Core–Shell Pt@Ir Nanothorns on Carbon Fiber Paper Electrodes for Carboxylic Acid Valorization via Kolbe Electrolysis

Yuan, Gang; Wang, Li; Zhang, Xiangwen; Luque, Rafael; Wang, Qingfa

doi:10.1021/acssuschemeng.9b05045

Cited by 17 publications

(20 citation statements)

References 27 publications

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“…Pt@Ir showed a significantly higher yield for hydrocarbon production than the reference commercial Pt/C catalyst. A self-supporting Pt@Ir NT catalyst with core-shell structure was also synthesized by controllable electrodeposition of Pt NT followed by the galvanic deposition of Ir on its surface in aqueous solutions, directly used as anode for the conversion of octanoate to hydrocarbons, in particular C7 hydrocarbons [248].…”

Section: Two-dimension and Carbonaceous Materialsmentioning

confidence: 99%

Support–Activity Relationship in Heterogeneous Catalysis for Biomass Valorization and Fine-Chemicals Production

et al. 2021

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Heterogeneous catalysts are progressively expanding their field of application, from high-throughput reactions for traditional industrial chemistry with production volumes reaching millions of tons per year, a sector in which they are key players, to more niche applications for the production of fine chemicals. These novel applications require a progressive utilization reduction of fossil feedstocks, in favor of renewable ones. Biomasses are the most accessible source of organic precursors, having as advantage their low cost and even distribution across the globe. Unfortunately, they are intrinsically inhomogeneous in nature and their efficient exploitation requires novel catalysts. In this process, an accurate design of the active phase performing the reaction is important; nevertheless, we are often neglecting the importance of the support in guaranteeing stable performances and improving catalytic activity. This review has the goal of gathering and highlighting the cases in which the supports (either derived or not from biomass wastes) share the worth of performing the catalysis with the active phase, for those reactions involving the synthesis of fine chemicals starting from biomasses as feedstocks.

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Section: Two-dimension and Carbonaceous Materialsmentioning

confidence: 99%

Support–Activity Relationship in Heterogeneous Catalysis for Biomass Valorization and Fine-Chemicals Production

et al. 2021

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“…Proposed individual steps such as lyocell fiber (LF) preparation, , cellulose carbonization, , and electrochemical deposition on the CF have been studied for a long time; − however, the combined fabrication process should consider more exquisite conditions to obtain the high-performance CF/metal NP micro/nanostructure. First, higher cellulose contents in the lyocell-based fiber precursor should be required to trigger higher mechanical strength.…”

Section: Introductionmentioning

confidence: 99%

“…Some studies demonstrated the method to fabricate CF from high-crystalline LFs; ,, however, a rare study was performed to measure the mechanical strength of the lyocell-based CF, compared to other cellulose-based ones. Although electrochemical deposition of metal NPs was conducted on the CF surface, most studies focused on electrochemical performance and particle formation. − …”

Section: Introductionmentioning

confidence: 99%

Gold Nanoparticle/Carbon Fiber Hybrid Structure from the Eco-Friendly and Energy-Efficient Process for Electrochemical Biosensing

Lim

Won

Nam

et al. 2022

ACS Sustainable Chem. Eng.

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The carbon fiber/metal nanoparticle hybrid structure is a widely studied material combination for various fields such as energy storage, highperformance composites, and biomedical tools. The versatile carbon fiber/gold nanoparticle structure was prepared using an eco-friendly and energy-efficient fabrication process to address the sustainability issue. First, cellulose fiber was prepared by an eco-friendly lyocell process. The study obtained high mechanical strength of the lyocell fiber through high cellulose contents, strict pulp dissolution conditions, modified spinning, and thermal elongation processes. Then, the lyocell fiber was changed to carbon fiber with stabilization under 5% tension and carbonization, resulting in high mechanical strength and Young's modulus. Finally, gold nanoparticles were electrochemically deposited on the lyocell-based carbon fiber surface. The electrochemical properties of the carbon fiber/gold nanoparticle system were drastically improved due to the high surface area of the nanostructured gold particles. Enhanced electrochemical property and biocompatibility from non-toxic material selection enabled the carbon fiber/gold nanoparticles for dopamine detection, a representative electrochemical biosensor. The detection result demonstrated that the hybrid structure provided high sensitivity and selectivity for dopamine sensing. Overall, this fabrication strategy opens up numerous application opportunities to address eco-friendly and sustainable development requirements.

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“…The oxygen revolution reaction (OER, not shown) is the major side reaction that occurs during Kolbe electrolysis at the anode under aqueous conditions, while it is suppressed under anhydrous conditions. 19,24 Pt (in oxidized form under operating conditions) is the most widely studied anode for Kolbe electrolysis, and other noble metal oxides like IrO2, RuO2, and graphene have also been shown to be active for this reaction 16,18,[25][26][27] .…”

mentioning

confidence: 99%

Understanding the reaction mechanism of Kolbe electrolysis on Pt anodes

Liu

Govindarajan

Prats

et al. 2021

Preprint

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Kolbe electrolysis has been proposed an efficient electrooxidation process to synthesize (un)symmetrical dimers from biomass-based carboxylic acids. However, the reaction mechanism of Kolbe electrolysis remains controversial. In this work, we develop a DFT- based microkinetic model to study the reaction mechanism of Kolbe electrolysis of acetic acid (CH3COOH) on both pristine and partially oxidized Pt anodes. We show that the shift in the rate-determining step of oxygen evolution reaction (OER) on Pt(111)@α-PtO2 surface from OH* formation to H2O adsorption gives rise to the large Tafel slopes, i.e., the inflection zones, observed at high anodic potentials in experiments on Pt anodes. The activity passivation as a result of the inflection zone is further exacerbated in the presence of Kolbe species (i.e., CH3COO* and CH3*). Our simulations find the CH3COO* decarboxylation and CH3* dimerization steps determine the activity of Kolbe reaction during inflection zone. In contrast to the Pt(111)@α-PtO2 surface, Pt(111) shows no activity towards Kolbe products as the CH3COO* decarboxylation step is limiting throughout the considered potential range. This work resolves major controversies in the mechanistic analyses of Kolbe electrolysis on Pt anodes: the origin of the inflection zone, and the identity of the rate limiting step.

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Core–Shell Pt@Ir Nanothorns on Carbon Fiber Paper Electrodes for Carboxylic Acid Valorization via Kolbe Electrolysis

Cited by 17 publications

References 27 publications

Support–Activity Relationship in Heterogeneous Catalysis for Biomass Valorization and Fine-Chemicals Production

Support–Activity Relationship in Heterogeneous Catalysis for Biomass Valorization and Fine-Chemicals Production

Gold Nanoparticle/Carbon Fiber Hybrid Structure from the Eco-Friendly and Energy-Efficient Process for Electrochemical Biosensing

Understanding the reaction mechanism of Kolbe electrolysis on Pt anodes

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