Electrochemical CO2 reduction reaction (CO2RR) to produce value‐added products has received tremendous research attention in recent years. With research efforts across the globe, remarkable advancement has been achieved, including the improvement of selectivity for the reduction products, the realization of efficient reduction beyond two electrons, and the delivery of industrially relevant current densities. In this review, we introduce the recent development of nanomaterials for CO2RR, including the zero‐dimensional graphene quantum dots, two‐dimensional materials such as metal chalcogenides and metal/covalent organic framework, single‐atom catalysts, and nanostructured metal catalysts. The engineering of materials into three‐dimensional structure will also be discussed. Finally, we will provide a summary of the catalytic performance and perspectives on future development.
Recent advances in laser-induced graphene (LIG) for environmental applications are comprehensively reviewed. Challenges and opportunities in solving environmental issues using LIG are discussed.
The incorporation of charged functional groups is effective to modulate the activity of molecular complexes for the CO2 reduction reaction (CO2RR), yet long‐term heterogeneous electrolysis is often hampered by catalyst leaching. Herein, an electrocatalyst of atomically thin, cobalt‐porphyrin‐based, ionic–covalent organic nanosheets (CoTAP‐iCONs) is synthesized via a post‐synthetic modification strategy for high‐performance CO2‐to‐CO conversion. The cationic quaternary ammonium groups not only enable the formation of monolayer nanosheets due to steric hindrance and electrostatic repulsion, but also facilitate the formation of a *COOH intermediate, as suggested by theoretical calculations. Consequently, CoTAP‐iCONs exhibit higher CO2RR activity than other cobalt‐porphyrin‐based structures: an 870% and 480% improvement of CO current densities compared to the monomer and neutral nanosheets, respectively. Additionally, the iCONs structure can accommodate the cationic moieties. In a flow cell, CoTAP‐iCONs attain a very small onset overpotential of 40 mV and a stable total current density of 212 mA cm–2 with CO Faradaic efficiency of >95% at −0.6 V for 11 h. Further coupling the flow electrolyzer with commercial solar cells yields a solar‐to‐CO conversion efficiency of 13.89%. This work indicates that atom‐thin, ionic nanosheets represent a promising structure for achieving both tailored activity and high stability.
Electrochemical CO2 reduction reaction (CO2RR) has received significant research interest in recent years due to its potential to mitigate carbon emissions while providing valuable fuels and chemicals. The performance of...
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.
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