Ni/TiO<sub>2</sub> heterostructures derived from phase separation for enhanced electrocatalysis of hydrogen evolution and biomass oxidative upgrading in anion exchange membrane electrolyzers

Zhang, Geng; Yu, Rui; Zhou, Yuqi; Lu, Wenxian; Cao, Fuyang

doi:10.1039/d3nr02896h

Cited by 11 publications

(2 citation statements)

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“…Moreover, it is necessary to increase the HMF concentration to improve the production efficiency, which has been well achieved in 1 M KOH, but almost all studies performed in 0.1 M KOH are limited to an HMF concentration of 10 mM or lower (Table S1). In addition, the anion exchange membrane (AEM) flow electrolyzer is an important device to construct HMF oxidation. − We found in our previous work that the FDCA yield in an AEM flow cell is always lower than that measured in a typical H-type nonflow cell even when the same HMF oxidation catalyst is used, ,, and the reason has not been well explored. Although development of high-performance catalysts is the main research direction for enhancing the HMF oxidation efficiency to FDCA, the resolution of these abovementioned critical issues is beneficial to increase the FDCA production.…”

Section: Introductionmentioning

confidence: 97%

Critical Practices in Improving the Electrochemical Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in 0.1 M KOH

Fan,

Zhao,

Wang

et al. 2024

ACS Sustainable Chem. Eng.

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The electrochemical oxidation of 5-hydroxymethylfurfural (HMF) is an efficient method to produce 2,5furandicarboxylic acid (FDCA). The moderate alkaline condition (pH ≈ 13) is a compromise between stability concern and catalytic efficiency. Herein, several critical issues are studied to improve the electrochemical oxidation of HMF to FDCA in 0.1 M KOH using NiO as the catalyst. The direct oxidation process of HMF is observed before the formation of Ni 3+ species, which follows an electrochemical reaction mechanism. By increasing the electrode area/electrolyte volume ratio and NiO loading, the reaction potential can be extended to a lower value (1.30 V RHE ) with high FDCA yield (>95%). Moreover, the FDCA yield of 97% is realized at the feeding HMF concentration of 40 mM in 0.1 M KOH by using an anion exchange membrane (AEM) as the separator of H-type electrolyzer in a three-electrode system. In addition, the adsorption of products by the electrolysis system and the compound penetration through the AEM from anolyte to catholyte cannot be ignored in a two-electrode flow cell. The slight decrease of alkali concentration in the catholyte is conducive to decreasing the penetration of products from anolyte to catholyte due to the inhibition of water transfer in the opposite direction in the AEM.

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Section: Introductionmentioning

confidence: 97%

Critical Practices in Improving the Electrochemical Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in 0.1 M KOH

Fan,

Zhao,

Wang

et al. 2024

ACS Sustainable Chem. Eng.

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“…Extensive efforts have been dedicated to optimizing the FDCA yield and Faradaic efficiency using advanced electrocatalyst structures. [22][23][24][25][26][27] Most studies have utilized highly alkaline conditions owing to the nucleophilicity of OH À and availability of earth-abundant catalytic materials, [28][29][30][31][32] but the alkaline environment significantly expedites the side-reaction of polymerization via aldolcondensation, leading to the low-quality FDCA product. [33][34][35] In addition, the separation of FDCA from the electrolytic system demands neutralization from the FDCA salt, which accompanies the formation of saline wastewater that needs additional burden on environmental treatment.…”

Section: Introductionmentioning

confidence: 99%

Ultra‐Dense Supported Ruthenium Oxide Clusters via Directed Ion Exchange for Efficient Valorization of 5‐Hydroxymethylfurfural

