Component-Controlled Synthesis and Assembly of Cu–Pd Nanocrystals on Graphene for Oxygen Reduction Reaction

Zheng, Yulin; Zhao, Shulin; Liu, Suli; Yin, Huanhuan; Chen, Yu-Yun; Bao, Jianchun; Han, Min; Dai, Zhihui

doi:10.1021/acsami.5b01541

Cited by 59 publications

(53 citation statements)

References 65 publications

(90 reference statements)

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“…For Pd alloy nanoparticles, it is commonly accepted that the outmost atomic layer consists of pure Pd, below which the transition metal atoms in the lattice induce the strain and the modified surface electronic structures (i.e., ligand effect). [5c,9] Compared with the lattice contraction induced by the strain effect, it is believed that the ligand effect plays a more critical role in determining the catalytic activity as well as the stability, which requires more precise and reliable measures to control the surface composition especially on the surface and subsurface layers …”

Section: Introductionmentioning

confidence: 99%

Synergistically Enhanced Oxygen Reduction Electrocatalysis by Subsurface Atoms in Ternary PdCuNi Alloy Catalysts

Wang

Luo

Zhu

et al. 2018

Adv Funct Materials

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For Pd-based alloy catalysts, the selection of metallic alloying elements and the construction of composition-gradient surface and subsurface layers are critical in achieving superior electrocatalytic activities in, e.g., the oxygen reduction reaction (ORR). Based on the Pd-containing alloy, highly monodispersed PdCuNi ternary alloy nanocrystals are prepared through a wet-chemical approach, and a solution-based oxidative surface treatment protocol is utilized to activate the surface of the nanocrystals. A drastically enhanced ORR activity can be achieved by removing the surface Ni and Cu atoms through the surface treatment protocol. The treated catalyst demonstrates a mass activity of 0.45 A mg Pd −1 in alkaline medium, 5 and 2.4 times those of commercial Pt/C and Pd/C, respectively. The first-principle calculation result suggests the critical roles of the coexistence of Ni and Cu atoms and their synergistic interaction beneath the outmost pure Pd layer in optimizing the oxygen binding energy for ORR. The calculation also suggests that the optimal binding energy of oxygen requires an appropriate Ni/Cu ratio in the subsurface layer. This work demonstrates a class of high-performance Pt-free ternary alloy ORR catalysts and may provide a general guideline for the structural design of Pd-based ternary alloy catalysts.

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Section: Introductionmentioning

confidence: 99%

Synergistically Enhanced Oxygen Reduction Electrocatalysis by Subsurface Atoms in Ternary PdCuNi Alloy Catalysts

Wang

Luo

Zhu

et al. 2018

Adv Funct Materials

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“…Note that the bimetallic alloys possess the so-named synergistic effects in the catalytic process; on one hand, the introduction of another metal can generate certain geometric configuration, which is called the ensemble effect, and on the other hand, the altered electronic structure induced by hetero te metal-metal bond is favorable for the activation of the catalyst [14,15]. A variety of Pd alloys, including PdAu [16][17][18], PdAg [19][20][21], PdRh [22], PdNi [23,24], PdCo [25,26], PdCu [27], and PdSn [28] have demonstrated higher ORR activities and enhanced long-term stabilities than the pure Pd-based catalysts.…”

Section: Introductionmentioning

confidence: 99%

Oxygen Reduction Reaction and Hydrogen Evolution Reaction Catalyzed by Pd–Ru Nanoparticles Encapsulated in Porous Carbon Nanosheets

