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Transient Solid-State Laser Activation of Indium for High-Performance Reduction of CO 2 to Formate
Ist Teil von
Small (Weinheim an der Bergstrasse, Germany), 2022-06, Vol.18 (24), p.e2201311
Ort / Verlag
Germany
Erscheinungsjahr
2022
Quelle
Wiley Online Library
Beschreibungen/Notizen
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 CO
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
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
, which is nearly 39 folds higher than that of commercial In (160.7 µmol h
), outperforming most of the previous results that have been reported under KHCO
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.