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A Pair-Electrosynthesis for Formate at Ultra-Low Voltage Via Coupling of CO₂ Reduction and Formaldehyde Oxidation.

ABSTRACT: Formate can be synthesized electrochemically by CO₂ reduction reaction (CO₂RR) or formaldehyde oxidation reaction (FOR). The CO₂RR approach suffers from kinetic-sluggish oxygen evolution reaction at the anode. To this end, an electrochemical system combining cathodic CO₂RR with anodic FOR was developed, which enables the formate electrosynthesis at ultra-low voltage. Cathodic CO₂RR employing the BiOCl electrode in H-cell exhibited formate Faradaic efficiency (FE) higher than 90% within a wide potential range from - 0.48 to - 1.32 V_RHE. In flow cell, the current density of 100 mA cm^-2 was achieved at - 0.67 V_RHE. The anodic FOR using the Cu₂O electrode displayed a low onset potential of - 0.13 V_RHE and nearly 100% formate and H₂ selectivity from 0.05 to 0.35 V_RHE. The CO₂RR and FOR were constructed in a flow cell through membrane electrode assembly for the electrosynthesis of formate, where the CO₂RR//FOR delivered an enhanced current density of 100 mA cm^-2 at 0.86 V. This work provides a promising pair-electrosynthesis of value-added chemicals with high FE and low energy consumption.

SUBMITTER: Li M

PROVIDER: S-EPMC9626726 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature

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A Pair-Electrosynthesis for Formate at Ultra-Low Voltage Via Coupling of CO2 Reduction and Formaldehyde Oxidation.

Li Mengyu M Wang Tehua T Zhao Weixing W Wang Shuangyin S Zou Yuqin Y

Nano-micro letters 20221101 1

Formate can be synthesized electrochemically by CO2 reduction reaction (CO2RR) or formaldehyde oxidation reaction (FOR). The CO2RR approach suffers from kinetic-sluggish oxygen evolution reaction at the anode. To this end, an electrochemical system combining cathodic CO2RR with anodic FOR was developed, which enables the formate electrosynthesis at ultra-low voltage. Cathodic CO2RR employing the BiOCl electrode in H-cell exhibited formate Fa ...[more]

PMID: 36319899

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Project description:Although apparent light inhibition of leaf day respiration is a widespread reported phenomenon, the mechanisms involved, including utilization of alternate respiratory pathways and substrates and light inhibition of TCA cycle enzymes are under active investigation. Recently, acetate fermentation was highlighted as a key drought survival strategy mediated through protein acetylation and jasmonate signaling. Here, we evaluate the light-dependence of acetate transport and assimilation in Populus trichocarpa trees using the dynamic xylem solution injection (DXSI) method developed here for continuous studies of C1 and C2 organic acid transport and light-dependent metabolism. Over 7 days, 1.0 L of [13C]formate and [13C2]acetate solutions were delivered to the stem base of 2-year old potted poplar trees, while continuous diurnal observations were made in the canopy of CO2, H2O, and isoprene gas exchange together with δ13CO2. Stem base injection of 10 mM [13C2]acetate induced an overall pattern of canopy branch headspace 13CO2 enrichment (δ13CO2 +27‱) with a diurnal structure in δ13CO2 reaching a mid-day minimum followed by a maximum shortly after darkening where δ13CO2 values rapidly increased up to +12‱. In contrast, 50 mM injections of [13C]formate were required to reach similar δ13CO2 enrichment levels in the canopy with δ13CO2 following diurnal patterns of transpiration. Illuminated leaves of detached poplar branches pretreated with 10 mM [13C2]acetate showed lower δ13CO2 (+20‱) compared to leaves treated with 10 mM [13C]formate (+320‱), the opposite pattern observed at the whole plant scale. Following dark/light cycles at the leaf-scale, rapid, strong, and reversible enhancements in headspace δ13CO2 by up to +60‱ were observed in [13C2]acetate-treated leaves which showed enhanced dihydrojasmonic acid and TCA cycle intermediate concentrations. The results are consistent with acetate in the transpiration stream as an effective activator of the jasmonate signaling pathway and respiratory substrate. The shorter lifetime of formate relative to acetate in the transpiration stream suggests rapid formate oxidation to CO2 during transport to the canopy. In contrast, acetate is efficiently transported to the canopy where an increased allocation towards mitochondrial dark respiration occurs at night. The results highlight the potential for an effective integration of acetate into glyoxylate and TCA cycles and the light-inhibition of citrate synthase as a potential regulatory mechanism controlling the diurnal allocation of acetate between anabolic and catabolic processes.

Dataset Information

A Pair-Electrosynthesis for Formate at Ultra-Low Voltage Via Coupling of CO₂ Reduction and Formaldehyde Oxidation.

Publications

A Pair-Electrosynthesis for Formate at Ultra-Low Voltage Via Coupling of CO<sub>2</sub> Reduction and Formaldehyde Oxidation.

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