Bare laser-synthesized palladium–gold alloy nanoparticles as efficient electrocatalysts for glucose oxidation for energy conversion applications

Holade, Yaovi; Hebié, Seydou; Maximova, Ksenia; Sentís, M.; Delaporte, Philippe; Kokoh, K. Boniface; Napporn, Têko W.; Kabashin, Andrei V.

doi:10.1039/d0cy01323d

Cited by 12 publications

(10 citation statements)

References 61 publications

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“…Glucose and xylose ECO was studied at different temperatures ( T = 5–40 °C). Cyclic voltammograms recorded in the sugar solutions show anodic peak current density increasing with increasing temperature (Figure SI-16) as observed earlier by Yei et al The Arrhenius kinetic theory enables the determination of the electrochemical activation energy E a using experimental data according to eq , where R refers to the universal gas constant (8.314 J mol –1 K –1 ), while I and T correspond to current and temperature, respectively. Using the voltammetric data, E a was evaluated at different oxidation potentials ( E ox ) applied for glucose and xylose.…”

Section: Results and Discussionsupporting

confidence: 68%

“…42 The intensity of the oxidation peak in the reverse scan shown in Figure 5 was lower for xylose oxidation than for glucose. This would indicate that oxidation products from xylose are more strongly adsorbed than those from glucose as observed by Rafai ̈deen et al 45 The Arrhenius kinetic theory enables the determination of the electrochemical activation energy E a using experimental data according to eq 8 46,47…”

Section: Resultsmentioning

confidence: 95%

“…The low E a values (<50 kJ mol −1 ) indicate that the kinetics for glucose and xylose oxidation are largely governed by diffusion processes. 17,46,50,51 Long-term electrolyses at a constant potential of 1.3 V RHE were carried out to study the bulk conversion and selectivity of glucose and xylose ECO. The conversion of glucose increased with higher reaction temperatures reaching 64.6% at 40 °C (Table 2).…”

Section: Resultsmentioning

confidence: 99%

“…In the present study, the E a values obtained for glucose ECO ranged from 8 to 22 kJ mol –1 , while those for xylose ranged from 13 to 24 kJ mol –1 . The low E a values (<50 kJ mol –1 ) indicate that the kinetics for glucose and xylose oxidation are largely governed by diffusion processes. ,,, …”

Section: Results and Discussionmentioning

confidence: 99%

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Influence of Reaction Parameters on Nanogold-Catalyzed Glucose and Xylose Oxidation: A Joint Experimental and DFT Study

Oña,

Laverdure,

Latonen

et al. 2024

ACS Catal.

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The electrocatalytic oxidation (ECO) of glucose on gold requires alkaline conditions and relatively high potentials (>0.3 V RHE ). Although the adsorption of hydroxide ions (OH ads ) is also known to occur under these conditions, the generally accepted proton-coupled electron transfer mechanism for sugar ECO does not explicitly state the role of OH ads in the sugar adsorption or oxidation steps. To investigate this, we carried out a combined experimental and density functional theory (DFT) study on the ECO of glucose and xylose over a nanogold catalyst under temperature and pH control. Grand canonical DFT (GC-DFT) was used to identify the preferred reaction mechanism in which OH ads facilitates the thermodynamically feasible formation of gluconic and xylonic acid. Calculated results also showed that OH ads plays a role in improving the acid selectivity. Constant-potential electrolyses in sugar solutions were performed using mesoporous (Sibunit) carbon-supported Au nanoparticles (AuNPs) with an average cluster size of 4.7 nm. Experimental results showed that the highest conversions for glucose (57.7%) and xylose (49.4%) were obtained at 25 °C and pH 12.5, with gluconic and xylonic acid selectivity of 81.5 and 87.8%, respectively. The catalytic activities were high considering the low Au loading (∼0.1% wt). Higher pH led to a decrease in the ECO rate possibly due to excess hydroxide ions blocking active sites for sugar adsorption. Our results highlight the importance of computational studies in elucidating reaction mechanisms for sugar ECO where sugar acids are the main oxidation products. This is crucial in designing reaction systems for the viable production of these value-added chemicals from biomass.

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Section: Results and Discussionsupporting

confidence: 68%

Section: Resultsmentioning

confidence: 95%

Section: Resultsmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

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Influence of Reaction Parameters on Nanogold-Catalyzed Glucose and Xylose Oxidation: A Joint Experimental and DFT Study

Oña,

Laverdure,

Latonen

et al. 2024

ACS Catal.

