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In this work, we explored a post-synthetic modification of the well-known graphitic carbon nitride (g-CN) by means of an "amorphization" treatment and evaluate the resulting change in photocatalytic activity towards the synthesis of valuable perfluoroalkyl derivatives. The as-prepared "super-amorphous" CN (SACN) exhibits a significant increase of the photocatalytic activity (up to a six-fold enhancement with the optimum structure with respect to g-CN), which originates from the lower degree of crystallinity of the CN and its reduced bandgap. The SACN photocatalysts display versatility and good tolerance towards functional group variations of the reagents, emerging as a potential new benchmark CN structure for heterogeneous organic photocatalysis.

Recently, the field of dual photocatalysis has grown rapidly, to become one of the most powerful tools for the functionalization of organic molecules under mild conditions. In particular, the merging of Earth-abundant nickel-based catalytic systems with visible-light-activated photoredox catalysts has allowed the development of a number of unique green synthetic approaches. This goes in the direction of ensuring an effective and sustainable chemical production, while safeguarding human health and environment. Importantly, this relatively new branch of catalysis has inspired an interdisciplinary stream of research that spans from inorganic and organic chemistry to materials science, thus establishing itself as one dominant trend in modern organic synthesis. This Review aims at illustrating the milestones on the timeline evolution of the photocatalytic systems used, with a critical analysis toward novel applications based on the use of photoactive two-dimensional carbon-based nanostructures. Lastly, forward-looking opportunities within this intriguing research field are discussed.

In this work, the development of a novel efficient heterogeneous catalytic system capable of driving Knoevenagel condensation reactions between benzaldehydes and malononitrile was reported. Specifically, we explored a post-synthetic modification of graphitic carbon nitride (g-CN) through a strong oxidation treatment by acid mixture (HNO3/H2SO4). The as-prepared oxidized CN material (CNO) shows a large number of surface acidic moieties, that can be easily deprotonated through an aqueous alkaline wash with different bases (NaOH, K2CO3, t-BuOK), to introduce a high density of reactive basic sites. The best catalyst is obtained with NaOH as the base (CNO-NaOH), and displays high reactivity and good tolerance towards functional group variations of the reagents, thus emerging as a potential new recyclable carbon nitride-based structure for organic base catalysis.

Visible light-driven production of fuels and value-added chemicals is currently one of the most intensely investigated research topics across various scientific disciplines, due to its potential to ease the World’s dependence on fossil fuels. In this perspective, we recapitulate some of the main features of dye-sensitized photocatalytic systems aimed at solar H2 production, focusing in particular on TiO2-based three-component assemblies with organic sensitizers. Relevant aspects include the structural and electronic properties of the sensitizers, the nature of the semiconductor and the hydrogen evolution catalysts, the role of the sacrificial donor and the effect of the reaction parameters on H2 production rate and stability. Besides presenting the most significant recent developments of the field, we also analyse some of its common practices in terms of experimental design, laboratory procedures and data presentation, trying to highlight their weaknesses and suggesting possible improvements. We then conclude with a short paragraph discussing the possible future development of this exciting research area.

The electrocatalytic CO2 reduction reaction (CO2RR) is an interfacial process, involving a minimum of three phases at the contact point of gaseous CO2 with the electrodic surface and the liquid electrolyte. As a consequence, surface chemistry at composite interfaces plays a central role for CO2RR selectivity and catalysis. Each interface defines a functional boundary, where active sites are exposed to a unique environment, with respect to distal sites in the bulk of organic and inorganic domains. While the individual role of each component-type is hardly predictable "a-solo", the interface ensemble works via a strategic interplay of individual effects, including: (i) enhanced electrical conductivity, (ii) high surface area and exposure of the interfacial catalytic sites, (iii) favorable diffusion and feeding of reactants, (iv) complementary interactions for the "on/off" stabilization of cascade intermediates, (v) a secondary sphere assistance to lower the activation energy of bottleneck steps, (vi) a reinforced robustness and long-term operation stability. Selected CO2RR case studies are compared and contrasted to highlight how the organic domains of carbon nanostructures merge with metal and metal-oxide active sites to separate tasks but also to turn them into a cooperative asset of mutual interactions, thus going beyond the classic "Divide et Impera" rule.

