Rediscovering Forgotten Members of the Graphene Family

López‐Salas, Nieves; Kossmann, Janina; Antonietti, Markus

doi:10.1021/accountsmr.0c00011

Cited by 18 publications

(18 citation statements)

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“…The chemistry of carbon suboxide and the polymer is largely forgotten; however, in our group we have recently developed a new facile synthesis and investigated the semiconducting properties of the polymer. 47 Poly(carbon suboxide) is an extremely versatile platform which can be used as such (as organic semiconductor) and perhaps serve for the synthesis of low-temperatures carbonaceous structures with defined chemical composition. For instance, it has already been shown that the polymer can thermally decompose through pure decarboxylation releasing only CO 2 or a mixture of CO 2 and CO. 48 This can produce different but well-controlled OFG in carbonaceous structures.…”

Section: Bottom-up Synthesis Of Oxygen-containing Carbonsmentioning

confidence: 99%

“We Are Here!” Oxygen Functional Groups in Carbons for Electrochemical Applications

2022

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Heteroatom doping of carbon networks may introduce active functional groups on the surface of the material, induce electron density changes that alter the polarity of the carbon surface, promote the formation of binding sites for molecules or ions, or make the surface catalytically active for different reactions, among many other alterations. Thus, it is no surprise that heteroatom doping has become a well-established strategy to enhance the performance of carbon-based materials for applications ranging from water remediation and gas sorption to energy storage and conversion. Although oxygen functionalization is sometimes inevitable (i.e., many carbon precursors contain oxygen functionalities), its participation in carbon materials performance is often overlooked on behalf of other heteroatoms (mainly nitrogen). In this Mini-review, we summarize recent and relevant publications on the effect that oxygen functionalization has on carbonaceous materials performance in different electrochemical applications and some strategies to introduce such functionalization purposely. Our aim is to revert the current tendency to overlook it and raise the attention of the materials science community on the benefits of using oxygen functionalization in many state-of-the-art applications.

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Section: Bottom-up Synthesis Of Oxygen-containing Carbonsmentioning

confidence: 99%

“We Are Here!” Oxygen Functional Groups in Carbons for Electrochemical Applications

2022

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“… , As shown by carbon nitride (C 3 N 4 ), covalent triazine-based frameworks (CTFs), imine-based covalent-organic frameworks, or poly(heptazine imides)-based frameworks, CN frameworks are known to be very chemically stable. − Furthermore, the high flexibility in building π-extended structures and combining different types of redox moieties is key to tune their electrochemical properties. ,, Taking these advantages, the archetype of anionic/cationic co-redox was demonstrated by using CTF-1, which is composed of the benzene rings as the anionic-redox moiety and the triazine rings as the cationic-redox moiety (Figure ). CN frameworks are also well-known for their very interesting electron-transfer-related functions. − As it was pointed out by a recent review, CN frameworks have quite a rich history; however, this field is still growing, for instance, recent successful preparation of graphdiyne, or new C x N y X z (X = B, F, S, etc.) materials .…”

Section: D π-Conjugated Framework As a Model Electrode Systemmentioning

confidence: 99%

Two-Dimensional π-Conjugated Frameworks as a Model System to Unveil a Multielectron-Transfer-Based Energy Storage Mechanism

Sakaushi

Nishihara

2021

Acc. Chem. Res.

