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Surface quality plays an important role in the performance of SRF cavities. We report the topographic evolution of H degassed, N and O doped Nb surfaces subjected to electropolishing using atomic force microscopy. N doped Nb shows a substantial increase in roughness due to formation of niobium nitrides into the surface. Implications of the topography on magnetic field enhancement and vortex entry are discussed.
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Presentation for NMSU Postdoctoral Symposium, Sept 20th, based on ExEx work
Carbon-based nanocomposites have been attracting extensive attention as high-performance catalysts in alkaline media towards the electrochemical reduction of oxygen. Herein, polyacrylonitrile nanoflowers are synthesized via a free-radical polymerization route and used as a structural scaffold and precursor, whereby controlled pyrolysis leads to the ready preparation of carbon nanocomposites (FeNi-NCF) doped with both metal (Fe and Ni) and nonmetal (N) elements. Transmission electron microscopy studies show that the FeNi-NCF composites retain the flower-like morphology, with the metal species atomically dispersed into the flaky carbon petals. Remarkably, despite a similar structure, elemental composition, and total metal content, the FeNi-NCF sample with a high Fe:Ni ratio exhibits an electrocatalytic performance towards oxygen reduction reaction (ORR) in alkaline media that is similar to that by commercial Pt/C, likely due to the Ni to Fe electron transfer that promotes the adsorption and eventual reduction of oxygen, as evidenced in X-ray photoelectron spectroscopic measurements. Results from this study underline the importance of the electronic properties of metal dopants in the manipulation of the ORR activity of carbon nanocomposites.
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We investigated the performance limitations of superconducting radio-frequency (SRF) cavities and materials using multiple experimental techniques. In particular, this study focuses on understanding the surface properties of nitrogen-doped Nb cavities and super?conducting thin films with higher Tc such as Nb3Sn. The main goal of this work is to use different techniques to better understand each aspect of the complex loss mechanism in superconductors to further improve the already highly efficient SRF cavities. Nitrogen doping applied to a Nb SRF cavity significantly improves the quality factor Q0 compared to a conventional Nb cavity, at an expense of reduced maximum accelerating gradient. The early quench mechanism was analyzed by using temperature maps before and during the quenching. The temperature maps revealed insignificant heating before the quench, and we concluded that nitrogen doping reduces critical magnetic fields in local regions, leading to premature quenching. To understand the origin of the increasing Q0 with the rf field, the density of states (DOS) of cold spots from nitrogen-doped and standard cavities were measured and analyzed using scanning tunneling microscopy. The results suggested that nitrogen doping reduces the spatial inhomogeneity of superconducting properties and shrinks the metallic suboxide layers, which tunes the DOS in such a way as to produce the field-induced reduction in the surface resistance. To characterize SRF thin films, an experimental setup for measuring a coplanar waveguide (CPW) resonator was developed and tested. A surface impedance measurement of the Nb film showed good agreement with the BCS calculation. The preliminary results from measurements of Nb3Sn and NbTiN films are also presented here. The nonlinear Meissner effect was investigated in Nb3Sn film CPW resonators by mea?suring the resonant frequency as a function of a parallel magnetic field. Contrary to a conventional quadratic dependence of the penetration depth ?(B) on the applied magnetic field B, as expected in s-wave superconductors, nearly a linear increase of ?(B) with B was observed. It was concluded that this behavior of ?(B) is due to weakly linked grain bound?aries on the polycrystalline Nb3Sn films, which can mimic the NLME expected in a clean d-wave superconductor.
Nitrogen doped carbon nanoparticles on highly porous carbon nanofiber electrodes were successfully synthesized via combining centrifugal spinning, chemical polymerization of pyrrole and a two-step heat treatment. Nanoparticle-on-nanofiber morphology with highly porous carbon nanotube like channels were observed from SEM and TEM images. Nitrogen doped carbon nanoparticles on highly porous carbon nanofiber (N-PCNF) electrodes exhibited excellent cycling and C-rate performance with a high reversible capacity of around 280 mA h g -1 in sodium ion batteries. Moreover, at 1000 mA g -1 , a high reversible capacity of 172 mA h g -1 was observed after 300 cycles. The superior electrochemical properties were attributed to a highly porous structure with enlarged d-spacings, enriched defects and active sites due to nitrogen doping. The electrochemical results prove that N-PCNF electrodes are promising electrode materials for high performance sodium ion batteries.
Nitrogen core-doping of graphene nanoribbons (GNRs) allows trigonal planar carbon atoms along the backbone of GNRs to be substituted by higher-valency nitrogen atoms. The excess valence electrons are injected into the π-orbital system of the GNR, thereby changing not only its electronic occupation but also its topological properties. We have observed this topological change by synthesizing dilute nitrogen core-doped armchair GNRs with a width of five atoms (N 2 -5-AGNRs). The incorporation of pairs of trigonal planar nitrogen atoms results in the emergence of topological boundary states at the interface between doped and undoped segments of the GNR. These topological boundary states are offset in energy by approximately ΔE = 300 meV relative to the topological end states at the termini of finite 5-AGNRs. Scanning tunneling microscopy (STM) and spectroscopy (STS) reveal that for finite GNRs the two types of topological states can interact through a linear combination of orbitals, resulting in a pair of asymmetric hybridized states. This behavior is captured by an effective Hamiltonian of nondegenerate diatomic molecules, where the analogous interatomic hybridization interaction strength is tuned by the distance between GNR topological modes.
