Transient Solid-State Laser Activation of Indium for High-Performance Reduction of CO2 to Formate

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Detail(s)

Original languageEnglish
Article number2201311
Journal / PublicationSmall
Volume18
Issue number24
Online published13 May 2022
Publication statusPublished - 16 Jun 2022

Abstract

Deficiencies in understanding the local environment of active sites and limited synthetic skills challenge the delivery of industrially-relevant current densities with low overpotentials and high selectivity for CO2 reduction. Here, a transient laser induction of metal salts can stimulate extreme conditions and rapid kinetics to produce defect-rich indium nanoparticles (L-In) is reported. Atomic-resolution microscopy and X-ray absorption disclose the highly defective and undercoordinated local environment in L-In. In a flow cell, L-In shows a very small onset overpotential of ≈92 mV and delivers a current density of ≈360 mA cm-2 with a formate Faradaic efficiency of 98% at a low potential of −0.62 V versus RHE. The formation rate of formate reaches up to 6364.4 µmol h-1 mg–1In, which is nearly 39 folds higher than that of commercial In (160.7 µmol h-1 mg–1In), outperforming most of the previous results that have been reported under KHCO3 environments. Density function theory calculations suggest that the defects facilitate the formation of *OCHO intermediate and stabilize the *HCOOH while inhibiting hydrogen adsorption. This study suggests that transient solid-state laser induction provides a facile and cost-effective approach to form ligand-free and defect-rich materials with tailored activities.

Research Area(s)

  • abundant defects, carbon dioxide reduction reaction, industrial-relevance formate production rate, laser activation, low overpotential

Citation Format(s)