Tunable Periodically Ordered Mesoporosity in Palladium Membranes Enables Exceptional Enhancement of Intrinsic Electrocatalytic Activity for Formic Acid Oxidation

Ding, Jia; Li, Zhi; Liu, Xiaorui; Liu, Bin; Liu, Jie; Deng, Yida; Han, Xiaopeng; Hu, Wenbin; Zhong, Cheng

doi:10.1002/ange.201914649

Cited by 22 publications

(20 citation statements)

References 58 publications

(64 reference statements)

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“…Accordingly, its MA approaches 27.25 A•mg −1 , higher than most reported activities of Pd-based electrocatalysts by more than one order of magnitude (Fig. 4(d) and Table S8 in the ESM) [24,[36][37][38][39][40][44][45][46][47][48][49]. These performances also compare favorably to those of single-atom catalysts (such as Ir and Rh) reported recently [42,43], which can be attributed to the unique structural advantages of NPG and their interaction with surface PdHCN.…”

Section: Faor Activities Of Npg-pd and Npg-pd-au Electrodesmentioning

confidence: 48%

Highly coordinated Pd overlayers on nanoporous gold for efficient formic acid electro-oxidation

et al. 2021

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Design and fabrication of highly efficient and stable electrocatalysts remain key challenges in green energy technologies such as low-temperature direct liquid fuel cells. Based on in-depth theoretical calculations, here we demonstrate that surface Pd atoms with high coordination numbers (HCNs) can effectively modulate their adsorption energies for CO and OH, and thus achieve very high performance for formic acid electro-oxidation reaction (FAOR). Based on epitaxial coating Pd atomic layers onto nanoporous gold (NPG) thin membranes and a slight further decoration of Au clusters on top, the resulted core-shell structured NPG-Pd-Au electrocatalyst can demonstrate Pd intrinsic and mass activities of 8.62 mA•cm −2 and 27.25 A•mg −1 respectively at the peak potential around 0.33 V versus saturated calomel electrode toward FAOR, which are far better than those of commercial Pd/C catalysts (1.09 mA•cm −2 and 0.32 A•mg −1 ) tested under the same conditions. Moreover, the membrane electrode assemblies based on these low precious metal loading electrodes can achieve an anode Pd power efficiency over 10 W•mg −1 in a direct formic acid fuel cell, which is two orders of magnitude higher than that of the commercial Pd/C. These results provide new inspirations for the development of revolutionary electrodes for energy technologies in a rational manner.

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Section: Faor Activities Of Npg-pd and Npg-pd-au Electrodesmentioning

confidence: 48%

Highly coordinated Pd overlayers on nanoporous gold for efficient formic acid electro-oxidation

et al. 2021

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“…The development of the active anode catalysts for the oxidation of formic acid plays an important role in the DFAFCs' technologies. Nowadays, compared with Pt, Pd-based catalysts are considered as a good candidate for anode catalysts because of their high power density and anti-poisoning ability [3,4]. However, the high cost and the low stability of Pd-based catalysts limit their practical application.…”

Section: Introductionmentioning

confidence: 99%

High Active PdSn Binary Alloyed Catalysts Supported on B and N Codoped Graphene for Formic Acid Electro-Oxidation

Chen

Pei

et al. 2020

Catalysts

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A series of PdSn binary catalysts with varied molar ratios of Pd to Sn are synthesized on B and N dual-doped graphene supporting materials. The catalysts are characterized by X-ray diffraction (XRD) and Transmission electron microscopy (TEM). Formic acid electro-oxidation reaction is performed on these catalysts, and the results reveal that the optimal proportion of Pd:Sn is 3:1. X-ray photoelectron spectroscopy (XPS) measurements show that when compared with 3Pd1Sn/graphene, B and N co-doping into the graphene sheet can tune the electronic structure of graphene, favoring the formation of small-sized metallic nanoparticles with good dispersion. On the other hand, when compared with the monometallic counterparts, the incorporation of Sn can generate oxygenated species that help to remove the intermediates, exposing more active Pd sites. Moreover, the electrochemical tests illustrate that 3Pd1Sn/BN-G catalyst with a moderate amount of Sn exhibits the best catalytic activity and stability on formic acid electro-oxidation, owing to the synergistic effect of the Sn doping and the B, N co-doping graphene substrate.

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“…Ding et al reported the synthesis of electrodeposited Pd membranes with periodically ordered mesoporosity (Figure 4a), which delivered a high ECSA of 90.5 m 2 g −1 and a peak gravimetric current density of 3340 mA mg −1 (7.8 times higher than Pd/C). When tested in a passive fuel cell setup, the catalyst delivered a power density of 24.7 mW cm −2 at room temperature (Ding et al, 2020). Cao et al reported the synthesis of ordered mesoporous Pt nanocubes, where small Pt nanoparticles (5 nm) were found to act as building blocks to form mesoporous crystalline Pt nanocubes by an oriented attachment mechanism (Figure 4b).…”

Section: Anode Electrocatalystsmentioning

confidence: 99%

Recent advances in electrocatalysts, mechanism, and cell architecture for direct formic acid fuel cells

Bhaskaran

Abraham²,

Chetty³

2021

WIREs Energy & Environment

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Direct formic acid fuel cells (DFAFCs) are potential candidates as power sources for various applications, especially in portable electronics and medical diagnostic devices. Though they have been the subject of considerable research, commercial prototypes of DFAFCs are rudimentary compared to other liquid fuel cells, particularly the widespread methanol‐based direct methanol fuel cells. Various strategies for rationally engineering the electrocatalysts for enhancing DFAFC performance have been explored in the last few years, such as alloying noble metals with earth‐abundant transition metals, designing specific morphological and structural arrangements, decorating the surface with corrosion‐tolerant cocatalysts, and providing better catalyst support for effective catalyst dispersion. An overall approach may be necessary and should include (i) understanding the underlying mechanism, which will guide the direction of catalyst engineering, (ii) employing morphological, compositional, and structural control of the electrocatalysts to improve catalyst utilization and enhance the intrinsic activity for real‐world applications, and (iii) integrating these in a proficiently designed cell architecture suitable for targeted applications. In this review, we focus on the recent advances in electrocatalysts, formic acid electrooxidation mechanisms, and DFAFC cell architectures, which could help address the opportunities and challenges of commercializing DFAFC as a prospective alternative power source for portable applications. This article is categorized under: Fuel Cells and Hydrogen > Science and Materials Energy Research & Innovation > Science and Materials

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Tunable Periodically Ordered Mesoporosity in Palladium Membranes Enables Exceptional Enhancement of Intrinsic Electrocatalytic Activity for Formic Acid Oxidation

Cited by 22 publications

References 58 publications

Highly coordinated Pd overlayers on nanoporous gold for efficient formic acid electro-oxidation

Highly coordinated Pd overlayers on nanoporous gold for efficient formic acid electro-oxidation

High Active PdSn Binary Alloyed Catalysts Supported on B and N Codoped Graphene for Formic Acid Electro-Oxidation

Recent advances in electrocatalysts, mechanism, and cell architecture for direct formic acid fuel cells

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