JULIO NANDENHA
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Artigo IPEN-doc 27425 Methane activation on PdMn/C‑ITO electrocatalysts using a reactor‑type PEMFC2020 - NANDENHA, J.; YAMASHITA, J.Y.; SOUZA, F.M.; FONTES, E.H.; BATISTA, B.L.; SANTOS, M.C.; LINARDI, M.; NETO, A.O.Various palladium and manganese supported in a mix of carbon and indium thin oxide (PdMn/C-ITO) compositions were synthesized by a sodium borohydride reduction process for methane activation at low temperatures in a proton exchange membrane fuel cell (PEMFC) reactor. These electrocatalysts were characterized by X-ray diffraction, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy XPS, inductively coupled plasma mass spectrometry ICP-MS, attenuated total reflection-Fourier transform infrared spectroscopy, cyclic voltammetry and a PEMFC reactor. The diffractograms of PdMn/C-ITO electrocatalysts revealed the face-centered cubic structure of palladium and the bixbyite cubic structure of In2O3. TEM experiments showed mean nanoparticle sizes between 4.7 and 5.2 nm for all electrocatalysts. XPS results showed the presence of palladium and manganese oxides, as well as Pd0 species. Cyclic voltammograms of PdMn/C-ITO electrocatalysts showed an increase in current density values after the methane adsorption, this result is related to formation of methanol or formic acidic. Polarization curves at 80 °C acquired in a PEMFC reactor showed that PdMn(70:30)/C-ITO and PdMn(50:50)/C-ITO have superior performance when compared to Pd/C-ITO indicating the beneficial effect of adding Mn, this behavior can be attributed to the bifunctional mechanism or to the electronic effect of support.Artigo IPEN-doc 27220 Methane activation at low temperature in an acidic electrolyte using PdAu/C, PdCu/C, and PdTiO2/C electrocatalysts for PEMFC2020 - SOUZA, FELIPE de M.; SOUZA, RODRIGO F.B. de; BATISTA, BRUNO L.; SANTOS, MAURO C. dos; FONSECA, FABIO C.; OLIVEIRA NETO, ALMIR; NANDENHA, JULIOPd/C, PdAu/C, PdCu/C, and PdTiO2/ C electrocatalysts were prepared by a sodium borohydride reduction process for methane activation at low temperatures in a PEMFC reactor. These electrocatalysts were characterized by XRD, TEM, XPS, ICP-MS, ATR-FTIR, and cyclic voltammetry. The diffractograms of Pd/C, PdAu(50:50)/C, PdCu(50:50)/C, and PdTiO2( 50:50)/C electrocatalysts showed peaks associated with Pd face-centered cubic structure. PdAu(50:50)/C showed a small shift in the peak center when it was compared to Pd/C, while PdCu(50:50)/C showed a shift to higher angles when it was also compared to Pd/C. This effect can be due to the formation of an alloy between Pd and Au, and Pd and Cu. By TEM experiments, a mean nanoparticle size was observed between 6.9 and 8.9 nm for all electrocatalysts. Cyclic voltammograms of Pd/C, PdAu/C, PdCu/C and PdTiO2/ C electrocatalysts showed an increase in current density values after the adsorption of methane The ATR-FTIR experiments showed for all electrocatalysts the formation of methanol and formic acidic. Polarization curves at 80 °C acquired in a PEMFC reactor showed that PdAu(50:50)/C and PdTiO2( 50:50)/C had superior performance when compared to Pd/C, indicating the beneficial effect of adding the co-catalyst; this behavior has been attributed to the bifunctional mechanism or electronic effect.Artigo IPEN-doc 26874 High activity of Pt–Rh supported on C–ITO for ethanol oxidation in alkaline medium2020 - CAMARGO, V.F. de; FONTES, E.H.; NANDENHA, J.; SOUZA, R.F.B. de; NETO, A.O.PtRh/C–ITO electrocatalysts were prepared in a single-step method using H2PtCl6 ·6H2O and RhCl3 ·xH2O as metal sources, sodium borohydride as the reducing agent and a physical mixture of 85% Vulcan Carbon XC72 and 15% In2O3 ·SnO2 (indium tin oxide—ITO) as support. PtRh/C–ITO were characterized by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy (XPS), cyclic voltammetry, chronoamperommetry, attenuated total reflectance, Fourier transform infrared spectroscopy and performance test on direct alkaline ethanol fuel cell. X-ray diffraction patterns for all PtRh/C–ITO indicated a shift in Pt (fcc) peaks, showing that Rh was incorporated into Pt lattice. Transmission electron microscopy for PtRh/C–ITO showed nanoparticles homogeneously distributed over the support with particles size between 3.0 and 4.0 nm. The XPS results for Pt70Rh30/C–ITO showed the presence of mixed oxidation states of Sn0 and SnO2 that could favor the oxidation of adsorbed intermediates by bifunctional mechanism. Pt90Rh10/C–ITO was more active in electrochemical studies, which could be associated with the C–C bond break. Experiments in direct alkaline ethanol fuel cells showed that the power density values obtained for Pt70Rh30/C–ITO and Pt90Rh10/C–ITO were higher than Pt/C, indicating the beneficial effect of Rh addition to Pt and the use of C–ITO support.Artigo IPEN-doc 26619 Activation of methane on PdZn/C electrocatalysts in an acidic electrolyte at low temperatures2019 - NANDENHA, J.; NAGAHAMA, I.H.F.; YAMASHITA, J.Y.; FONTES, E.H.; AYOUB, J.M.S.; SOUZA, R.F.B. de; FONSECA, F.C.; NETO, A.O.PdZn/C electrocatalysts were prepared by sodium borohydride utilized as reducing agent for activation methane in an acidic medium at room temperature and in a proton exchange membrane fuel cell (PEMFC) at 80°C. The materials prepared were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The diffractograms of the PdZn/C electrocatalysts showed only peaks associated with Pd face-centered cubic (fcc) structure. Cyclic voltammograms (CV) of all electrocatalysts after adsorption of methane shown an increment in current during the anodic scan, this effect was more pronounced for Pd(70)Zn(30)/C. In situ ATR-FTIR (Attenuated Total Reflectance-Fourier Transform Infrared) experiments was not observed the formation of intermediates adsorbed for PdZn/C electrocatalysts, this behavior indicated that the methane oxidation occurs by parallel mechanisms. Polarization curves at 80°C in PEMFC show that Pd(90)Zn(10)/C has superior performance over the other electrocatalysts in methane oxidation.Artigo IPEN-doc 26482 Partial oxidation of methane and generation of electricity using a PEMFC2019 - NANDENHA, J.; PIASENTIN, R.M.; SILVA, L.G.M.; FONTES, E.H.; NETO, A.O.; SOUZA, R.F.B. deThe aim of this work was to produce methanol through partial oxidation of methane. The gas fed in a solid membrane reactor- PEM fuel cell type (H2/H2O2 + CH4) has been used for electrosynthesis of methanol at room temperature, with electricity cogeneration as a benefit. It was observed that the current density measured when injected CH4 in the cathode decreased about 45%. This occurs due to the conversion of methane inmethanol in some ranges of potentials. In the other hand, in lower ranges of cell potential, formaldehyde was found. In this work, methane was injected on the cathode together with H2O2 solution, where it was observed that the catalytic layer adsorbed CH4 and H2O2 in active sites, which produced OH− radicals that reacted with the hydrocarbon.