Wall- and Hybridisation-Selective Synthesis of Nitrogen-Doped Double-Walled Carbon Nanotubes

Abstract

Controlled nitrogen-doping is ap owerfulm ethodology to modify the properties of carbon nanostructures and produce functional materials for electrocatalysis,e nergy conversion and storage,a nd sensing, among others.H erein, we report aw all-and hybridisation-selective synthetic methodology to produce double-walled carbon nanotubes with an inner tube doped exclusively with graphitic sp 2 -nitrogen atoms. Our measurements shed light on the fundamental properties of nitrogen-doped nanocarbons opening the door for developing their potential applications.Controlled substitutional nitrogen-doping is ap owerful methodology to modify the properties of carbon nanostructures. [1][2][3][4][5][6][7][8][9][10][11][12][13][14] Thes ynthesis and characterisation of nitrogendoped fullerenes,c arbon nanotubes,g raphene and graphene nanoribbons have revealed that nitrogen-doped carbon nanostructures are promising materials for electrocatalysis, [2-9, 11, 13, 14] energy conversion and storage, [2, 4-7, 10, 13, 14] and sensing, [13,14] among others.T he synthesis of nitrogen-doped nanocarbons still presents challenges for controlling:( i) the inclusion percent and the distribution of nitrogen within the [*] Dr.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under https://doi.

Exclusive Substitutional Nitrogen Doping on Graphene Decoupled from an Insulating Substrate

“…Regarding the N incorporation into the lattice of N-graphene grown on the Cu(111) substrate, Figure 3 b,d shows the core level N 1s spectra where the components below 399 eV recorded straight after the molecular deposition correspond to the nitrilic and pyridinic bonding environments in agreement with the structure of the molecule. 40 On the other hand, after annealing, the N-graphene spectrum is notoriously different. A considerable number of studies reported in the literature have focused on N-graphene, but in seldom cases, both local and bulk sensitive methods have successfully proven to be a N incorporation profile.…”

“…A dicyanopyrazophenanthroline C 16 H 6 N 6 molecule was used as C/N feedstock, and its synthesis and capability to induce the incorporation on the graphene network have been reported elsewhere. 40 We have grown N-doped graphene, and its spectroscopic characterization has been carried out in situ in ultrahigh vacuum (UHV) via photoemission spectroscopy (PES) in different energy ranges as explained later, as well as with low-energy electron diffraction (LEED). PES was performed using a dedicated spectrometer equipped with a monochromated Al Kα source (1486.6 eV) and a Scienta RS4000 analyzer.…”

“…Herein, we report an on-surface synthesis method to grow N-graphene using a nitrogen-rich polycyclic aromatic hydrocarbon as feedstock, namely, dicyanopyrazophenanthroline (see Figure 1 ). 40 This derivative possesses a high C/N ratio (16:6): all the nitrogen atoms are incorporated into the aromatic framework in sp 2 - or other sp-N configuration, and it can be deposited by sublimation. The molecular deposition studies on different surfaces include single-crystalline Cu(111), polycrystalline copper foil, and the corresponding oxidized surfaces.…”