Bifunctional Pt/Au Janus electrocatalysts for simultaneous oxidation/reduction of furfural with bipolar electrochemistry

Ketkaew, Marisa; Assavapanumat, Sunpet; Klinyod, Sorasak; Kuhn, Alexander; Wattanakit, Chularat

doi:10.1039/d1cc06759a

Cited by 19 publications

(15 citation statements)

References 33 publications

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“…Cu is the only metal that is highly selective towards both furfuryl alcohol and 2-methyl furan at different acidic conditions. [5][6][7][8][9][10][11][12][13][14] The past decade has witnessed great progress in exploring furfural reduction over different metal electrodes, and the major products reported in previous studies are summarized in Figure 1.…”

Section: Introductionmentioning

confidence: 99%

“…Furfuryl alcohol and pinacols, e.g., hydrofuroin are the most common products, while 2-methyl furan and tetrahydrofurfuryl alcohol are only selectively produced on limited metals at very acidic conditions [5][6][7][8][9][10][11][12][13][14] . In particular, copper shows potential as a multi-selective electrocatalyst for furfural reduction, as it is able to produce both FAL, a precursor to polymers and resin 15 , and 2-MF, a well-known alternative drop-in biofuel 16 , with nearly 100% selectivity at moderate potentials (ca.…”

Section: Introductionmentioning

confidence: 99%

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Unraveling the reaction mechanisms for furfural electroreduction on copper

Liu

Mukadam

Scott

et al. 2023

Preprint

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Electrochemical routes for the valorization of biomass-derived feedstock molecules offer sustainable pathways to produce chemicals and fuels. However, the underlying reaction mechanisms for their electrochemical conversion remain elusive. In particular, the exact role of proton-electron coupled transfer and electrocatalytic hydrogenation in the reaction mechanisms for biomass electroreduction are disputed. In this work, we study the reaction mechanism underlying the electroreduction of furfural, an important biomass-derived platform chemical, combining grand-canonical (constant-potential) density functional theory -based microkinetic simulations and pH dependent experiments on Cu under acidic conditions. Our simulations indicate the second PCET step in the reaction pathway to be the rate- and selectivity-determining for the production of the two main products of furfural electroreduction on Cu, furfuryl alcohol and 2-methyl furan, at moderate overpotentials. We further identify the source of Cu’s ability to produce both products with comparable activity in their nearly equal activation energies. Furthermore, our microkinetic simulations suggest that surface hydrogenation steps play a minor role in determining the overall activity of furfural electroreduction compared to PCET steps due to the low steady-state hydrogen coverage predicted under reaction conditions, the high activation barriers for surface hydrogenation and the observed pH dependence of the reaction.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Unraveling the reaction mechanisms for furfural electroreduction on copper

Liu

Mukadam

Scott

et al. 2023

Preprint

View full text Add to dashboard Cite

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“…The concept of bipolar electrochemistry has been adapted for metals electrodeposition on carbon substrates, [21][22][23][24] (Bio)electroanalysis, [25] electrocatalysis, [26][27] bioelectrocatalysis, [28] and electrosynthesis of various organic, inorganic, [29] and polymeric [30] materials. So far, bipolar electrochemistry has never been adapted for mercury depollution purposes.…”

Section: Introductionmentioning

confidence: 99%

Efficient Removal of Mercury from Polluted Aqueous Solutions Using the Wireless Bipolar Electrochemistry Technique

Fattah

2022

ChemistryOpen

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Mercury represents one of the major toxic pollutants in water that affect human and ecosystem. Extensive efforts have been globally invested to remove mercury using various chemical and electrochemical approaches. In this study, I propose the use of bipolar electrochemistry for the first time for mercury depollution process. Mercury(II) is removed from aqueous solutions by direct electrodeposition on millimeter scale graphite rods held in a bipolar setup. By adjusting the strength of the applied electric field and the number of the graphite rods the efficiency of the system can be controlled. This wireless technique allows the use of multiple graphite rod arrays within the bulk cell which resulted in high removal efficiency (98 %) of Hg 2 + ions from the polluted solution. The method is straightforward, green, and efficient. The concept can be adapted to remove other heavy metal ions or electrochemically active contaminants from polluted water as long as their reduction potentials are within the water stability window.

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“…The wireless bipolar electrode (BPE) is a kind of wireless electrode or array , that is polarized by driving electrodes to produce a cathode and anode with Faraday reactions at both ends. After development for more than two decades, it has a wide range of applications in metal corrosion, − bioanalysis, − electroanalysis, − synthesis of functional materials, − and nanomotors. − …”

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confidence: 99%

Monitoring Bipolar Electrochemistry and Hydrogen Evolution Reaction of a Single Gold Microparticle under Sub-Micropipette Confinement

et al. 2023

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Herein, an approach to track the process of autorepeating bipolar reactions and hydrogen evolution reaction (HER) on a micro gold bipolar electrode (BPE) is established. Once blocking the channel of the sub-micropipette tip, the formed gold microparticle is polarized into the wireless BPE, which induces the dissolution of the gold at the anode and the HER at the cathode. The current response shows a periodic behavior with three regions: the bubble generation region (I), the bubble rupture/generation region (II), and the channel opening region (III). After a stable low baseline current of region I, a series of positive spike signals caused by single H2 nanobubbles rupture/generation are recorded standing for the beginning of region II. Meanwhile, the dissolution of the gold blocking at the orifice will create a new channel, increasing the baseline current for region III, where the synthesis of gold occurs again, resulting in another periodic response. Finite element simulations are applied to unveil the mechanism thermodynamically. In addition, the integral charge of the H2 nanobubbles in region II corresponds to the consumption of the anode gold. It simultaneously monitors autorepeating bipolar reactions of a single gold microparticle and HER of a single H2 nanobubble electrochemically, which reveals an insightful physicochemical mechanism in nanoscale confinement and makes the glass nanopore an ideal candidate to further reveal the heterogeneity of catalytic capability at the single particle level.

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Bifunctional Pt/Au Janus electrocatalysts for simultaneous oxidation/reduction of furfural with bipolar electrochemistry

Abstract: The sustainable conversion of biomass-derived compounds into high added-value products is a very important contemporary scientific challenge. In this context, we report here the simultaneous electro-oxidation/-reduction of a biomass-derived compound...

Cited by 19 publications

References 33 publications

Unraveling the reaction mechanisms for furfural electroreduction on copper

Unraveling the reaction mechanisms for furfural electroreduction on copper

Efficient Removal of Mercury from Polluted Aqueous Solutions Using the Wireless Bipolar Electrochemistry Technique

Monitoring Bipolar Electrochemistry and Hydrogen Evolution Reaction of a Single Gold Microparticle under Sub-Micropipette Confinement

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