The Effect of Lattice Strain on the Catalytic Properties of Pd Nanocrystals

Kuo, Chun Hong; Lamontagne, Leo K.; Brodsky, Casey N.; Chou, Lien‐Yang; Zhuang, Jia; Sneed, Brian T.; Sheehan, Margaret K.; Tsung, Chia Kuang

doi:10.1002/cssc.201300447

Cited by 116 publications

(124 citation statements)

References 48 publications

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“…On the other hand, Au 4f spectra saw positive shift of AuCu 3 relative to pure Au, while d-band center increased. [ 103,104 ] When subjected to tensile or compressive strain, shell metals undergo the change in overlap of d-electrons that leads to altered d-band widths, hence upshift/ downshift of d-band center towards Fermi level. [ 101 ] As a signifi cant descriptor of ORR activity, the location of d-band center cannot be too high or too low.…”

Section: Tuning Of Bimetallic Catalystsmentioning

confidence: 99%

Non‐Pt Nanostructured Catalysts for Oxygen Reduction Reaction: Synthesis, Catalytic Activity and its Key Factors

Xia

Chen

et al. 2016

Advanced Energy Materials

170

107

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caused by electrochemical polarization, Ohmic polarization and mass transport polarization. [ 4 ] The electrochemical reaction occurring on the cathode is oxygen reduction reaction (ORR). It is kinetically much more sluggish as compared to anode reaction, thereby calling for effi cient ORR catalysts. [ 1 ] Basically for ORR catalysis there are two main pathways, i.e., direct 4e pathway (O 2 + 4H + + 4e − → 2H 2 O) and 2 by 2e pathway (O 2 + 2H + + 2e → H 2 O 2 , H 2 O 2 + 2H + + 2e → 2H 2 O), the latter of which ends up with H 2 O 2 generation in 2-electron pathway or H 2 O generation in 4-electron pathway, making the 4-electron pathway more efficient and desirable. [ 1,5 ] In the past few decades, Pt catalysts have been considered to be the best catalysts; however, typical problems facing Pt, including unsatisfactory long-term durability due to dissolution, methanol crossover and CO poisoning, are hindrances to mass application of PEMFC and make it a nontrivial issue to develop some novel cathode electrocatalysts. [ 6,7 ] Moreover, around half of the cost of PEMFC power system is the fuel cell stack cost, a large proportion of which stems from expensive Pt catalysts; unlike other stack components, Pt catalyst cost seems to be less affected by economies of sale due to the scarcity and increasing demand of Pt. [ 8 ] Many strategies have therefore been proposed to address these challenges. They can reasonably be classifi ed into two types, i.e., lowering the Pt concentration by mixing Pt with other metals to form Pt-based alloys [ 7,9 ] or Pt-skin/skeleton surface structures, [ 10,11 ] and developing non-Pt catalysts [ 12 ] or even metalfree catalysts. [ 13 ] Recently, a wide variety of non-Pt ORR catalysts have been intensively studied as substitutes for state-ofthe-art Pt or Pt-based catalysts. Monometallic catalysts such as Au, Ag with tunable particle size, morphology and preferential surface orientation have attracted growing attention due to their enhanced activities; in particular, monometallic catalysts supported on graphene or its derivatives are shown to have extraordinary catalytic performance and long-term durability since graphene, with its sp 2 -hybridized honeycomb structure, enhances mass transport and electron transfer, and the synergetic coupling between monometallic catalysts and graphene supports prevents the occurrence of particle dissolution and aggregation. [ 6,14 ] Similarly, metal chalcogenides grown on (heteroatom-doped) graphenes have noticeably higher ORR activities relative to unsupported counterparts due to the Pt-based electrocatalysts for the oxygen reduction reaction (ORR) are the topic of extensive and intensive research since a few decades. Nevertheless, the scarcity of these Pt-based electrocatalysts, their high cost and unsatisfactory durability are the primary hindrances to their further commercialization. In recent years, non-Pt electrocatalysts have garnered considerable interest as alternatives to Pt-based catalysts for the ORR. This review highlights the synthesis, catalyti...

