2018
DOI: 10.1016/j.jcat.2018.04.029
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Control of nitrogen activation ability by Co-Mo bimetallic nanoparticle catalysts prepared via sodium naphthalenide-reduction

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Cited by 39 publications
(43 citation statements)
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“…[38][39][40] We deconvoluted the XPS data and found that the spectra displayed a range of binding energies corresponding to different oxidation states (Tables S5-S13 †). The positions of the key peaks in the high resolution Co 2p3/2 at 778.1/778.4 AE 0.1 eV (before/aer 1000 cycles) and Mo 3d5/2 at 227.7/227.9 AE 0.1 eV (before/aer 1000 cycles) were in good agreement with the values of 778.5 eV and 228.2 eV reported by Hosono's group for Co 3 Mo 3 N prepared in ammonia at 785 C. 39 These values are consistent with the expected low valent state of metals due to the intermetallic nature of Co 3 Mo 3 N. We noted that although Mo-O and Co-O oxides were also present (inevitable as Co 3 Mo 3 N powders were handled in air), the peaks remained at the same position and intensity before and aer electrolysis. Finally, the analysis of 380-430 eV region, where both signals from Mo 3p and N 1s are present, showed a striking similarity with the Mo 3p spectra previously reported in the literature.…”
Section: Resultsmentioning
confidence: 99%
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“…[38][39][40] We deconvoluted the XPS data and found that the spectra displayed a range of binding energies corresponding to different oxidation states (Tables S5-S13 †). The positions of the key peaks in the high resolution Co 2p3/2 at 778.1/778.4 AE 0.1 eV (before/aer 1000 cycles) and Mo 3d5/2 at 227.7/227.9 AE 0.1 eV (before/aer 1000 cycles) were in good agreement with the values of 778.5 eV and 228.2 eV reported by Hosono's group for Co 3 Mo 3 N prepared in ammonia at 785 C. 39 These values are consistent with the expected low valent state of metals due to the intermetallic nature of Co 3 Mo 3 N. We noted that although Mo-O and Co-O oxides were also present (inevitable as Co 3 Mo 3 N powders were handled in air), the peaks remained at the same position and intensity before and aer electrolysis. Finally, the analysis of 380-430 eV region, where both signals from Mo 3p and N 1s are present, showed a striking similarity with the Mo 3p spectra previously reported in the literature.…”
Section: Resultsmentioning
confidence: 99%
“…Finally, the analysis of 380-430 eV region, where both signals from Mo 3p and N 1s are present, showed a striking similarity with the Mo 3p spectra previously reported in the literature. 39 The deconvolution of the spectrum (Fig. S14 †) allowed us to assign the position of N 1s peak at 397.0 AE 0.1 eV.…”
Section: Resultsmentioning
confidence: 99%
“…Isotopic nitrogen exchange studies have also demonstrated that, dependent upon pre-treatment conditions, a significant fraction of the lattice nitrogen can be exchanged [21] . In addition, N vacancy sites have been shown to be important for N 2 activation on supported Co-Mo nanoparticles [22] . In an investigation of the isostructural Co 3 Mo 3 C system aimed at developing understanding of the potential role of lattice N in catalytic ammonia synthesis, onset of activity was found to occur at higher temperatures than that of Co 3 Mo 3 N and also to be associated with progressive substitution of lattice C by N during the course of the reaction [23] .…”
mentioning
confidence: 99%
“…33,34 In this work, sodium naphthalenide driven reduction has been applied to prepare CoMo bimetallic particles supported upon CeO 2 which possess enhanced activity with respect to Co 3 Mo 3 N. Characterisation suggested that the active phase comprises dispersed nanosized Co 3 Mo 3 N on the CeO 2 support and interestingly, as dispersion increased, so did the ammonia synthesis turnover frequency which was related to the enhanced ease of formation of nitrogen vacancies. 34 Taking our work further, we have investigated in detail two mechanisms of ammonia synthesis on Co 3 Mo 3 N-(111) surfaces, which are depicted in Scheme 3. 35 The first is a Langmuir-Hinshelwood based dissociative mechanism which happens at surface cavities.…”
Section: Computational Modellingmentioning
confidence: 97%