Ceria (CeO2) nanostructures are well-known in catalysis for energy and environmental preservation and remediation. Recently, they have also been gaining momentum for biological applications in virtue of their unique redox properties that make them antioxidant or pro-oxidant, depending on the experimental conditions and ceria nanomorphology. In particular, interest has grown in the use of biotemplates to exert control over ceria morphology and reactivity. However, only a handful of reports exist on the use of specific biomolecules to template ceria nucleation and growth into defined nanostructures. This review focusses on the latest advancements in the area of biomolecular templates for ceria nanostructures and existing opportunities for their (bio)applications.

Practical-scale on-site production of hydrogen peroxide (H2O2) via two-electron (2e(-)) oxygen reduction reaction (ORR) relies on efficient, robust, and selective electrocatalysts. Among them, carbon-based materials are cheap, abundant, durable, and their surface properties can be tuned to favor the 2e(-) ORR pathways, resulting in higher efficiency and facilitating possible scale-up towards commercially appealing levels. Here, we demonstrate that the selective installment of carboxyl groups on the surface of N-doped graphene yielding a material named graphene acid (N-GA) promotes the catalytic 2e(-) ORR, achieving a H2O2 faradaic efficiency (FE) as high as 70 % in acidic media (pH=0.96) and a H2O2 productivity in long term bulk electrolysis that could reach 107.8 mmol g(catalyst)(-1) h(-1) under optimized conditions. Extended XPS analysis and density functional theory (DFT) calculations revealed that surface carboxylic acid functional groups play a significant role in achieving the high activity of N-GA for 2e(-) ORR.

The importance of sensing hydrogen peroxide (H2O2) is due to its ubiquity, being extensively used in industry and also being a biologically relevant side-product of several enzymatic processes. Electrochemical sensing is one of the most robust and simple methods for sensing H2O2 and the discovery of new electroactive materials, particularly at the nanoscale, represents a very hot topic of research. Here, we prove that upon appropriate integration of oxidized single-walled carbon nanohorns (ox-SWCNHs) into a per se moderate H2O2 sensor such as cerium dioxide (CeO2), the sensitivity toward H2O2 is enhanced by almost two orders of magnitude (from 0.4 to 160 μA cm−2 mM−1), on par with that of state-of-the-art metal or metal oxide-based sensors. The modified electrode is also very stable (82% response after 2 weeks of continuous use) and the results highly reproducible. The developed nanohybrid ox-SWCNHs@CeO2, characterized fully and whose average size is about 70 nm as measured by both TEM and AFM, was also tested in real case studies such as washing liquids and milk and was confirmed to be a robust and highly selective material, being not affected neither by the presence of complex matrices, nor by interferents in several organic substrates. The high recovery confirmed the excellent specificity and flexibility of this new electrocatalytic material. Fil: Bracamonte, Maria Victoria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina. University of Trieste; Italia Fil: Melchionna, Michele. University of Trieste; Italia Fil: Giuliani, Angela. University of Trieste; Italia Fil: Nasi, Lucía. CNR-IMEM Institute; Italia Fil: Tavagnacco, Claudio. University of Trieste; Italia Fil: Prato, Maurizio. University of Trieste; Italia. Carbon Nanobiotechnology Laboratory; España. BasqueFdnSci; España Fil: Fornasiero, Paolo. University of Trieste; Italia

Nanostructured gels have emerged as an attractive functional material to innovate the field of energy, with applications ranging from extraction and purification to nanocatalysts with unprecedented performance. In this review we discuss the various classes of nanostructured gels and the most recent advancements in the field with a perspective on future directions of this challenging area.

Electrocatalysis, particularly related to fuel cell applications or other processes related to sustainability, has been steadily advanced by the design of new hierarchical materials involving two or more phases. One particularly appealing type of structure features metal species confined within carbon layers. These materials combine the benefits of the two components, which often work in synergy. However, given the intrinsic catalytic activity of carbon and the fact that the metal may be chemically inaccessible, in many cases, which of the two phases is the truly active site is not fully clear. Particularly for pure core–shell systems, where the metal is completely covered by carbon, the identification of the specific task of each component is not trivial. Many reported works on this type of bi-component catalyst are speculative in this regard. It is important for catalyst development that future studies on these systems will include a thorough cross-check of the reactivity aspects by means of combination of suitable techniques or experiments to unravel probable mechanisms and that assumptions are avoided.

