Understanding the enhanced catalytic activity of Cu1@Pd3(111) in formic acid dissociation, a theoretical perspective

He, Feng; Li, Kai; Xie, Guangyou; Wang, Ying; Jiao, Menggai; Tang, Hao; Wu, Zhijian

doi:10.1016/j.jpowsour.2016.03.062

Cited by 39 publications

(22 citation statements)

References 69 publications

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“…Evenw hen the activity was normalized by the ECSA, our catalyst still showede nhanced specific activity (Figure4c). [38][39][40] Therefore, the superior performance of the as-prepared 3D super-branched PdCu alloy is probablya scribed to the improved electronic properties provided by the alloyed structure as well as the unique branched structures. Alloying with other secondary metals is usually effective for enhancement of the activity and the stability of the catalysts.…”

Section: Resultsmentioning

confidence: 99%

“…Alloying with other secondary metals is usually effective for enhancement of the activity and the stability of the catalysts. [38][39][40] Therefore, the superior performance of the as-prepared 3D super-branched PdCu alloy is probablya scribed to the improved electronic properties provided by the alloyed structure as well as the unique branched structures. [38,41] The surfacea rea and mass activity of the 3D super-branched PdCu alloy in comparison with other reported Pd-based electrocatalyst materials are summarized in Ta ble S1 (Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

“…A comparison of the current density of formic acid oxidation at 0.3 V on the 3D super‐branched PdCu alloy, 3D branched Pd, and PdB catalyst shows that our sample exhibits higher current density than those of 3D branched Pd and PdB (Figure d). Alloying with other secondary metals is usually effective for enhancement of the activity and the stability of the catalysts . Therefore, the superior performance of the as‐prepared 3D super‐branched PdCu alloy is probably ascribed to the improved electronic properties provided by the alloyed structure as well as the unique branched structures .…”

Section: Resultsmentioning

confidence: 99%

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Three‐Dimensional Super‐Branched PdCu Nanoarchitectures Exposed on Controlled Crystal Facets

Iqbal

Kim

et al. 2016

Chemistry A European J

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Despite the great success of controlled synthesis of metal nanocrystals with various sizes and morphologies, an efficient one-pot approach to preparing well-organized three-dimensional (3D) structures with unique facets exposed remains a great challenge. Herein, we report a unique 3D nanoarchitecture for PdCu alloy, created by a simple chemical reduction method, in which nanosized octahedral PdCu nanocrystals are directly assembled into 3D super-branched structures. Detailed investigations of its electrocatalytic performance demonstrate that the as-prepared facet-controlled PdCu super-branched nanostructures possess higher activity towards the formic acid oxidation reaction in comparison to the commercially available Pd black catalyst.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

See 1 more Smart Citation

Three‐Dimensional Super‐Branched PdCu Nanoarchitectures Exposed on Controlled Crystal Facets

Iqbal

Kim

et al. 2016

Chemistry A European J

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“…Thus, the method of improving the selectivity of FA decomposition (via dehydrogenation pathway) is desirable. To achieve this goal, FA decomposition on Pd surface has been studied both experimentally [8][9][10][11][12] and theoretically [13][14][15][16][17][18]. The experimental study showed that the reaction pathway on Pd(111) surface proceeds primarily via a dehydrogenation pathway at 280 K with the formation of CO 2 and H 2 , and HCOOgenerated by the cleavage of O-H bond in HCOOH is an important intermediate to enhance the reaction rate [8].…”

Section: Introductionmentioning

confidence: 99%

“…Besides pure Pd catalyst, there are also many studies focus on the Pd based alloys, such as Pd-Au [19], Pd-Ag [20], and Pd alloying with other metals [21][22][23] in order to enhance the dehydrogenation pathway. For the theoretical study, it is reported that the dehydrogenation pathway of FA decomposition on Pd(111) surface is the dominate pathway [14,17] based on the different density functionals. However, the obtained rate determining step is found to be different.…”

Section: Introductionmentioning

confidence: 99%

Density functional study on formic acid decomposition on Pd(111) surface: a revisit and comparison with other density functional methods

Wang

et al. 2021

J Mol Model

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The mechanism of formic acid decomposition on Pd(111) surface has been investigated by several theoretical methods in previous studies, including PBE and PW91. These results indicated that the mechanism is different from different methods, and even by using the same method (i.e., PBE), the mechanism is also different. In this study, we have revisited the formic acid decomposition on Pd(111) surface by using another density functional RPBE and by including van der Waals interaction which is neglected in the previous studies. Our results showed that the formic acid is decomposed via O-H bond cleavage to form bi-HCOO*, and the most favorable pathway is HCOOH* → bi-HCOO*+H* → CO 2 +2H*.The energy barrier is 0.55 eV at the rate-determining step. This conclusion is consistent with one of the PBE study. This demonstrated that computational methods have great in uence on the reaction mechanism, and care should be taken in selecting the appropriate computational methods.

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Co and Ni Ratio Modulation‐Derived Electron Deficient Pd Trimetallic Catalysts for Enhanced Formic Acid Electrooxidation

Li,

Jiang,

Zhu

et al. 2024

ChemistrySelect

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PdCoNi trimetallic catalysts attracted extensive interest in direct formic acid fuel cells due to high poisoning resistance and high activity for formic acid electro‐oxidation (FAO). Herein, a series of Pd0.75CoxNiy/C alloys with a modulated ratio of Co and Ni are synthesized to investigate the effect of Co and Ni content on the electronic structure of Pd for FAO. The physical analysis demonstrated that the introduction of Co and Ni induces the lattice strain effect compared to monometallic Pd catalysts. As a consequence of fixing the total amount of Co and Ni, the strain effect is restricted, and the electronic perturbation of Pd is successfully regulated by varying the ratio of Co and Ni in Pd0.75CoxNiy/C trimetallic alloys. Pd loses more electrons, the bond strength of Pd−H is weakened, and FAO activity is enhanced first and then decreased as the Co content increases. Among the trimetallic catalysts, Pd0.75Co0.125Ni0.125/C trimetallic catalyst exhibits the highest current density of 3.253 mA cm−2 owing to the optimum electronic perturbation and Pd−H bond strength. This work provides a valuable guideline for future studies of Pd‐based trimetallic alloys.

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Understanding the enhanced catalytic activity of Cu1@Pd3(111) in formic acid dissociation, a theoretical perspective

Cited by 39 publications

References 69 publications

Three‐Dimensional Super‐Branched PdCu Nanoarchitectures Exposed on Controlled Crystal Facets

Three‐Dimensional Super‐Branched PdCu Nanoarchitectures Exposed on Controlled Crystal Facets

Density functional study on formic acid decomposition on Pd(111) surface: a revisit and comparison with other density functional methods

Co and Ni Ratio Modulation‐Derived Electron Deficient Pd Trimetallic Catalysts for Enhanced Formic Acid Electrooxidation

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