Nanoalloying effects on the catalytic activity of the formate oxidation reaction over AgPd and AgCuPd aerogels

Wang, Qiao; Chen, Fuyi; Guo, Longfei; Jin, Tao; Liu, Huazhen; Wang, Xiaolu; Gong, Xiaofang; Liu, Yaxing

doi:10.1039/c9ta00664h

Cited by 84 publications

(59 citation statements)

References 67 publications

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“…This low-intensity peak turns into a small broadband within the 2θ range from 38.7 to 41.6 • for the bimetallic 3% AgPd-Fe 3 O 4 sample. This band, along with the glimpsed wide bump centered at 45.5 • , is in full agreement with previously reported XRD patterns of bimetallic AgPd alloys presenting fcc crystalline structure [41][42][43][44], especially with those containing Ag:Pd molar ratio of 2:8 [42] or between 3:7 and 1:9 [41]. The main XRD diffraction of metal Pd is barely observed for the 2% Pd-Fe 3 O 4 sample and the region becomes totally flat for the 1% Pd-Fe 3 O 4 , which is coherent to the quantitative detection limit (<2%) associated to the XRD technique for multiphase mixtures [45].…”

Section: Development Of Nanocomposite (Ag)pd-fe 3 O 4 Materialssupporting

confidence: 92%

“…This lowintensity peak turns into a small broadband within the 2θ range from 38.7 to 41.6° for the bimetallic 3% AgPd-Fe3O4 sample. This band, along with the glimpsed wide bump centered at 45.5°, is in full agreement with previously reported XRD patterns of bimetallic AgPd alloys presenting fcc crystalline structure [41][42][43][44], especially with those containing Ag:Pd molar ratio of 2:8 [42] or between 3:7 and Furthermore, semiquantitative analysis of the XRD data by X'Pert Highscore Plus software confirmed the major presence of an orthorhombic Fe 3 O 4 structure in all (Ag)Pd-Fe 3 O 4 catalysts from Figure 3. Only for 1% Pd-Fe 3 O 4 and 3% AgPd-Fe 3 O 4 samples did the semiquantitative phase analysis provide a minor coexistence with the cubic Fe 3 O 4 structure (ca.…”

Section: Development Of Nanocomposite (Ag)pd-fe 3 O 4 Materialssupporting

confidence: 92%

“…On the other hand, an additional low-intensity peak at 2θ = 40.1° can be observed for the 3% Pd-Fe3O4 catalyst (Figure 3c), which corresponds to the (111) plane of metal Pd [41,42,44]. This lowintensity peak turns into a small broadband within the 2θ range from 38.7 to 41.6° for the bimetallic 3% AgPd-Fe3O4 sample.…”

Section: Development Of Nanocomposite (Ag)pd-fe 3 O 4 Materialsmentioning

confidence: 92%

“…XRD patterns of nanocomposite catalysts based on magnetite (from 85 • C synthesis using Fe 3+ /Fe 2+ molar ratio of 4) doped with Pd or Pd -Ag: 1% Pd-Fe 3 O 4 (a), 2% Pd-Fe 3 O 4 (b), 3% Pd-Fe 3 O 4 (c), 3% AgPd-Fe 3 O 4 (d). Symbols: (---) Fe 3 O 4 (ICSD: 01-075-1609); the highlighted strip defines the region where the highest intensity diffractions for pure Pd, pure Ag, and AgPd alloys are found[41][42][43][44].…”

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confidence: 99%

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(Ag)Pd-Fe3O4 Nanocomposites as Novel Catalysts for Methane Partial Oxidation at Low Temperature

et al. 2020

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Nanostructured composite materials based on noble mono-(Pd) or bi-metallic (Ag/Pd) particles supported on mixed iron oxides (II/III) with bulk magnetite structure (Fe3O4) have been developed in order to assess their potential for heterogeneous catalysis applications in methane partial oxidation. Advancing the direct transformation of methane into value-added chemicals is consensually accepted as the key to ensuring sustainable development in the forthcoming future. On the one hand, nanosized Fe3O4 particles with spherical morphology were synthesized by an aqueous-based reflux method employing different Fe (II)/Fe (III) molar ratios (2 or 4) and reflux temperatures (80, 95 or 110 °C). The solids obtained from a Fe (II)/Fe (III) nominal molar ratio of 4 showed higher specific surface areas which were also found to increase on lowering the reflux temperature. The starting 80 m2 g−1 was enhanced up to 140 m2 g−1 for the resulting optimized Fe3O4-based solid consisting of nanoparticles with a 15 nm average diameter. On the other hand, Pd or Pd-Ag were incorporated post-synthesis, by impregnation on the highest surface Fe3O4 nanostructured substrate, using 1–3 wt.% metal load range and maintaining a constant Pd:Ag ratio of 8:2 in the bimetallic sample. The prepared nanocomposite materials were investigated by different physicochemical techniques, such as X-ray diffraction, thermogravimetry (TG) in air or H2, as well as several compositions and structural aspects using field emission scanning and scanning transmission electron microscopy techniques coupled to energy-dispersive X-ray spectroscopy (EDS). Finally, the catalytic results from a preliminary reactivity study confirmed the potential of magnetite-supported (Ag)Pd catalysts for CH4 partial oxidation into formaldehyde, with low reaction rates, methane conversion starting at 200 °C, far below temperatures reported in the literature up to now; and very high selectivity to formaldehyde, above 95%, for Fe3O4 samples with 3 wt.% metal, either Pd or Pd-Ag.

