalytic performance. Furthermore, the strong alkalinity of catalyst could adjust the bond energy of the active metal and N (M–N), which were conducive to desorption of the recombinant N₂ from the metal surface, promoting to ammonia decomposition. Among the Ni/SiC catalysts, 30Ni/SiC-700 synthesized with the Ni loading of 30 wt% and calcination temperature of 700 °C, exhibited the optimal ammonia conversion rate of 93.4% at 600 °C under the space speed of 30,000 mL∙g_cat⁻¹∙h⁻¹, and demonstrated a long-term stability, suggesting a very promising catalyst in ammonia decomposition.

With the development of photocatalytic hydrogen production technology, the effective transport of photogenerated carrier electrons is still one of the main factors affecting the performance of photocatalytic hydrogen evolution. In this work, graphdiyne was prepared by ball milling method. The CoMo-MOF with polyhedral structure was introduced into graphdiyne to construct S-scheme heterojunction to promote the efficient transfer of photogenerated carriers and enhanced hydrogen evolution activity. Graphdiyne is a new carbon material with adjustable band gap, which is synthesized from the hybrid of sp and sp², and has excellent electrical conductivity. CoMo-MOF is a polyhedral structure that can provide more active sites and promote photocatalytic hydrogen evolution. The weak point of poor conductivity in CoMo-MOF has been successfully improved by combining CoMo-MOF with graphdiyne, and the migration rate of photogenerated carriers has been accelerated. The hydrogen evolution property of graphdiyne/CoMo-MOF is 300 μmol, which is 19.61 times that of graphdiyne and 9.03 times that of CoMo-MOF. Therefore, the construction of S-scheme heterojunction provides a transport channel for electron transfer and improves the efficiency of photogenerated carrier separation. This work provides a new train of thought of design to introduce MOFs materials into carbon materials for photocatalytic hydrogen evolution.

Artificial photosynthesis harnesses clean and sustainable solar power to catalyze the conversion of CO₂ and H₂O molecules into valuable chemicals and O₂. This sustainable approach combines energy conversion with environmental pollution control. Non-oxide photocatalysts with broad visible-light absorption and suitable band structures, hold immense potential for CO₂ conversion. Nevertheless, they still face numerous challenges in practical applications, particularly in CO₂ conversion with H₂O. Surface modification and functionalization play the significant role in improving the activity of non-oxide photocatalysts. Multifarious strategies, such as cocatalyst loading, surface regulation, doping engineering, and heterostructure construction, have been explored to optimize light harvesting, bandgap driving force, electron–hole pairs separation/transfer, CO₂ adsorption, activation, and catalysis processes. This review summarizes recent progress in surface modification strategies for non-oxide photocatalysts and discusses their enhancement mechanisms for efficient CO₂ conversion. These insights are expected to guide the design of high-performance non-oxide photocatalyst systems.

Graphical Abstract

Surface modification of non-oxide photocatalysts having broad visible-light absorption holds immense potential for CO₂ reduction with H₂O towards clean energy conversion.