The ethanol oxidation reaction on bimetallic PdxAg1-x nanosheets in alkaline media and their mechanism study

Lao, Xianzhuo; Yang, Min; Chen, Jianyu; Zhang, Lian Ying; Guo, Peizhi

doi:10.1016/j.electacta.2021.137912

Cited by 42 publications

(53 citation statements)

References 47 publications

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“…The catalytic current densities of the Pd 20 Sn 24 NP‐modified GCEs in different catalytic temperature and reaction media are shown in Figure 7 and Table S2. It can be concluded that higher values of temperature, pH value, and ethanol concentration should have positive effects on overall reaction especially for the rate determination step on EOR [27,41] …”

Section: Resultsmentioning

confidence: 99%

“…It can be concluded that higher values of temperature, pH value, and ethanol concentration should have positive effects on overall reaction especially for the rate determination step on EOR. [27,41] Figure 8A shows a series of CV curves of the Pd 20 Sn 24 NPmodified GCE at different cycles. The current density increases gradually and reaches the peak value at the 39 th cycle, corresponding to the activation of Pd atoms and removal of surfactants produced by synthesis reactions, followed by the expose of fresh Pd atoms.…”

Section: Electrochemical Propertymentioning

confidence: 99%

“…XPS was recorded with an ESCALab220i-XLelectronic spectrometer from VG Scientific using 300 W A Kα radiation. [27]…”

Section: Materials Characterizationmentioning

confidence: 99%

“…Herein, we report that bimetallic Pd x Sn y NPs with large surface areas were used as electrocatalysts for EOR. The Pd x Sn y NPs were synthesized by an oil-bath approach with H 2 PdCl 4 and SnCl 2 • 2H 2 O as precursors, L-AA as the reducing agent, and cetyltrimethylammonium bromide as the structure-directing [27] Results and Discussion…”

Section: Introductionmentioning

confidence: 99%

“…3.2‐fold higher than commercial Pd/C counterpart) and remained 1603 mA mg −1 after 300 cycles. By controlling the catalytic temperature and OH − /ethanol concentrations, the mechanisms of Pd x Sn y NPs for EOR were discussed in detail [27] …”

Section: Introductionmentioning

confidence: 99%

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Synthesis of Free‐Standing Alloyed PdSn Nanoparticles with Enhanced Catalytic Performance for Ethanol Electrooxidation

Zhang

Yan

et al. 2021

ChemElectroChem

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Alloyed Pd-based nanostructured materials have been demonstrated as highly active fuel cell anode electrocatalysts for the alcohol oxidation reaction. Challenges remain in the controlled synthesis of freestanding PdM alloys catalysts through optimization of their interfacial and surface structures, which can prevent degradation and poor durability. Herein, we present an oil-bath-based approach to synthesize Pd x Sn y nanoparticles (NPs) with L-ascorbic acid (AA) as a reducing agent and cetyltrimethylammonium bromide as a structure-directing agent. Pd x Sn y NPs (x/y = 0.66, 0.83, and 1.11) show a particular freestanding shape. Among the three alloys, Pd 20 Sn 24 (x/y = 0.83) NPs have the best electrocatalytic activity (2018 mA mg À 1 ) toward the ethanol oxidation reaction (EOR). The enhanced performance of Pd x Sn y NPs might be attributed to i) a change in the electron structure of Pd, ii) varied interatomic distance within a unit cell, and iii) weak adsorption of in-situ generated oxygen-containing (e. g. *OH and PdÀ O) or carbon-containing (e. g. *CH 3 CHOH, *CH 3 CHO, and *CH 3 CO) intermediate species. Experimental data proposed that higher catalytic temperature, higher pH values, and higher ethanol concentration should accelerate each step of electrooxidation of the EOR.

