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

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 mgIn–1$mg_{{\rm{In}}}^{--1}$, which is nearly 39 folds higher than that of commercial In (160.7 µmol h‐1 mgIn–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.

Bifunctional BiPd Alloy Particles Anchored on Carbon Matrix for Reversible Zn–CO2 Battery

“…As far as the CO 2 RR-to-formate process is concerned, several pure metals (such as In, Bi, and Sn) based catalysts achieved preferably FE formate . , Unfortunately, these aforementioned non-noble metals are insufficient to drive FAO performance, which is essential to the charging process of the Zn–CO 2 battery system. The target catalyst design should consider catalyzing CO 2 RR (discharging process) and FAO (charging process) simultaneously.…”

Defect engineering of two-dimensional materials for advanced energy conversion and storage

“…Affected by the binding state of intermediates, various reduction products can be synthesized, such as CO, HCOOH, CH 4 , HCHO, CH 3 OH, C 2 H 4 , C 2 H 5 OH, and n -C 3 H 7 OH. 316–324 From a thermodynamic view, the CO 2 RR is kinetically sluggish with a large overpotential owing to the extremely high stability of CO 2 molecules and multiple electron transfer processes. 325–328 Therefore, rational electrocatalyst design is necessary to reduce the overpotential and extra energy input for enhanced conversion efficiency.…”

Electrocatalytic Reduction of Carbon Dioxide to High-Value Multicarbon Products with Metal–Organic Frameworks and Their Derived Materials

“…The heavy reliance of anthropogenic activities and industrialization on fossil fuels has dramatically increased the concentrations of atmospheric greenhouse gases, especially carbon dioxide (CO 2 ). − Growing concern in the areas of global warming, extreme weather, climate change, and energy crisis is driving research on efficient CO 2 conversion to achieve carbon neutrality. − Given the advantage of being able to be powered by renewable electricity, the electrocatalytic CO 2 reduction reaction (CO 2 RR) has emerged as one of the most promising and sustainable methods to convert CO 2 to valuable chemicals and fuels, especially highly valuable multicarbon (C 2+ ) products like ethylene (C 2 H 4 ), acetic acid (CH 3 COOH), ethanol (C 2 H 5 OH), and n-propanol ( n -C 3 H 7 OH). − Among various types of electrocatalysts, copper (Cu)-based materials exhibited the most efficient electrochemical CO 2 conversion toward C 2+ products. − To date, great effort, such as composition regulation, − morphology adjustment, , defect control, − strain modulation, , and phase engineering, − has been devoted to modulating Cu-based electrocatalysts to boost the C 2+ production in CO 2 RR. However, due to the multiple electron-transfer processes and competitive reactions, it is still challenging to regulate the CO 2 RR reaction pathway toward C 2+ products. − Meanwhile, most CO 2 RR electrocatalysts still demonstrate inferior activity, poor selectivity and low stability that limit the industry-scale applications. − Hence, it is critically important to explore novel high-performance CO 2 RR electrocatalysts to efficiently convert CO 2 molecules to C 2+ products.…”