The widespread use of fuel cell technology is hampered by the use of expensive and scarce platinum metal in electrodes which is required to facilitate the sluggish oxygen reduction reaction (ORR). In this work, a viable synthetic approach was developed to prepare iron-based sulfur and nitrogen dual doped porous carbon (Fe@SNDC) for use in ORR. Benzimidazole, a commercially available monomer, was used as a precursor for N doped carbon and calcined with potassium thiocyanate at different temperatures to tune the pore size, nitrogen content and different types of nitrogen functionality such as pyridinic, pyrrolic and graphitic. The Fe@SNDC–950 with high surface area, optimum N content of about 5 at% and high amount of pyridinic and graphitic N displayed an onset potential and half-wave potential of 0.98 and 0.83 V vs RHE, respectively, in 0.1 M KOH solution. The catalyst also exhibits similar oxygen reduction reaction performance compared to Pt/C (20 wt%) in acidic media. Furthermore, when compared to commercially available Pt/C (20 wt%), Fe@SNDC–950 showed enhanced durability over 6 h and poison tolerance in case of methanol crossover with the concentration up to 3.0 M in oxygen saturated alkaline electrolyte. Finally, our study demonstrates that the presence of N and S along with Fe-N moieties synergistically served as ORR active sites while the high surface area with accessible pores allowed for efficient mass transfer and interaction of oxygen molecules to the active sites contributing to the ORR activity of the catalyst.
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We used a combination of x-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) to investigate how the presence of a ruthenium (Ru) metal substrate modifies the N-D bond strength of the pyridinic nitrogen species in nitrogen (N)-doped graphene (Gr) on Ru(0001) compared to metal-free highly-oriented pyrolytic graphite (HOPG) substrate. The N-dopants were introduced through low-energy N+/N2+ irradiation. N is embedded in the carbon materials in two predominant configurations: as graphitic N (GN: N substituted in the hexagonal C lattice) and pyridinic N (PN: substitutional N adjacent to a C vacancy). XPS data showed that upon atomic deuterium (D) exposure at 220 K, the PN peak shifted to a higher binding energy by +1.2 eV for HOPG and +1.0 eV for N-doped graphene on Ru(0001), while the GN peak remained unchanged, indicating that the D atoms bound solely to pyridinic N. 85% of PN sites on HOPG can be saturated with D atoms, whereas only ~30% of pyridinic N sites are able to bind D atoms in N-doped Gr/Ru(0001). Our DFT analysis shows that this difference is due to the coordination of PN to Ru atoms, which necessitates bond cleavage of the N-Ru interaction prior to D atom adsorption. D begins desorbing from N-HOPG at ~573 K and is fully desorbed by ~973 K, whereas desorption from N-doped graphene on Ru(0001) begins at ~290 K, with complete desorption observed at ~700 K, indicating that the Ru metal weakens the N-D bond strength. We also studied a high-surface-area, layered, and porous N-doped carbon material, internally labeled NC900, which was synthesized by pyrolysis of glucose and graphitic carbon nitride (g-C3N4) at 1173 K. D exposure caused a +1.1 eV PN peak shift in NC900, with no change in the GN peak. Moreover, the NC900 exhibited the same desorption behavior as HOPG, demonstrating that well-defined model systems can effectively capture the behavior of more complex N-doped carbon materials.
Abstract Single‐atom catalysts (SACs) have attracted much attentions due to the advantages of high catalysis efficiency and selectivity. However, the controllable and efficient synthesis of SACs remains a significant challenge. Herein, we report a controlled one‐pot synthesis of nickel single atoms embedded on nitrogen‐doped carbon nanotubes (NiSA−N−CNT) and nitrogen‐doped graphene (NiSA−N−G). The formation of NiSA−N−CNT is due to the solid‐to‐solid rolling up mechanism during the high temperature pyrolysis at 800 °C from the stacked and layered Ni‐doped g‐C 3 N 4 , g‐C 3 N 4 −Ni structure to a tubular CNT structure. Addition of citric acid introduces an amorphous carbon source on the layered g‐C 3 N 4 −Ni and after annealing at the same temperature of 800 °C, instead of formation of NiSA−N−CNT, Ni single atoms embedded in planar graphene type supports, NiSA−N−G were obtained. The density functional theory (DFT) calculation indicates the introduction of amorphous carbon source substantially reduces the structure fluctuation or curvature of layered g‐C 3 N 4 ‐Ni intermediate products, thus interrupting the solid‐to‐solid rolling process and leading to the formation of planar graphene type supports for Ni single atoms. The as‐synthesized NiSA−N−G with Ni atomic loading of ∼6 wt% catalysts shows a better activity and stability for the CO 2 reduction reaction (CO 2 RR) than NiSA−N−CNT with Ni atomic loading of ∼15 wt% due to the open and exposed Ni single atom active sites in NiSA−N−G. This study demonstrates for the first time the feasibility in the control of the microstructure of carbon supports in the synthesis of SACs.
