Transient Solid‐State Laser Activation of Indium for High‐Performance Reduction of CO2 to Formate. Issue 24 (13th May 2022) - Guo, Weihua
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 m g In – 1 $mg_{{\rm{In}}}^{--1}$, which is nearly 39 folds higher than that of commercial In (160.7 µmol h ‐1 m g In – 1 $mg_{{\rm{In}}}^{--1}$ ), 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. Abstract : Transient solid‐state laser induction of metal salts can produce highly defective and undercoordinated indium nanoparticles (L‐In) with a high density of vacancies, self‐interstitial defects, and stacking faults, which deliver industrially‐relevant current densities and formate production with low overpotentials and high formate selectivity.