Pt1In单原子合金用于可见光驱动CO2甲酰化苯胺

IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Nano Energy Pub Date : 2025-01-14 DOI:10.1016/j.nanoen.2025.110673
Peng Bai , Jiafa Chen , Yicheng Zhao , Yongdan Li
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引用次数: 0

摘要

二氧化碳甲酰化为将二氧化碳转化为增值化学品提供了一条有前途的途径。该过程通常通过热催化方法和附加还原剂进行,这增加了能耗和系统的复杂性。在此,我们报道了在N,N-二甲基甲酰胺(DMF)溶剂中,在室温下,Pt1In-ZnOx单原子合金催化剂上光催化CO2甲酰化苄胺。通过Pt-In键将Pt单原子锚定在In纳米粒子上,并伴有电子从In到Pt的转移,提高了对可见光的吸收能力和光生载流子的分离效率。此外,还促进了二氧化碳和苄胺在Pt1In单原子合金表面的吸附和活化。在可见光下反应6 h, n -苄基甲酰胺的收率达到48.6 mmol g-1,选择性为95.3%。通过一系列的原位表征和理论计算,提出了一种可能的反应机理。DMF的分解-再生循环参与光催化过程,扩大了反应区域,从而促进了苄胺的甲酰化。该光催化体系具有良好的循环稳定性和通用性。本研究为单原子合金催化剂的合理设计提供了新的思路,为二氧化碳的可持续利用提供了有效途径。
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Pt1In single atom alloy for visible-light-driven CO2 formylation of benzylamine
CO2 formylation of amines provides a promising route to convert CO2 into value-added chemicals. That process is usually performed through a thermo-catalytic approach with additional reducing agents, which increases the energy consumption and the complexity of the system. Herein, we report photocatalytic CO2 formylation of benzylamine over Pt1In-ZnOx single-atom-alloy catalyst at room temperature in N,N-dimethylformamide (DMF) solvent. The anchoring of Pt single atoms onto In nanoparticles through Pt-In bonds accompanied with electron transfer from In to Pt improves the absorption capacity for visible light and the separation efficiency of photogenerated charge carriers. Furthermore, the adsorption and activation of CO2 and benzylamine are promoted on the surface of Pt1In single-atom-alloy. After 6 h reaction under visible-light, the yield of N-benzylformamide reaches 48.6 mmol g−1 with a 95.3 % selectivity. A possible reaction mechanism is proposed based on a series of in situ characterizations and theoretical calculations. A decomposition-regeneration cycle of DMF is involved in the photocatalytic process, which extends the reaction region and thus facilitates the formylation of benzylamine. The photocatalytic system exhibits good cycling stability and universality. This work provides new insights for the rational design of single-atom-alloy catalyst and an efficient approach for the sustainable utilization of CO2.
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来源期刊
Nano Energy
Nano Energy CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
30.30
自引率
7.40%
发文量
1207
审稿时长
23 days
期刊介绍: Nano Energy is a multidisciplinary, rapid-publication forum of original peer-reviewed contributions on the science and engineering of nanomaterials and nanodevices used in all forms of energy harvesting, conversion, storage, utilization and policy. Through its mixture of articles, reviews, communications, research news, and information on key developments, Nano Energy provides a comprehensive coverage of this exciting and dynamic field which joins nanoscience and nanotechnology with energy science. The journal is relevant to all those who are interested in nanomaterials solutions to the energy problem. Nano Energy publishes original experimental and theoretical research on all aspects of energy-related research which utilizes nanomaterials and nanotechnology. Manuscripts of four types are considered: review articles which inform readers of the latest research and advances in energy science; rapid communications which feature exciting research breakthroughs in the field; full-length articles which report comprehensive research developments; and news and opinions which comment on topical issues or express views on the developments in related fields.
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Editorial Board Optimizing interface properties of perylene-diimide-based cathode interlayer material by reducing 2-hydroxyethyl groups to achieve organic solar cells with efficiency over 19% Homogenizing composition to achieve high-performance Mg3Bi2-type thermoelectrics Intensified flow and mass transfer in lithium slurry redox flow batteries enabled by a bionic leafvein flow field Single-crystal Ni-rich layered oxide cathodes with LiNbO3-Li3BO3 coating for sulfide all-solid-state batteries
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