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“…This accounts for the fact that pure and surfactant-free NPs produced by LSPC have been widely explored for biological and biomedical applications. 12 Recent illustrative examples of applications of the NPs in catalysis include Pt x Y for the ORR, 134 PdAu for glucose oxidation, 135 Pt NPs for the ORR toward fuel cell development, 136 or Au NPs for CO 2 electroreduction. 137 The size range typically obtained is 2−100 nm.…”

Section: Laser Synthesis and Processing Of Colloids (Lspc)mentioning

confidence: 99%

Surfactant-Free Colloidal Syntheses of Precious Metal Nanoparticles for Improved Catalysts

2023

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Colloidal syntheses of nanomaterials offer multiple benefits to study, understand, and optimize unsupported and supported catalysts. In particular, colloidal syntheses are relevant to the synthesis of (precious) metal nanoparticles. By separating the synthesis of the active phase, i.e., the nanoparticles, from supporting steps, a deeper knowledge and rational control of the properties of supported catalysts is gained. The effect(s) of the size, shape, and composition of the nanoparticle, the nature of the support, or the metal loading on a support can be studied in more systematic ways. The fundamental knowledge gained paves the way for catalyst optimization by tuning the catalyst activity, selectivity, and stability. However, most colloidal syntheses require the use of additives or surfactants, which are detrimental to most catalytic reactions because they typically block catalyst active sites. Surfactant removal is therefore often required, which adds complexity to the synthesis and the analysis of the obtained results. Developing surfactant-free strategies to obtain stable colloidal nanoparticles is therefore a rising field of research that is here reviewed. A focus is given to laser synthesis and processing of colloids-, solution plasma process-, N,N-dimethylformamide-, polyol-, and recently reported monoalcohol-based syntheses. The relevance of these synthetic approaches for catalysis is detailed with a focus on heterogeneous catalysis and electrocatalysis.

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Progress in Biomass Electro‐Valorization for Paired Electrosynthesis of Valuable Chemicals and Fuels

Abderrahmane,

Tingry,

Cornu

et al. 2024

Adv Energy and Sustain Res

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Environmental and energy concerns surrounding the use of fossil fuels are driving an increasingly rapid transition to sustainable and eco‐responsible processes. Electrochemical processes can provide the necessary sustainability and economic roadmap for storing intermittent and renewable electricity by synthesizing, in cogeneration electrolyzers, energy carriers and/or synthetic chemicals (hydrogen, ammonia, etc.) via flagship reduction reactions (hydrogen evolution reaction (HER), nitrogen reduction reaction (NRR), etc.). To balance the electrochemical process, these cathodic processes have long been coupled to the oxygen evolution reaction (OER), which ultimately consumes almost 90% of the energy input. Recent years have witnessed an overwhelming development of anode scenarios based on biomass substrates, because OER cannot be driven below a certain potential threshold, while organics are thermodynamically more favorable. Therefore, paired electrolysis, which refers to cases where electrochemical oxidation and reduction are desired, embraces the electrocatalysis community for the electrolytic production of hydrogen, ammonia, etc. (cathode side), in parallel with value‐added chemicals (anode side), all with a modest electricity input. The trade‐off is selectivity at relevant current densities. This review discusses, the progress, challenges, and potential of biomass‐fueled paired electrosynthesis of valuable chemicals and fuels. Fundamental principles, main biomass solubilization methods, and different scenarios for paired electrosynthesis are presented.

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Bare laser-synthesized palladium–gold alloy nanoparticles as efficient electrocatalysts for glucose oxidation for energy conversion applications

Abstract: Electrochemical energy converters based on biomass-based organic molecules such as glucose have recently demonstrated a great potential for the development of functional bioimplantable devices such as pacemakers, but such converters...

Cited by 12 publications

References 61 publications

Influence of Reaction Parameters on Nanogold-Catalyzed Glucose and Xylose Oxidation: A Joint Experimental and DFT Study

Influence of Reaction Parameters on Nanogold-Catalyzed Glucose and Xylose Oxidation: A Joint Experimental and DFT Study

Surfactant-Free Colloidal Syntheses of Precious Metal Nanoparticles for Improved Catalysts

Progress in Biomass Electro‐Valorization for Paired Electrosynthesis of Valuable Chemicals and Fuels

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