Tian

Tang

et al. 2018

Catalysts

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Developing bi-functional electrocatalysts for both oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) is crucial for enhancing the energy transfer efficiency of metal-air batteries and fuel cells, as well as producing hydrogen with a high purity. Herein, a series of Pd-Ru alloyed nanoparticles encapsulated in porous carbon nanosheets (CNs) were synthesized and employed as a bifunctional electrocatalyst for both ORR and HER. The TEM measurements showed that Pd-Ru nanoparticles, with a size of approximately 1-5 nm, were uniformly dispersed on the carbon nanosheets. The crystal and electronic structures of the Pd x Ru 100−x /CNs series were revealed by powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The as-prepared samples exhibited effective ORR activity in alkaline media and excellent HER activity in both alkaline and acid solutions. The Pd 50 Ru 50 /CNs sample displayed the best activity and stability among the series, which is comparable and superior to that of commercial 10% Pd/C. For ORR, the Pd 50 Ru 50 /CNs catalyst exhibited an onset potential of 0.903 V vs. RHE (Reversible Hydrogen Electrode) and 11.4% decrease of the current density after 30,000 s of continuous operation in stability test. For HER, the Pd 50 Ru 50 /CNs catalyst displayed an overpotential of 37.3 mV and 45.1 mV at 10 mA cm −2 in 0.1 M KOH and 0.5 M H 2 SO 4 , respectively. The strategy for encapsulating bimetallic alloys within porous carbon materials is promising for fabricating sustainable energy toward electrocatalysts with multiple electrocatalytic activities for energy related applications.

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“…In addition, although the price of precious metal Pd is fluctuating widely as the market demand changes rapidly, developing Pd‐based catalysts is still of great importance to replace Pt ones because the reserve of Pd is much higher than Pt in nature. Previous research efforts focused on enhancing the activity of Pd catalysts by alloying Pd with 3d‐transition metals M (M=Fe, Co, Ni, Cu) . Most of these Pd−M alloys, either bi‐ or tri‐metallic, exhibited a high catalytic activity and durability in alkaline media .…”

Section: Introductionmentioning

confidence: 99%

Fully Ordered and Trace Au‐Doped Intermetallic PdFe Catalyst with Extra High Activity and Durability toward Oxygen Reduction Reaction

Zhu

et al. 2018

ChemistrySelect

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Developing Pt-free catalysts with high activity and durability is considered as an essential step for cost reduction and real commercialization of fuel cells. Previous Pt-free catalysts are either lack of activity and/or insufficient in durability. Here we report the first synthesis of a carbon-supported PdFe catalyst with a fully ordered intermetallic structure by controlling the atomic ratio of Pd and Fe and high-temperature annealing for structural ordering. This intermetallic catalyst is then doped with a trace amount of Au (atomic ratio of Au/Pd: 1/50) mainly in the surface region of the ordered lattice. Such an Au-doped intermetallic PdFe catalyst is finally demonstrated to possess a comparable catalytic activity and much better durability for oxygen reduction reaction than the commercial catalyst of Pt/ C. For example, the half-wave potential of the Au-PdFe catalyst decreases at a rate 9 times slower than that of Pt/C catalyst after potential cycling under harsh electrochemical conditions. The excellent activity and durability of this new catalyst is attributed to the ordered structure of PdFe particles and the protective effect of the surface Au doping. This study provides a new strategy to developing Pt-free catalysts, lowering the production cost, and accelerating the practical application of fuel cells.

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Component-Controlled Synthesis and Assembly of Cu–Pd Nanocrystals on Graphene for Oxygen Reduction Reaction

Cited by 59 publications

References 65 publications

Synergistically Enhanced Oxygen Reduction Electrocatalysis by Subsurface Atoms in Ternary PdCuNi Alloy Catalysts

Synergistically Enhanced Oxygen Reduction Electrocatalysis by Subsurface Atoms in Ternary PdCuNi Alloy Catalysts

Oxygen Reduction Reaction and Hydrogen Evolution Reaction Catalyzed by Pd–Ru Nanoparticles Encapsulated in Porous Carbon Nanosheets

Fully Ordered and Trace Au‐Doped Intermetallic PdFe Catalyst with Extra High Activity and Durability toward Oxygen Reduction Reaction

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