Solar-driven highly selective conversion of glycerol to dihydroxyacetone using surface atom engineered BiVO4 photoanodes

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июнь 28, 2024

Abstract Dihydroxyacetone is the most desired product in glycerol oxidation reaction because of its highest added value and large market demand among all possible products. However, selectively oxidative secondary hydroxyl groups for highly efficient dihydroxyacetone production still poses a challenge. In this study, we engineer surface BiVO 4 by introducing bismuth-rich domains oxygen vacancies (Bi-rich 4-x ) to systematically modulate adsorption enhance photo-induced charge separation photoelectrochemical into conversion. As result, Bi-rich increases photocurrent density from 1.42 4.26 mA cm −2 at 1.23 V vs. reversible hydrogen electrode under AM 1.5 G illumination, as well selectivity 54.0% 80.3%, finally achieving rate 361.9 mmol m h −1 that outperforms reported values. The atom customization opens way regulate solar-driven organic transformation pathway toward carbon chain-balanced product.

Язык: Английский

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Synergistic Lewis and Brønsted Acid Sites Promote OH* Formation and Enhance Formate Selectivity: Towards High‐efficiency Glycerol Valorization

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(14)

Опубликована: Фев. 15, 2024

As a sustainable valorization route, electrochemical glycerol oxidation reaction (GOR) involves in formation of key OH* and selective adsorption/cleavage C-C(O) intermediates with multi-step electron transfer, thus suffering from high potential poor formate selectivity for most non-noble-metal-based electrocatalysts. So, it remains challenging to understand the structure-property relationship as well construct synergistic sites realize high-activity high-selectivity GOR. Herein, we successfully achieve dual-high performance low potentials superior GOR by forming Lewis Brønsted acid Ni-alloyed Co-based spinel. The optimized NiCo oxide solid-acid electrocatalyst exhibits (1.219 V@10 mA/cm

Язык: Английский

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A Solid‐Solution with Asymmetric Ni‐O‐Cr Sites for Boosting Protonation toward Anodic Oxidation

Advanced Energy Materials, Год журнала: 2024, Номер 14(38)

Опубликована: Июль 14, 2024

Abstract Replacing the slow protonation process of oxygen evolution reaction (OER) with fast alcohol electro‐oxidation can decrease driving potentials, thus improving overall efficiency electrochemical devices. However, formation effective catalytic sites for oxidation remains challenging in accelerating to inhibit metal leaching and improve catalyst stability. Herein, asymmetric Ni‐O‐Cr are constructed by alloying Cr into NiO matrix optimize coordination environments, showing significantly enhanced stability during electro‐oxidation. The maintain constant valence states Ni oxidation, efficiently suppressing dissolution even at high potentials. In situ characterizations combined theoretical calculations indicate that adsorption activation OH* molecules compared pure NiO, increasing anodic kinetics. results also smaller gap 3 d ‐O 2 p strengthens charge transfer, leading This work gives insights boosting using sites‐enriched solid‐solution electrocatalysts.

Язык: Английский

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Construction of Ag─Co(OH)₂ Tandem Heterogeneous Electrocatalyst Induced Aldehyde Oxidation and the Co‐Activation of Reactants for Biomass Effective and Multi‐Selective Upgrading

Advanced Materials, Год журнала: 2024, Номер 36(26)

Опубликована: Фев. 8, 2024

Abstract The electrocatalytic oxidation of 5‐hydroxymethylfurfural (HMF) provides a feasible way for utilization biomass resources. However, how to regulate the selective synthesis multiple value‐added products is still great challenge. cobalt‐based compound promising catalyst due its direct and indirect properties, but weak adsorption capacity restricts further development. Herein, by constructing Ag─Co(OH) 2 heterogeneous catalyst, efficient 5‐hydroxymethyl‐2‐furanoic acid (HMFCA) 2,5‐furan dicarboxylic (FDCA) at different potential ranges are realized. Based on various physical characterizations, electrochemical measurements, density functional theory calculations, it proved that addition Ag can effectively promote aldehyde group carboxyl group, then generate HMFCA low potential. Moreover, introduction activate compounds, thus strengthening organic molecules OH − species, promoting formation FDCA. This work achieves two chemicals one tandem deeply analyzes enhancement mechanism which powerful guidance development catalysts.

Язык: Английский

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Molybdenum, tungsten doped cobalt phosphides as efficient catalysts for coproduction of hydrogen and formate by glycerol electrolysis

Journal of Colloid and Interface Science, Год журнала: 2024, Номер 665, С. 152 - 162

Опубликована: Март 19, 2024

Язык: Английский

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