scholarly journals Surfactant-Free Colloidal Strategies for Highly Dispersed and Active Supported IrO2 Catalysts: Synthesis and Performance Evaluation for the Oxygen Evolution Reaction

Author(s):  
Francesco Bizzotto ◽  
Jonathan Quinson ◽  
Johanna Schröder ◽  
Alessandro Zana ◽  
Matthias Arenz

Supported Ir oxide catalysts obtained from surfactant-free colloidal Ir nanoparticles (NPs) synthesized in alkaline methanol (MeOH), ethanol (EtOH), and ethylene glycol (EG) are investigated and compared. The comparison of independent techniques such as transition electron microscopy (TEM), small angle X-ray scattering (SAXS), and electrochemistry allows shedding light on the parameters that affect the dispersion of the active phase as well as the catalytic activity. The colloidal dispersions obtained are suitable to develop supported catalysts with little NP agglomeration on a carbon support leading to highly active catalysts with more than 400 A g<sup>-1</sup><sub>Ir</sub> reached at 1.5 V<sub>RHE</sub> for the OER. While the more common surfactant-free alkaline EG synthesis requires flocculation and re-dispersion leading to Ir loss, the main difference between methanol and ethanol as solvent is related to the dispersibility of the support material. The choice of the suitable monoalcohol determines the maximum achieved Ir loading on the support without detrimental particle agglomeration. This simple consideration on catalyst design can readily lead to significantly improved catalysts.

2021 ◽  
Author(s):  
Francesco Bizzotto ◽  
Jonathan Quinson ◽  
Johanna Schröder ◽  
Alessandro Zana ◽  
Matthias Arenz

Supported Ir oxide catalysts obtained from surfactant-free colloidal Ir nanoparticles (NPs) synthesized in alkaline methanol (MeOH), ethanol (EtOH), and ethylene glycol (EG) are investigated and compared. The comparison of independent techniques such as transition electron microscopy (TEM), small angle X-ray scattering (SAXS), and electrochemistry allows shedding light on the parameters that affect the dispersion of the active phase as well as the catalytic activity. The colloidal dispersions obtained are suitable to develop supported catalysts with little NP agglomeration on a carbon support leading to highly active catalysts with more than 400 A g<sup>-1</sup><sub>Ir</sub> reached at 1.5 V<sub>RHE</sub> for the OER. While the more common surfactant-free alkaline EG synthesis requires flocculation and re-dispersion leading to Ir loss, the main difference between methanol and ethanol as solvent is related to the dispersibility of the support material. The choice of the suitable monoalcohol determines the maximum achieved Ir loading on the support without detrimental particle agglomeration. This simple consideration on catalyst design can readily lead to significantly improved catalysts.


Chemistry ◽  
2021 ◽  
Vol 3 (1) ◽  
pp. 338-359
Author(s):  
Magdalena Bonarowska ◽  
Zbigniew Kaszkur ◽  
Krzysztof Matus ◽  
Alicja Drelinkiewicz ◽  
Tomasz Szumełda ◽  
...  

We present an efficient strategy for synthesising the PdAu catalysts with a homogeneous PdAu alloy phase for environmentally important hydrodechlorination of tetrachloromethane in the gas phase. The synthesis of carbon-supported catalysts involved two major steps: (i) incorporation of palladium and gold nanoparticles into carbon support and (ii) activation of the catalysts. The critical part of this work was to find the optimal conditions for both steps. Thus, the incorporation of the nanoparticles was carried out in two ways, by impregnation and direct redox reaction method using acetone solutions of metal precursor salts. The activation was performed either by a conventional thermal reduction in hydrogen or flash irradiation in a microwave oven. The homogeneity and structure of the PdAu alloy were found to depend on the catalyst activation method critically. In all cases, we observed better homogeneity for catalysts that were subject to microwave irradiation. Moreover, the flash microwave irradiation of prepared catalysts provided catalysts of better stability and selectivity towards the desired products (hydrocarbons) in the hydrodechlorination of tetrachloromethane as compared to the catalyst obtained by conventional thermal activation in hydrogen.


2021 ◽  
Author(s):  
Guokang Han ◽  
Yongrong Sun ◽  
Yuxin Liu ◽  
Lingfeng Li ◽  
Xudong Li ◽  
...  

The nature of carbon support has huge effects on the catalytic properties of supported catalysts. When utilized for electrochemical purposes as support for precious metal in acid media, the oxygen...


Nanoscale ◽  
2015 ◽  
Vol 7 (21) ◽  
pp. 9467-9471 ◽  
Author(s):  
Meiling Xiao ◽  
Ligang Feng ◽  
Jianbing Zhu ◽  
Changpeng Liu ◽  
Wei Xing

A rapid strategy to synthesize a highly active PtRu alloy nano-sponge catalyst system for methanol electro-oxidation is presented. The greatly increased Pt utilization, anti-CO poisoning ability and electronic effect result from the porous nano-sponge structure.


2012 ◽  
Vol 84 (3) ◽  
pp. 495-508 ◽  
Author(s):  
Ekaterina S. Lokteva ◽  
Anton A. Peristyy ◽  
Natalia E. Kavalerskaya ◽  
Elena V. Golubina ◽  
Lada V. Yashina ◽  
...  

Laser electrodispersion (LED) of metals is a promising technique for the preparation of heterogeneous catalysts as an alternative to wet impregnation of supports with the corresponding salt solutions. The LED technique can be used to deposit highly active chloride- and nitrate-free metal nanoparticles onto carbon or oxide supports. We report preparation and properties of new Ni-, Pd-, and Au-containing alumina-supported catalysts with low metal loadings (10–3–10–4 % mass) and their comparison with the previously studied carbon (Sibunit) supported systems. The catalysts demonstrate high stability and extremely high specific catalytic activity (by 2–3 orders of magnitude higher than for traditional catalysts) in the gas-phase hydrodechlorination (HDC) of chlorobenzene (CB).


