Toward a mechanistic understanding of electrocatalytic nanocarbon

Abstract

Electrocatalytic nanocarbon (EN) is a class of material receiving intense interest as a potential replacement for expensive, metal-based electrocatalysts for energy conversion and chemical production applications. The further development of EN will require an intricate knowledge of its catalytic behaviors, however, the true nature of their electrocatalytic activity remains elusive. This review highlights work that contributed valuable knowledge in the elucidation of EN catalytic mechanisms. Experimental evidence from spectroscopic studies and well-defined molecular models, along with the survey of computational studies, is summarized to document our current mechanistic understanding of EN-catalyzed oxygen, carbon dioxide and nitrogen electrochemistry. We hope this review will inspire future development of synthetic methods and in situ spectroscopic tools to make and study well-defined EN structures.

Strong Electronic Coupling of Graphene Nanoribbons onto Basal Plane of a Glassy Carbon Electrode

“…Graphitic nanocarbon materials have recently been recognized as promising electrocatalysts for a range of useful transformations, such as the reduction of dioxygen to water, dinitrogen to ammonia, and carbon dioxide to methanol. − The success of these electrode materials is attributed to the high electronic conductivity of graphitic carbon, the high surface area of nanocarbon electrodes made using template-directed pyrolysis, and the presence of reactive catalytic functional groups obtained by heteroatom doping of otherwise chemically inert carbon framework. Further progress in the field requires the synthesis of nanocarbon electrodes with complex multinuclear catalytic motifs that go beyond “single-atom catalysts.” Unfortunately, the introduction of such well-defined catalytic functionalities is limited by the extreme temperatures required to graphitize carbon precursors, at which most functional groups undergo decomposition.…”

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO2 electroreduction

“…The electrocatalytic nanocarbon thus plays a significant role that should not be ignored. 121 Furthermore, SACs derived from MOFs or COFs can adsorb CO 2 gas due to their porous nature, which affects the reaction results. 58 To sum up, research on active molecular models is very important, but this should not be the sole point by which to evaluate a catalytic system.…”

“…122 Specically, tting the results from Fourier-transform EXAFS (FT-EXAFS) can help to infer the interatomic distances between the absorber and scattering atoms and coordination numbers. 121,122 Fig. 6a shows the different valence states of two Cu-N-C catalysts prepared at different pyrolysis temperatures and a comparison of their Cu Kedge XANES spectra with reference samples.…”

Mesoporous S,N-Codoped Carbon/CoxSy Hybrid Catalyst for Efficient Bifunctional Oxygen Electrocatalysis in Rechargeable Zn–Air Batteries

“…Nanoporous carbon materials, especially mesoporous carbon, have become robust candidates due to the eye-catching advantages of the high conductivity, wide raw material sources, low price, and designed nanoarchitecture . Unfortunately, the intrinsic activity of pure carbon electrocatalysts is still too low to meet the performance requirements of air electrodes .…”