Protein and peptide phosphorylation regulate numerous pathological processes, however, their characterization is challenging due to their low abundance and transient nature. Therefore, nanomaterials are being developed to address this demanding task. In particular, carbon nanostructures are attracting interest as scaffolds for functional nanocomposites, yet only isolated studies exist on the topic, and little is known on the effect of nanocarbon morphology on templating nanocomposites. In this work, we compared oxidized carbon nanotubes, graphene oxide, oxidized carbon nanohorns and oxidized graphitized carbon black, as scaffolds for magnetized nanocomposites. The nanomaterials were extensively characterized with experimental and in silico techniques. Next, they were applied to phosphopeptide enrichment from cancer cell lysates for NanoHPLC-MS/MS, with selectivity as high as nearly 90% and several-thousand identification hits. Overall, new insights emerged for the understanding and the design of nanocomposites for phosphoproteomics.[Figure not available: see fulltext.]

Introduction: “Here comes the sun, and I say it’s alright”. The line from the famous and comforting Beatles’ song sounds like a perfect slogan for today’s crusade toward a more sustainable world. A never-tiring memento that, as long as the Sun shines in the sky, there will always be hope to heal a world suffering from an impressive increase in energetic demand. Sunlight brings a gigantic energy pack, and modern scientists are investing a huge amount of time, resources, and intellectual exercise into best exploiting it. Therefore, the fast-growing number of discoveries on photocatalysis comes as no surprise, and quite obviously they are accompanied by a ballistic number of publications (Figure 1). However, is this latter number truly justified or is the chain of events pining for sustainability and clean energy generating an overpopulation of contributions to the topic? Assuming that all such publications always reach a minimum standard of quality and novelty, the question for now must remain unanswered, because research is an unpredictable animal that can feed from any little fruit. However, a different but relevant question could be possibly answered: is it possible to establish a common protocol, set of rules, that makes all these publications useful for moving forward in a harmonized fashion the knowledge on photocatalysis?

The Oxygen Reduction Reaction (ORR) catalyzed by N-carbon electrocatalyst was investigated, focusing on the fundamental features for the selective H2O2 formation. The electrochemical characterization was primarily performed by the use of the Rotating Ring Disk Electrode (RRDE) tool in both hydrodynamic Linear Sweep Voltammetry (LSV) mode and by Chronoamperometry (CA) measurement. We rationalized the structure/activity relationship, reaching a new state-of-the-art in terms of current density for the H2O2 generation. The study also explored the performance in relation with the electrode deposit procedure that is of fundamental importance to achieve a suitable macroscopic electrode preparation. Furthermore, the electrode implementation in a polymer membrane static flow electrolyzer setup, was evaluated to understand how the material catalytic features such as current ranges and selectivity scale up from a classical three electrode system to a more realistic application-focused environment.

The exceptional and unique properties of cerium dioxide have encouraged scientists to exploit this material beyond its traditional role as a promoter in automotive engines. Electrochemical processes relevant to fuel cells, electrolyzers, and sensors can be facilitated or even directly catalyzed by the CeO2, whose redox properties are ideal for electrochemistry. However, given the insulating nature of pure ceria, the inclusion of conductive materials at the boundary with the metal oxide is necessary to boost the catalytic activity. Carbon in its various forms and morphologies is a dominant component in ceria-based electrocatalysts, significantly facilitating electron transfers and providing high surface area and improved stability. Moreover, given the improved electronic conductivity of reduced CeO2 in the wake of the decreased grain boundary impedance, the combination with a conductive component, such as carbon, can facilitate a reduction of the ceria.

Electrocatalytic oxygen reduction (ORR) is an emerging synthetic strategy to prepare H2 O2 in a sustainable fashion. N-doped graphitic carbon with embedded cobalt nanoparticles was selected as an advanced material able to selectively trigger the ORR to form H2 O2 with a faradaic efficiency of almost 100 % at very positive applied potentials. The production of H2 O2 proceeded with high rates as calculated by bulk electrolysis (49 mmol g-1 h-1 ) and excellent current densities (≈-0.8 mA cm-2 at 0.5 V vs. reversible hydrogen electrode). The totally selective behavior depended on the combination of concomitant material features, such as the textural properties, the nature of the metal, the distribution of N moieties, the acidic environment, and the applied potential.