Author(s):  
Jesús Andrés Tavizón Pozos ◽  
Gerardo Chávez Esquivel ◽  
Ignacio Cervantes Arista ◽  
José Antonio de los Reyes Heredia ◽  
Víctor Alejandro Suárez Toriello

Abstract The influence of Al2O3–ZrO2 and TiO2–ZrO2 supports on NiMo-supported catalysts at a different sulfur concentration in a model hydrodeoxygenation (HDO)-hydrodesulfurization (HDS) co-processing reaction has been studied in this work. A competition effect between phenol and dibenzothiophene (DBT) for active sites was evidenced. The competence for the active sites between phenol and DBT was measured by comparison of the initial reaction rate and selectivity at two sulfur concentrations (200 and 500 ppm S). NiMo/TiO2–ZrO2 was almost four-fold more active in phenol HDO co-processed with DBT than NiMo/Al2O3–ZrO2 catalyst. Consequently, more labile active sites are present on NiMo/TiO2–ZrO2 than in NiMo/Al2O3–ZrO2 confirmed by the decrease in co-processing competition for the active sites between phenol and DBT. DBT molecules react at hydrogenolysis sites (edge and rim) preferentially so that phenol reacts at hydrogenation sites (edge and edge). However, the hydrogenated capacity would be lost when the sulfur content was increased. In general, both catalysts showed similar functionalities but different degrees of competition according to the highly active NiMoS phase availability. TiO2–ZrO2 as the support provided weaker metal-support interaction than Al2O3–ZrO2, generating a larger fraction of easily reducible octahedrally coordinated Mo- and Ni-oxide species, causing that NiMo/TiO2–ZrO2 generated precursors of MoS2 crystallites with a longer length and stacking but with a higher degree of Ni-promotion than NiMo/Al2O3–ZrO2 catalyst.


2013 ◽  
Vol 46 (5) ◽  
pp. 1508-1512 ◽  
Author(s):  
Byron Freelon ◽  
Kamlesh Suthar ◽  
Jan Ilavsky

Coupling small-angle X-ray scattering (SAXS) and ultra-small-angle X-ray scattering (USAXS) provides a powerful system of techniques for determining the structural organization of nanostructured materials that exhibit a wide range of characteristic length scales. A new facility that combines high-energy (HE) SAXS and USAXS has been developed at the Advanced Photon Source (APS). The application of X-rays across a range of energies, from 10 to 50 keV, offers opportunities to probe structural behavior at the nano- and microscale. An X-ray setup that can characterize both soft matter or hard matter and high-Zsamples in the solid or solution forms is described. Recent upgrades to the Sector 15ID beamline allow an extension of the X-ray energy range and improved beam intensity. The function and performance of the dedicated USAXS/HE-SAXS ChemMatCARS-APS facility is described.


2020 ◽  
Author(s):  
Shima Alinejad ◽  
Jonathan Quinson ◽  
Johanna Schröder ◽  
Jacob J. K. Kirkensgaard ◽  
Matthias Arenz

In this work, we investigate the stability of four different types of Pt/C fuel cell catalysts upon applying accelerated degradation tests (ADTs) in a gas diffusion electrode (GDE) setup equipped with an anion exchange membrane (AEM). In contrast to previous investigations exposing the catalysts to liquid electrolyte, the GDE setup provides a realistic three-phase boundary of the reactant gas, catalyst and ionomer which enables reactant transport rates close to real fuel cells. Therefore, the GDE setup mimics the degradation of the catalyst under more realistic reaction conditions as compared to conventional electrochemical cells. Combining the determination of the loss in electrochemically active surface area (ECSA) of the Pt/C catalysts via CO stripping measurements with the change in particle size distribution determined by small-angle X-ray scattering (SAXS) measurements, we demonstrate that i) the degradation mechanism depends on the investigated Pt/C catalyst and might indeed be different to the one observed in conventional electrochemical cells, ii) degradation is increased in an oxygen gas atmosphere (as compared to an inert atmosphere), and iii) the observed degradation mechanism depends on the mesoscopic environment of the active phase. The measurements indicate an increased particle growth if small and large particles are immobilized next to each other on the same carbon support flakes as compared to a simple mix of two catalysts with small and large particles, respectively.


2014 ◽  
Vol 70 (a1) ◽  
pp. C1173-C1173
Author(s):  
Kamila Wiaderek ◽  
Olaf Borkiewicz ◽  
Nathalie Pereira ◽  
Jan Ilavsky ◽  
Glenn Amatucci ◽  
...  

Batteries are complex multicomponent devices wherein mesoscale phenomena–the nanoscale structure and chemistry of different components, and interactions thereof–drive functionality and performance. For example, electron/ion transport within the composite electrodes relies on bi-continuous nanostructuring to form electrically and ionicly conductive paths. Electrochemical conversion of different salts of a given metal yields a common and ostensibly identical product: the zero valent metal. For example, maximal lithiation of iron-based electrodes produces metallic iron nanoparticles for oxide, fluoride, and oxyfluoride electrodes alike. Accordingly, these provide an opportunity to explore the coupling of nanostructure development and anion chemistry, and correlate these with electrochemical performance. We combine synchrotron-based small angle X-ray scattering (SAXS) and pair distribution function (PDF) measurements to probe metallic iron formed by electrochemical conversion of different iron compounds across multiple length-scales and decouple the influence of anion chemistry and reaction temperature on the atomic structure and nanoscale morphology.


Sign in / Sign up

Export Citation Format

Share Document