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Section: Development Of Nanocomposite (Ag)pd-fe 3 O 4 Materialssupporting

confidence: 92%

Section: Development Of Nanocomposite (Ag)pd-fe 3 O 4 Materialssupporting

confidence: 92%

Section: Development Of Nanocomposite (Ag)pd-fe 3 O 4 Materialsmentioning

confidence: 92%

mentioning

confidence: 99%

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(Ag)Pd-Fe3O4 Nanocomposites as Novel Catalysts for Methane Partial Oxidation at Low Temperature

et al. 2020

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“…[18,23,[35][36] A mass activity of PdÀ Ni/KB is 7.8 A mg À 1 Pd (see Table S5), with a two-fold increase from PdÀ Ni/VC shows the superior fuel oxidation rate due to the effective utilization of the well distributed activated Pd sites in PdÀ Ni/KB during alkaline formate oxidation. [18,23,[35][36] A mass activity of PdÀ Ni/KB is 7.8 A mg À 1 Pd (see Table S5), with a two-fold increase from PdÀ Ni/VC shows the superior fuel oxidation rate due to the effective utilization of the well distributed activated Pd sites in PdÀ Ni/KB during alkaline formate oxidation.…”

Section: Influence Of Varying Carbon Support On Pdni Catalyst Performmentioning

confidence: 99%

Binary Pd−Ni Nanoalloy Particles over Carbon Support with Superior Alkaline Formate Fuel Electrooxidation Performance

et al. 2019

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Formate is the one legitimate carbon-neutral fuel that has the capability of being considered an alternative to alcohol fuels amidst the growing demand for efficient fuel-cell systems. In this manuscript, we demonstrate, for the first time, a class of binary PdÀ Ni alloy nanoparticles over two different carbon supports showing exceptional enhancement of the formate oxidation reaction (FOR) performance in alkaline medium, compared to Pd/C. The synergistic effects of Pd and oxophilic Ni along with the electronic structure alteration of Pd induced through alloying resulted in an effective change in its catalytic ability, leading to a 5-time enhancement in the overall current density along with a lower overpotential during formate oxidation compared to Pd/C. The more active Pd catalytic sites of the nanoalloy helped to yield mass activities as high as 4.5 A mg À 1 Pd and 7.8 A mg À 1 Pd during FOR. The structural and electrochemical analysis justifies the synergistic effects and alterations in the Pd lattice ensuing a superior enhancement of electrochemically active Pd sites.Direct liquid fuel cells (DLFCs) are regarded as one of the energy carriers of the future due to their plentiful advantages, including high power density, ease of handling and being part of the renewable energy series. [1][2][3][4][5] With alkaline-type direct liquid fuel cells being given greater attention than acid-type fuel cells, [6][7] formate is an ideal fuel alternative to ethanol and methanol. [8] Direct formate fuel cells (DFFCs) are also receiving immense attention due to the increased formate fuel regeneration possibilities especially those involving CO 2 . [9][10][11] Formate is further advantageous in terms of its nontoxic and environmentally friendly nature. [12][13] As such, DFFCs currently need potential efficient and stable catalysts for widespread commer-cial applications. Palladium is the catalyst that has shown the most promising prospects for enhanced liquid-fuel oxidation kinetics in alkaline media and that could effectively replace platinum. [14][15][16] However, there is an imminent need for performance improvements in Pd catalysts in terms of their efficiency and durability before they can be effectively utilized in alkaline DFFCs. Previous reports suggest that the formate oxidation reaction on the Pd surface proceeds through the decomposition of COO À into CO 3 2À in alkaline medium. [17] When considering advancements in Pd-based anode catalysts for alkaline formate oxidation, transition metal alloying has been shown to increase the alcohol and formic acid/formate fuel oxidation capabilities [5,[18][19][20][21] and to the best of our knowledge, alkaline formate oxidation using Pd-transition metal alloy catalysts has seldom been studied and is largely unexplored. Alloy catalysts of Pd with Au or Cu have been reported with marginal increases in the alkaline formate oxidation performance. [22][23] PdÀ Co alloy over Vulcan carbon obtained via solid-solution processing could yield a good FOR kinetics in our recent study. [18]...

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Porphyrin Aerogel Catalysts for Oxygen Reduction Reaction in Anion‐Exchange Membrane Fuel Cells

Zion

Douglin

Cullen

et al. 2021

Adv Funct Materials

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Platinum group metal (PGM)‐free catalysts for oxygen reduction reaction have shown high oxygen reduction reaction activity in alkaline media. In order to further increase the power density of anion‐exchange membrane fuel cells (AEMFCs), PGM‐free catalysts need to have a high site density to reach high current densities. Herein, synthesis, characterization, and utilization of heat‐treated iron porphyrin aerogels are reported as cathode catalysts in AEMFCs. The heat treatment effect is thoroughly studied and characterized using several techniques, and the best performing aerogel is studied in AEMFC, showing excellent performance, reaching a peak power density of 580 mW cm−2 and a limiting current density of as high as 2.0 A cm−2, which can be considered the state‐of‐the‐art for PGM‐free based AEMFCs.

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Nanoalloying effects on the catalytic activity of the formate oxidation reaction over AgPd and AgCuPd aerogels

Abstract: Nanoalloying effects and dealloying endow D-AgCuPd aerogels with significantly enhanced FOR activity compared to their monometallic, bimetallic and trimetallic counterparts.

Cited by 84 publications

References 67 publications

(Ag)Pd-Fe3O4 Nanocomposites as Novel Catalysts for Methane Partial Oxidation at Low Temperature

(Ag)Pd-Fe3O4 Nanocomposites as Novel Catalysts for Methane Partial Oxidation at Low Temperature

Binary Pd−Ni Nanoalloy Particles over Carbon Support with Superior Alkaline Formate Fuel Electrooxidation Performance

Porphyrin Aerogel Catalysts for Oxygen Reduction Reaction in Anion‐Exchange Membrane Fuel Cells

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