Efficient electroreduction of carbonyl compounds to alcohols over Fe/Fe2O3 interfaces

IF 42.8 1区化学 Q1 CHEMISTRY, PHYSICAL

Nature Catalysis Pub Date : 2025-04-02 DOI:10.1038/s41929-025-01316-7

Jin Lin, Zhenpeng Liu, Haofei Wu, Zhiqi Wang, Guangqiu Wang, Ju Bu, Yanan Wang, Pan Liu, Junjie Wang, Jian Zhang

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Abstract

Catalytic hydrogenation of carbonyl compounds is widely used in chemical manufacturing and biomass refining, but current thermocatalytic processes require elevated temperatures, high-pressure H₂ and expensive catalysts. Here we demonstrate an electroreduction of carbonyl compounds over Fe/Fe₂O₃ interfaces in Fe/Fe₂O₃ nanoarrays (Fe/Fe₂O₃ NAs), where Fe and Fe₂O₃ species synergistically accelerate the kinetics of acetone hydrogenation by promoting acetone adsorption and H* formation. With acetone as the probe molecule, an isopropanol partial current density of 1.6 A cm⁻² and ~100% selectivity are achieved in 1 M KOH aqueous solution. Even in a large-scale, two-electrode electrolyser, Fe/Fe₂O₃ NAs stably deliver an acetone conversion of >99%, an isopropanol selectivity of 100%, and an isopropanol production rate of 21.6 g g_cat⁻¹ h⁻¹ at 0.2 A cm⁻² over a 1,000-h operation. Moreover, Fe/Fe₂O₃ NAs were applied in the electrochemical hydrogenation of various carbonyl compounds to corresponding alcohols with high conversion rates and selectivities.

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羰基化合物在Fe/Fe2O3界面上高效电还原为醇

羰基化合物的催化加氢广泛应用于化工制造和生物质精炼，但目前的热催化工艺需要高温、高压H2和昂贵的催化剂。在Fe/Fe2O3纳米阵列（Fe/Fe2O3 NAs）中，羰基化合物在Fe/Fe2O3界面上电还原，其中Fe和Fe2O3物质通过促进丙酮吸附和H*形成协同加速丙酮加氢动力学。以丙酮为探针分子，在1 M KOH水溶液中，异丙醇的偏电流密度为1.6 A cm−2，选择性为~100%。即使在大型双电极电解槽中，Fe/Fe2O3 NAs也能稳定地提供99%的丙酮转化率，100%的异丙醇选择性，以及在0.2 a cm−2下超过1000小时的异丙醇产率为21.6 g gcat−1 h−1。此外，Fe/Fe2O3 NAs应用于各种羰基化合物的电化学加氢反应，具有较高的转化率和选择性。

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.