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      Laser-ablation assisted strain engineering of gold nanoparticles for selective electrochemical CO2 reduction

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      Author(s)
      Zhang, C.
      Zhang, W.
      Karadaş, Ferdi
      Low, J.
      Long, R.
      Liang, C.
      Wang, J.
      Li, Z.
      Xiong, Y.
      Date
      2022-04-19
      Source Title
      Nanoscale
      Electronic ISSN
      2040-3372
      Publisher
      Royal Society of Chemistry
      Volume
      20
      Issue
      14
      Pages
      7702 - 7710
      Language
      English
      Type
      Article
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      Abstract
      Strain engineering can endow versatile functions, such as refining d-band center and inducing lattice mismatch, on catalysts for a specific reaction. To this end, effective strain engineering for introducing strain on the catalyst is highly sought in various catalytic applications. Herein, a facile laser ablation in liquid (LAL) strategy is adopted to synthesize gold nanoparticles (Au NPs) with rich compressive strain (Au-LAL) for electrochemical CO2 reduction. It is demonstrated that the rich compressive strain can greatly promote the electrochemical CO2 reduction performance of Au, achieving a CO partial current density of 24.9 mA cm−2 and a maximum CO faradaic efficiency of 97% at −0.9 V for Au-LAL, while it is only 2.77 mA cm−2 and 16.2% for regular Au nanoparticles (Au-A). As revealed by the in situ Raman characterization and density functional theory calculations, the presence of compressive strain can induce a unique electronic structure change in Au NPs, significantly up-shifting the d-band center of Au. Such a phenomenon can greatly enhance the adsorption strength of Au NPs toward the key intermediate of CO2 reduction (i.e., *COOH). More interestingly, we demonstrate that, an important industrial chemical feedstock, syngas, can be obtained by simply mixing Au-LAL with Au-A in a suitable ratio. This work provides a promising method for introducing strain in metal NPs and demonstrates the important role of strain in tuning the performance and selectivity of catalysts.
      Permalink
      http://hdl.handle.net/11693/111433
      Published Version (Please cite this version)
      https://doi.org/10.1039/D2NR01400A
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