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Section: Tuning Of Bimetallic Catalystsmentioning

confidence: 99%

Non‐Pt Nanostructured Catalysts for Oxygen Reduction Reaction: Synthesis, Catalytic Activity and its Key Factors

Xia

Chen

et al. 2016

Advanced Energy Materials

170

107

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“…Further, the high surface area or presence of high surface active atoms, which is increased as a result of the introduction of an inner surface of the core in addition to the outer surface of the shell as well as presence of cage effect, sharp corners, edges and rough surface in its structure can be attributed to the overall better catalytic activity than solid Pd nanostructures. In addition, the confinement of reactive species inside the cavities also supports the high catalytic efficiency of hollow and porous bimetallic nanocatalysts …”

Section: Resultsmentioning

confidence: 84%

“…Bimetallic nanoparticles with core‐shell structure possess complex electronic interaction between two elements and exhibit better catalytic efficiency. This enhancement is mainly due to the ligand effect which modifies the position of d‐band center and alters the charge transfer, adsorption and activation energy of the electrocatalyst …”

Section: Introductionmentioning

confidence: 99%

Cubic Palladium Nanorattles with Solid Octahedron Gold Core for Catalysis and Alkaline Membrane Fuel Cell Applications

et al. 2019

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Herein, we report the synthesis of palladium nanorattles (Au‐Pd NRTs) comprising of a gold octahedral core caged within a thin porous cubic palladium shell. The introduction of core‐shell and porous architecture was realized by combining seed mediated and galvanic replacement reaction techniques. Next, we examined the catalytic efficiency of the nanocatalyst in comparison with solid palladium nanocube (Pd‐NC) of similar size for the degradation of p‐nitrophenol and organic dyes. The rate constant of Au‐Pd NRTs was found nearly 12 times higher than the Pd‐NCs. Further, we exploited our catalyst for electrochemical oxygen reduction reaction (ORR) and observed its high intrinsic ORR activity. Compared with commercialized Pt/C, the Au‐Pd NRT displayed nearly comparable onset and half‐wave potential values and excellent durability upon potential cycling. The system level validation in a single‐cell mode of alkaline exchange membrane fuel cell also confirms the efficiency of the present catalyst to serve as a potential cathode catalyst for realistic device applications.

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“…[11] We have developed an ew synthetic condition to grow highly uniform Au-Pd core-shell cubes (ca. [35] Here we show that lattice expansion can still be observed in Au-Pd THH nanocrystals with very thick Pd shells.I nterestingly,f or Au-Pd core-shell nanocubes and octahedra, it is the Au (200) peaks showing slight right-shift by 0.20-0.258 8 2 q.S imilar right-shift for the Au peak was also recorded in various Au-Pd core-shell nanocrystals reported previously but not recognized at that time. [13] Apart from core-shell particles,60nm Pd cubes and 61 nm octahedra have also been synthesized.…”

mentioning

confidence: 61%

Facet‐Dependent and Light‐Assisted Efficient Hydrogen Evolution from Ammonia Borane Using Gold–Palladium Core–Shell Nanocatalysts

et al. 2016

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Au-Pd core-shell nanocrystals with tetrahexahedral (THH), cubic, and octahedral shapes and comparable sizes were synthesized. Similar-sized Au and Pd cubes and octahedra were also prepared. These nanocrystals were used for the hydrogen-evolution reaction (HER) from ammonia borane. Light irradiation can enhance the reaction rate for all the catalysts. In particular, Au-Pd THH exposing {730} facets showed the highest turnover frequency for hydrogen evolution under light with 3-fold rate enhancement benefiting from lattice strain, modified surface electronic state, and a broader range of light absorption. Finite-difference time-domain (FDTD) simulations show a stronger electric field enhancement on Au-Pd core-shell THH than those on other Pd-containing nanocrystals. Light-assisted nitro reduction by ammonia borane on Au-Pd THH was also demonstrated. Au-Pd tetrahexahedra supported on activated carbon can act as a superior recyclable plasmonic photocatalyst for hydrogen evolution.

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The Effect of Lattice Strain on the Catalytic Properties of Pd Nanocrystals

Cited by 116 publications

References 48 publications

Non‐Pt Nanostructured Catalysts for Oxygen Reduction Reaction: Synthesis, Catalytic Activity and its Key Factors

Non‐Pt Nanostructured Catalysts for Oxygen Reduction Reaction: Synthesis, Catalytic Activity and its Key Factors

Cubic Palladium Nanorattles with Solid Octahedron Gold Core for Catalysis and Alkaline Membrane Fuel Cell Applications

Facet‐Dependent and Light‐Assisted Efficient Hydrogen Evolution from Ammonia Borane Using Gold–Palladium Core–Shell Nanocatalysts

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