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Section: Resultsmentioning

confidence: 99%

Section: Electrochemical Propertymentioning

confidence: 99%

“…XPS was recorded with an ESCALab220i-XLelectronic spectrometer from VG Scientific using 300 W A Kα radiation. [27]…”

Section: Materials Characterizationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Synthesis of Free‐Standing Alloyed PdSn Nanoparticles with Enhanced Catalytic Performance for Ethanol Electrooxidation

Zhang

Yan

et al. 2021

ChemElectroChem

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Organic Heterocyclic Strategy for Precisely Regulating Electronic State of Palladium Interface to Boost Alcohol Oxidation

Zhao

Zhang

et al. 2022

Adv Funct Materials

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Exploring highly‐efficient palladium (Pd)‐based electrocatalysts for the alcohol oxidation reaction (AOR) is crucial yet challenging for chemists due to the vague Pd interface with an uncontrollable electronic environment. Herein, an organic heterocyclic strategy is used for the first time to modulate the electronic state of Pd electrocatalysts by anchoring Pd nanoparticles to conjugated microporous polymers (CMPs) with varied S‐, N‐, O‐, or S, N‐heterocycles. Among these CMPs, the S, N‐containing thiazole heterocyclic polymer SNC with Pd catalyst exhibits highly‐efficient current densities of 1575.0 mA mgPd−1 for methanol oxidation and 1071.0 mA mgPd−1 for ethanol oxidation, which are among the highest performance in the heterocyclic modulated Pd systems and surpass the commercial Pd black catalyst. Detailed theory calculations suggest that although the furan (O‐heterocycle) polymer OC has the strongest charge transfer (0.057 |e|) with the Pd cluster, the moderate electron transfer (0.041 |e|) of the Pd/SNC heterojunction with an S···N···Pd noncovalent interaction shows the best catalytic reaction kinetics. Moreover, the d‐band of the Pd/SNC system is closer to the volcano vertex than its counterparts. These results indicate that appropriate electron transfer intensity regulation of Pd electronic state by well‐defined heterocyclic structures may significantly improve AOR activity.

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Porous PdWM (M = Nb, Mo and Ta) Trimetallene for High C1 Selectivity in Alkaline Ethanol Oxidation Reaction

Qin

Huang

et al. 2021

Advanced Science

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Direct ethanol fuel cells are among the most efficient and environmentally friendly energy-conversion devices and have been widely focused. The ethanol oxidation reaction (EOR) is a multielectron process with slow kinetics. The large amount of by-product generated by incomplete oxidation greatly reduces the efficiency of energy conversion through the EOR. In this study, a novel type of trimetallene called porous PdWM (M = Nb, Mo and Ta) is synthesized by a facile method. The mass activity (15.6 A mg Pd −1 ) and C1 selectivity (55.5%) of Pd 50 W 27 Nb 23 /C trimetallene, obtained after optimizing the compositions and proportions of porous PdWM, outperform those of commercial Pt/C (1.3 A mg Pt −1 , 5.9%), Pd/C (5.0 A mg Pd −1 , 7.2%), and Pd 97 W 3 /C bimetallene (9.5 A mg Pd −1 , 14.1%). The mechanism by which Pd 50 W 27 Nb 23 /C enhances the EOR performance is evaluated by in situ Fourier transform infrared spectroscopy and density functional theory calculations. It is found that W and Nb enhance the adsorption of CH 3 CH 2 OH and oxophilic high-valence Nb accelerates the subsequent oxidation of CO and -CH x species. Moreover, Nb promotes the cleavage of C-C bonds and increases the C1 selectivity. Pd 60 W 28 Mo 12 /C and Pd 64 W 27 Ta 9 /C trimetallene synthesized by the same method also exhibit excellent EOR performance.

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The ethanol oxidation reaction on bimetallic PdxAg1-x nanosheets in alkaline media and their mechanism study

Cited by 42 publications

References 47 publications

Synthesis of Free‐Standing Alloyed PdSn Nanoparticles with Enhanced Catalytic Performance for Ethanol Electrooxidation

Synthesis of Free‐Standing Alloyed PdSn Nanoparticles with Enhanced Catalytic Performance for Ethanol Electrooxidation

Organic Heterocyclic Strategy for Precisely Regulating Electronic State of Palladium Interface to Boost Alcohol Oxidation

Porous PdWM (M = Nb, Mo and Ta) Trimetallene for High C1 Selectivity in Alkaline Ethanol Oxidation Reaction

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