Resorcinol formaldehyde-derived carbon xerogel (RFC) is a versatile material with tuneable properties, synthesized through a simple sol-gel method. This study presents nitrogen-doped RF carbon xerogel (N-RFC) with 11.8 at% nitrogen doping, offering a microporous architecture ideal for alkali metal-ion (Li, Na, K) batteries. The porous N-doped framework enhances electrochemical performance by improving ion transport, increasing active storage sites, and significantly boosting metal-ion adsorption, particularly through pyrrolic nitrogen, as revealed by first-principles calculations supported by XPS analysis. N-RFC anodes showed excellent cycling stability, high-capacity retention, and fast charge/discharge capabilities, rendering them suitable for commercial applications. Notably, the N-RFC anode demonstrates high-rate long-term cycling stability, retaining its capacity of 83.5 % (188 mAh/g at 2 C-rate) and 50 % (133 mAh/g at 1250 mA/g) over 1000 cycles for Li and Na-ion batteries, respectively, favorable for commercial battery applications. Additionally, N-RFC demonstrates a reversible capacity of 120 mAh/g after 394 cycles with a retention of 82 % for K-ion batteries. The ability of the material to accommodate larger ions like Na + and K + further emphasizes its versatility and potential application in diverse alkali metal-ion battery systems.
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Renewably driven, electrochemical conversion of carbon dioxide into value-added products is expected to be a critical tool in global decarbonization. However, theoretical studies based on the computational hydrogen electrode largely ignore the nonlinear effects of the applied potential on the calculated results, leading to inaccurate predictions of catalytic behavior or mechanistic pathways. Here, we use grand canonical density functional theory (GC-DFT) to model electrochemical CO2 reduction (CO2R) over metal- and nitrogen-doped graphene catalysts (MNCs) and explicitly include the effects of the applied potential. We used GC-DFT to compute the CO2 to CO reaction intermediate energies at -0.3, -0.7, and -1.2 VSHE catalyzed by MNCs each doped with 1 of the 10 3d block metals coordinated by four pyridinic nitrogen atoms. Our results predict that Sc-, Ti-, Co-, Cu-, and Zn-N4Cs effectively catalyze CO2R at moderate to large reducing potentials (-0.7 to -1.2 VSHE). ZnN4C is a particularly promising electrocatalyst for CO2R to CO both at low and moderate applied potentials based on our thermodynamic analysis. Our findings also explain the observed pH independence of CO production over FeN4C and predict that the rate-determining step of CO2R over FeN4C is not *CO2- formation but rather *CO desorption. Additionally, the GC-DFT-computed density of states analysis illustrates how the electronic states of MNCs and adsorbates change non-uniformly with applied potential, resulting in a significantly increased *CO2- stability relative to other intermediates and demonstrating that the formation of the adsorbed *CO2- anion is critical to CO2R activation. This work demonstrates how GC-DFT paves the way for physically realistic and accurate theoretical simulations of reacting electrochemical systems.
Nanotechnology can improve the performance of dental polymers. The objective of this study was to modify the surfaces of nanoparticles with silanes and proteins, characterize nanoparticles’ agglomeration levels and interfaces between nanoparticles and the polymeric matrix. Undoped (n-TiO 2 ), nitrogen-doped (N_TiO 2 ) and nitrogen-fluorine co-doped titanium dioxide nanoparticles (NF_TiO 2 ) were synthesized and subjected to surface modification procedures in preparation for Small-Angle X-Ray Scattering (SAXS) and Small-Angle Neutron Scattering (SANS) characterizations. Experimental adhesives were manually synthesized by incorporating 20% (v/v) of n-TiO 2 , N_TiO 2 or NF_TiO 2 (as-synthesized or surface-modified) into OptiBond Solo Plus (OPTB). Specimens (n = 15/group; d = 6.0 mm, t = 0.5 mm) of OPTB and experimental adhesives were characterized using Time-of-Flight Secondary Ion Mass Spectroscopy (ToF-SIMS), 2-D ToF-SIMS chemical imaging and SANS. SAXS results indicated that surface-modified nanoparticles displayed higher scattering intensities in a particle-size dependent manner. ToF-SIMS results demonstrated that nanoparticles’ incorporation did not adversely impact the parental polymer. 2-D ToF-SIMS chemical imaging demonstrated the distribution of Ti + and confirmed nitrogen-doping levels. SANS results confirmed nanoparticles’ functionalization and revealed the interfaces between nanoparticles and the polymer matrix. Metaloxide nanoparticles were successfully fabricated, incorporated and covalently functionalized in a commercial dental adhesive resin, thereby supporting the utilization of nanotechnology in dentistry.