Lei,

Chen,

Jiang

et al. 2024

Angew Chem Int Ed

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Maximizing the loading of active centers without aggregation for a supported catalyst is a grand challenge but essential for achieving high gravimetric activity, especially toward multi‐step reactions. The oxidation of 5‐hydroxymethylfurfural (HMF), a key biomass‐derived platform molecule, into 2,5‐furandicarboxylic acid (FDCA), a promising alternative to polyester monomer, is such a multi‐step reaction that involves 6 electron transfers. Herein, we devised a strategy of creating ultra‐dense supported Ru oxide clusters on a Co hydroxyanion (CoHA) support. Pyrimidine ligands were first incorporated into the CoHA interlayers, and their subsequent evacuation created porous channels for the directed ion exchange with the built‐in anions in CoHA, which allows the dense and mono‐disperse functionalization of RuCl62‐ anions and their resulting Ru oxide clusters. These ultra‐dense Ru oxide clusters not only enable high HMF electrooxidation currents under neutral conditions but also create microscopic channels in‐between the clusters for the expedited re‐adsorption and oxidation of intermediates toward highly oxidized product, such as 5‐formyl‐2‐furoic acid (FFCA) and FDCA. A two‐stage HMF oxidation process, consisting of ambient conversion of HMF into FFCA and FFCA oxidation into FDCA under 60 oC, was eventually developed to first achieve a high FDCA yield of 92.1% with significantly reduced polymerization.

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Unlocking Efficient Hydrogen Production: Nucleophilic Oxidation Reactions Coupled with Water Splitting

Wang,

Zheng,

et al. 2024

Advanced Materials

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Electrocatalytic water splitting driven by sustainable energy is a clean and promising water‐chemical fuel conversion technology for the production of high purity green hydrogen. However, the sluggish kinetics of anodic oxygen evolution reaction (OER) pose challenges for large‐scale hydrogen production, limiting its efficiency and safety. Recently, the anodic OER has been replaced by a nucleophilic oxidation reaction (NOR) with biomass as the substrate and coupled with hydrogen evolution reaction (HER), which has attracted great interest. Anode NOR offers faster kinetics, generates high‐value products, and reduces energy consumption. By coupling NOR with hydrogen evolution reaction, hydrogen production efficiency can be enhanced while yielding high‐value oxidation products or degrading pollutants. Therefore, NOR‐coupled HER hydrogen production is another new green electrolytic hydrogen production strategy after electrolytic water hydrogen production, which is of great significance for realizing sustainable energy development and global decarbonization. This review explores the potential of nucleophilic oxidation reactions as an alternative to OER and delves into NOR mechanisms, guiding future research in NOR‐coupled hydrogen production. It assesses different NOR‐coupled production methods, analyzing reaction pathways and catalyst effects. Furthermore, it evaluates the role of electrolyzers in industrialized NOR‐coupled hydrogen production and discusses future prospects and challenges. This comprehensive review aims to advance efficient and economical large‐scale hydrogen production.This article is protected by copyright. All rights reserved

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Ni/TiO₂ heterostructures derived from phase separation for enhanced electrocatalysis of hydrogen evolution and biomass oxidative upgrading in anion exchange membrane electrolyzers

Abstract: The construction of heterostructure is an effective strategy to enhance the electrocatalysis for hydrogen evolution reaction (HER) and biomass oxidative upgrading. Herein, a Ni/TiO2 heterostructure prepared by a phase-separation strategy...

Cited by 11 publications

References 55 publications

Critical Practices in Improving the Electrochemical Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in 0.1 M KOH

Critical Practices in Improving the Electrochemical Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in 0.1 M KOH

Ultra‐Dense Supported Ruthenium Oxide Clusters via Directed Ion Exchange for Efficient Valorization of 5‐Hydroxymethylfurfural

Unlocking Efficient Hydrogen Production: Nucleophilic Oxidation Reactions Coupled with Water Splitting

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Ni/TiO2 heterostructures derived from phase separation for enhanced electrocatalysis of hydrogen evolution and biomass oxidative upgrading in anion exchange membrane electrolyzers

Abstract: The construction of heterostructure is an effective strategy to enhance the electrocatalysis for hydrogen evolution reaction (HER) and biomass oxidative upgrading. Herein, a Ni/TiO2 heterostructure prepared by a phase-separation strategy...

Cited by 11 publications

References 55 publications

Critical Practices in Improving the Electrochemical Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in 0.1 M KOH

Critical Practices in Improving the Electrochemical Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in 0.1 M KOH

Ultra‐Dense Supported Ruthenium Oxide Clusters via Directed Ion Exchange for Efficient Valorization of 5‐Hydroxymethylfurfural

Unlocking Efficient Hydrogen Production: Nucleophilic Oxidation Reactions Coupled with Water Splitting

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Ni/TiO₂ heterostructures derived from phase separation for enhanced electrocatalysis of hydrogen evolution and biomass oxidative upgrading in anion exchange membrane electrolyzers