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The development of efficient carbon dioxide reduction reaction (CO2RR) catalysts is one of the practical solutions to the current environmental problems. Usually, metal-doped catalysts are used for the CO2RR, but the metal elements can easily aggregate, resulting in a reduction in the catalytic performance. In this study, NiFe-LDH was exfoliated to single layer by a solid-phase exfoliation strategy, wherein Ni and Fe were doped on the char material owing to the pyrolysis of the solid-phase exfoliation agent, and the NiFe-CN catalyst with a gauzy and porous structure was obtained. The catalyst possessed excellent catalytic performance; particularly, when the mass fraction of NiFe-LDH was 1 wt%, the prepared catalyst (NiFe-CN-1) showed a faradaic efficiency of 93.5% for the reduction of CO2 to CO at −0.8 V (vs. reversible hydrogen electrode (RHE)) with a CO current density of 10.4 mA cm−2, which was due to the sufficient exposure of active sites and efficient proton transfer channels of NiFe-CN. This strategy provides a new idea to easily mass produce CO2RR electrocatalysts in an environmentally benign way. [ABSTRACT FROM AUTHOR]

In recent decades, significant progress has been achieved in rational developments of electrocatalysts through constructing novel atomistic structures and modulating catalytic surface topography, realizing substantial enhancement in electrocatalytic activities. Numerous advanced catalysts were developed for electrochemical energy conversion, exhibiting low overpotential, high intrinsic activity, and selectivity. Yet, maintaining the high catalytic performance under working conditions with high polarization and vigorous microkinetics that induce intensive degradation of surface nanostructures presents a significant challenge for commercial applications. Recently, advanced operando and computational techniques have provided comprehensive mechanistic insights into the degradation of surficial functional structures. Additionally, various innovative strategies have been devised and proven effective in sustaining electrocatalytic activity under harsh operating conditions. This review aims to discuss the most recent understanding of the degradation microkinetics of catalysts across an entire range of anodic to cathodic polarizations, encompassing processes such as oxygen evolution and reduction, hydrogen reduction, and carbon dioxide reduction. Subsequently, innovative strategies adopted to stabilize the materials' structure and activity are highlighted with an in-depth discussion of the underlying rationale. Finally, we present conclusions and perspectives regarding future research and development. By identifying the research gaps, this review aims to inspire further exploration of surface degradation mechanisms and rational design of durable electrocatalysts, ultimately contributing to the large-scale utilization of electroconversion technologies. [ABSTRACT FROM AUTHOR]

The design of highly stable, effective, and selective electrocatalysts is essential for electrochemical reduction of carbon dioxide (CO2). Here, on the basis of density functional theory (DFT) computations, the reaction mechanisms of the reduction of CO2 over a series of bis(iminothiolato)metal (TMIT, TM = Mn, Fe, Co, Ni, Cu, Ru, Rh, and Pd) were studied. It is found that the CO2RR activity of TMIT depends on the choice of the central metal atom. Our results demonstrated that HCOOH is the main product for TMIT (TM = Mn, Fe, Co, Ni, Cu, Pd). Among them, MnIT and FeIT are promising CO2RR catalysts for the HCOOH production due to the good selectivity and catalytic activity with the low overpotential of 0.34 V and 0.35 V, respectively. For RuIT and RhIT, the main product is CO, and the strong adsorption of CO on the catalyst surfaces would poison the catalysts. This makes RhIT and RuIT not good CO2RR catalysts. We anticipate that this work may shed new light on the development of high-performance metal organic framework (MOF)-based electrocatalysts. [ABSTRACT FROM AUTHOR]

It is of paramount importance to design and develop highly active and selective electrocatalysts for the CO2 reduction reaction. Herein, we obtained bismuth-based catalysts consisting of oxidized Bi2O2CO3 and metallic Bi featuring local shortened inter-layer Bi–Bi bonds from in situ reduction of bismuth oxyiodide (BiOI) microflowers, which showed over 90% formate faradaic efficiency in a wide negative potential region. [ABSTRACT FROM AUTHOR]