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Metrics & MoreArticle Recommendations CONSPECTUS: Although electrochemical energy storage is commonplace in our society, further advancements in this technology are indispensable for the transition to a low-carbon society. Recent intensive research has expanded concepts in this field; however, finding one suitable material to obtain a high energy density accomplishing the criteria of next-generation batteries is still a conundrum. To solve this issue, material investigations based on big data combined with artificial intelligence are a present trend. On the contrary, this Account focuses on an alternative approach, i.e., fundamental research to shed light on key basic principles to design new electrode materials and new principles achieving multielectron transfer, which is a key to improve a specific capacity. In addition to the cation-redox mechanism, materials showing the multielectron-transfer mechanism based on cation-/anion-redox can enrich material choices with high theoretical energy densities. The challenge in this mechanism is that a rational design of electrode materials based on microscopic understanding of underlying electrode processes has not been fully achieved so far. This is a key bottleneck in machine-learning approaches as well because the reliability of outputs from an algorithm is dependent on the reliability of data from a corresponding microscopic electrode process. Therefore, uncovering fundamental mechanisms in electrochemical energy storage remains one of the primary goals for the present research. In our series of investigations, we developed concepts for replacing complex practical electrode materials, such as polyanion or Li-rich layered oxides, by simplified model systems based on two-dimensional (2D) π-conjugated frameworks, which are based on purely organic aromatic systems and metal-containing coordination polymers. These materials are relatively simple, but it is still possible to control their complexity of systems in order to mimic certain aspects of structure−property relations in practical electrode materials. In particular, recent studies have shown that we can tune electronic structures of 2D π-conjugated frameworks, which is a key feature to investigate electron-transfer mechanisms, along with the concept of the threefold correlation approach, i.e., the relations in chemical structures, electronic structures, and electrochemical reactions. In this Account, several model studies focusing on microscopic understandings of structure-electrochemical energy storage functions are presented in which we investigate how the structural periodicity and nature of the coordination environment affect their electronic properties and the electrochemical reactions. In particular, we investigate the effects of combinations of linkers and metal ions toward the mechanism of the electrochemical energy storage reaction. We identified few major factors determining the energy storage mechanism of 2D π-conjugated frameworks. Local configurations of coordinate covalent bonding and organic linkers in...

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“…Though synthetic efforts to produce polymeric C 1 N 1 can be found as early as in the 1800s when scientists condensed metal cyanides (i.e., production of paracyan), the advances in technology did not allow then to characterize whether the produced materials were crystalline or had a good photocatalytic response (Lopez-Salas et al, 2020). Surprisingly, despite the potential of C 1 N 1 materials, the amount of reported cases of successful C 1 N 1 syntheses is still very limited.…”

Section: Cn Materials (Cmentioning

confidence: 99%

CxNy: New Carbon Nitride Organic Photocatalysts

López‐Salas

Albero

2021

Front. Mater.

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The search for metal-free and visible light-responsive materials for photocatalytic applications has attracted the interest of not only academics but also the industry in the last decades. Since graphitic carbon nitride (g-C3N4) was first reported as a metal-free photocatalyst, this has been widely investigated in different light-driven reactions. However, the high recombination rate, low electrical conductivity, and lack of photoresponse in most of the visible range have elicited the search for alternatives. In this regard, a broad family of carbon nitride (CxNy) materials was anticipated several decades ago. However, the attention of the researchers in these materials has just been awakened in the last years due to the recent success in the syntheses of some of these materials (i.e., C3N3, C2N, C3N, and C3N5, among others), together with theoretical simulations pointing at the excellent physico-chemical properties (i.e., crystalline structure and chemical morphology, electronic configuration and semiconducting nature, or high refractive index and hardness, among others) and optoelectronic applications of these materials. The performance of CxNy, beyond C3N4, has been barely evaluated in real applications, including energy conversion, storage, and adsorption technologies, and further work must be carried out, especially experimentally, in order to confirm the high expectations raised by simulations and theoretical calculations. Herein, we have summarized the scarce literature related to recent results reporting the synthetic routes, structures, and performance of these materials as photocatalysts. Moreover, the challenges and perspectives at the forefront of this field using CxNy materials are disclosed. We aim to stimulate the research of this new generation of CxNy-based photocatalysts, beyond C3N4, with improved photocatalytic efficiencies by harnessing the striking structural, electronic, and optical properties of this new family of materials.

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Rediscovering Forgotten Members of the Graphene Family

Cited by 18 publications

References 54 publications

“We Are Here!” Oxygen Functional Groups in Carbons for Electrochemical Applications

“We Are Here!” Oxygen Functional Groups in Carbons for Electrochemical Applications

Two-Dimensional π-Conjugated Frameworks as a Model System to Unveil a Multielectron-Transfer-Based Energy Storage Mechanism

CxNy: New Carbon Nitride Organic Photocatalysts

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