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Efficient electrochemical production of glucaric acid and H₂ via glucose electrolysis.

ABSTRACT: Glucose electrolysis offers a prospect of value-added glucaric acid synthesis and energy-saving hydrogen production from the biomass-based platform molecules. Here we report that nanostructured NiFe oxide (NiFeO_x) and nitride (NiFeN_x) catalysts, synthesized from NiFe layered double hydroxide nanosheet arrays on three-dimensional Ni foams, demonstrate a high activity and selectivity towards anodic glucose oxidation. The electrolytic cell assembled with these two catalysts can deliver 100?mA?cm^-2 at 1.39?V. A faradaic efficiency of 87% and glucaric acid yield of 83% are obtained from the glucose electrolysis, which takes place via a guluronic acid pathway evidenced by in-situ infrared spectroscopy. A rigorous process model combined with a techno-economic analysis shows that the electrochemical reduction of glucose produces glucaric acid at a 54% lower cost than the current chemical approach. This work suggests that glucose electrolysis is an energy-saving and cost-effective approach for H₂ production and biomass valorization.

SUBMITTER: Liu WJ

PROVIDER: S-EPMC6959317 | biostudies-literature | 2020 Jan

REPOSITORIES: biostudies-literature

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Efficient electrochemical production of glucaric acid and H2 via glucose electrolysis.

Liu Wu-Jun WJ Xu Zhuoran Z Zhao Dongting D Pan Xiao-Qiang XQ Li Hong-Chao HC Hu Xiao X Fan Zhi-Yong ZY Wang Wei-Kang WK Zhao Guo-Hua GH Jin Song S Huber George W GW Yu Han-Qing HQ

Nature communications 20200114 1

Glucose electrolysis offers a prospect of value-added glucaric acid synthesis and energy-saving hydrogen production from the biomass-based platform molecules. Here we report that nanostructured NiFe oxide (NiFeOx) and nitride (NiFeNx) catalysts, synthesized from NiFe layered double hydroxide nanosheet arrays on three-dimensional Ni foams, demonstrate a high activity and selectivity towards anodic glucose oxidation. The electrolytic cell assembled with these two catalysts ca ...[more]

PMID: 31937783

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Project description:BackgroundThe biomanufacturing of D-glucaric acid has attracted increasing interest because it is one of the top value-added chemicals produced from biomass. Saccharomyces cerevisiae is regarded as an excellent host for D-glucaric acid production.ResultsThe opi1 gene was knocked out because of its negative regulation on myo-inositol synthesis, which is the limiting step of D-glucaric acid production by S. cerevisiae. We then constructed the biosynthesis pathway of D-glucaric acid in S. cerevisiae INVSc1 opi1Δ and obtained two engineered strains, LGA-1 and LGA-C, producing record-breaking titers of D-glucaric acid: 9.53 ± 0.46 g/L and 11.21 ± 0.63 g/L D-glucaric acid from 30 g/L glucose and 10.8 g/L myo-inositol in fed-batch fermentation mode, respectively. However, LGA-1 was preferable because of its genetic stability and its superior performance in practical applications. There have been no reports on D-glucaric acid production from lignocellulose. Therefore, the biorefinery processes, including separated hydrolysis and fermentation (SHF), simultaneous saccharification and fermentation (SSF) and consolidated bioprocessing (CBP) were investigated and compared. CBP using an artificial microbial consortium composed of Trichoderma reesei (T. reesei) Rut-C30 and S. cerevisiae LGA-1 was found to have relatively high D-glucaric acid titers and yields after 7 d of fermentation, 0.54 ± 0.12 g/L D-glucaric acid from 15 g/L Avicel and 0.45 ± 0.06 g/L D-glucaric acid from 15 g/L steam-exploded corn stover (SECS), respectively. In an attempt to design the microbial consortium for more efficient CBP, the team consisting of T. reesei Rut-C30 and S. cerevisiae LGA-1 was found to be the best, with excellent work distribution and collaboration.ConclusionsTwo engineered S. cerevisiae strains, LGA-1 and LGA-C, with high titers of D-glucaric acid were obtained. This indicated that S. cerevisiae INVSc1 is an excellent host for D-glucaric acid production. Lignocellulose is a preferable substrate over myo-inositol. SHF, SSF, and CBP were studied, and CBP using an artificial microbial consortium of T. reesei Rut-C30 and S. cerevisiae LGA-1 was found to be promising because of its relatively high titer and yield. T. reesei Rut-C30 and S. cerevisiae LGA-1were proven to be the best teammates for CBP. Further work should be done to improve the efficiency of this microbial consortium for D-glucaric acid production from lignocellulose.

Project description:Three imidazole-based hybrid materials, coded as IGOPS, IPS and impyridine@SiO2 nanohybrids, were prepared via the covalent immobilization of N-ligands onto a mesoporous nano-SiO2 matrix for H2 generation from formic acid (FA). BET and HRTEM demonstrated that the immobilization of the imidazole derivative onto SiO2 has a significant effect on the SSA, average pore volume, and particle size distribution. In the context of FA dehydrogenation, their catalytic activity (TONs, TOFs), stability, and reusability were assessed. Additionally, the homologous homogeneous counterparts were evaluated for comparison purposes. Mapping the redox potential of solution Eh vs. SHE revealed that poly-phosphine PP3 plays an essential role in FA dehydrogenation. On the basis of performance and stability, [Fe2+/IGOPS/PP3] demonstrated superior activity compared to other heterogeneous catalysts, producing 9.82 L of gases (VH2 + CO2) with TONs = 31,778, albeit with low recyclability. In contrast, [Fe2+/IPS/PP3] showed the highest stability, retaining considerable performance after three consecutive uses. With VH2 + CO2 = 7.8 L, [Fe2+/impyridine@SiO2/PP3] activity decreased, and it was no longer recyclable. However, the homogeneous equivalent of [Fe2+/impyridine/PP3] was completely inactive. Raman, FT/IR, and UV/Vis spectroscopy demonstrated that the reduced recyclability of [Fe2+/IGOPS/PP3] and [Fe2+/impyridine@SiO2/PP3] nanohybrids is due to the reductive cleavage of their C-O-C bonds during catalysis. An alternative grafting procedure is proposed, applying here to the grafting of IPS, resulting in its higher stability. The accumulation of water derived from substrate's feeding causes the inhibition of catalysis. In the case of [Fe2+-imidazole@SiO2] nanohybrids, simple washing and drying result in their re-activation, overcoming the water inhibition. Thus, the low-cost imidazole-based nanohybrids IGOPS and IPS are capable of forming [Fe2+/IGOPS/PP3] and [Fe2+/IPS/PP3] heterogeneous catalytic systems with high stability and performance for FA dehydrogenation.

Dataset Information

Efficient electrochemical production of glucaric acid and H₂ via glucose electrolysis.

Publications

Efficient electrochemical production of glucaric acid and H<sub>2</sub> via glucose electrolysis.

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