In this issue of Chem, Li and co-workers accessed the formation of high-density single Pt atoms thanks to the use of a well-devised support and ion exchange. The high Pt density in isolated form causes a high selectivity and rate toward the formation of hydrogen peroxide from the electrochemical reduction of oxygen.

One of the recent trends in electrocatalytic reactions involves the oxygen reduction reaction (ORR), where a new paradigm has been shaped to exploit this reaction for the synthesis of hydrogen peroxide (H2 O2 ). H2 O2 is a very versatile chemical of high commercial value, prepared currently through poorly sustainable processes. The emergence of metal-free carbon catalysts for the selective synthesis of H2 O2 is expected to revolutionize ORR research, beckoning at the development of new industrial schemes. The complexities of the mechanism and the factors dominating the selectivity of the process have been unveiled through a combination of theoretical and experimental studies.

The widespread industrial use of H2O2 has provoked great interest in the development of new and more efficient materials for its detection. Enzymatic electrochemical sensors have drawn particular attention, primarily because of their excellent selectivity. However, their high cost, instability, complex immobilization, and inherent tendency toward denaturation of the enzyme significantly limit their practical usefulness. Inspired by the powerful proton-catalyzed H2O2 reduction mechanism of peroxidases, we have developed a well-defined and densely functionalized carboxylic graphene derivative (graphene acid, GA) that serves as a proton source and conductive electrode for binding and detecting H2O2. An unprecedented H2O2 sensitivity of 525 μA cm–2 mM–1 is achieved by optimizing the balance between the carboxyl group content and scaffold conductivity of GA. Importantly, the GA sensor greatly outperforms all reported carbon-based H2O2 sensors and is superior to enzymatic ones because of its simple immobilization, low cost, and uncompromised sensitivity even after continuous operation for 7 days. In addition, GA-based sensing electrodes remain highly selective in the presence of interferents such as ascorbic acid, paracetamol, and glucose, as well as complex matrices such as milk. GA-based sensors thus have considerable potential for use in practical industrial sensing technologies.

Cerium Oxide (CeO2): Synthesis, Properties and Applications provides an updated and comprehensive account of the research in the field of cerium oxide based materials. The book is divided into three main blocks that deal with its properties, synthesis and applications. Special attention is devoted to the growing number of applications of ceria based materials, including their usage in industrial and environmental catalysis and photocatalysis, energy production and storage, sensors, cosmetics, radioprotection, glass technology, pigments, stainless steel and toxicology. A brief historical introduction gives users background, and a final chapter addresses future perspectives and outlooks to stimulate future research.

Carbon nanotubes and graphene possess a unique extended π-system that makes them stand out among carbon nanostructures. The resulting electronic properties enable electron or charge flow along one or two directions, respectively, thus offering the opportunity to connect electronically different entities that come into contact, be they living cells or catalytic systems. Using these carbon nanostructures thus holds great promise in providing innovative solutions to address key challenges in the fields of medicine and energy. Here, we discuss how chemical functionalization of these carbon nanostructures is a crucial tool to master their properties and deliver innovation.

Mechanically robust, chemically stable and electronically active carbon nanotubes (CNTs) are widely used as supports in catalysis. Synergistic effects between CNT and the active phase critically depend on the homogeneity of the carbon/inorganic interface, whose assembly is difficult to achieve without admixtures of free-standing inorganic matrix. Here we show that Fe-filled CNTs, employed as nanocatalyst supports, allow a facile preparation of highly pure and uniform CNT/nanocatalyst materials, by taking advantage of magnetic separation from poorly-defined components (e.g. aggregates of inorganic nanocatalysts). The higher homogeneity translates into higher catalytic activity in two industrially important processes: the photocatalytic hydrogen production and the water-gas shift reaction, WGSR (increase of ~48% activity for the former and up to ~45% for the latter as compared to catalysts isolated by standard filtration). In addition, the magnetic Fe core in the nanotubes enables effective separation and re-use of the nanocatalyst without loss of activity. This study demonstrates significant potential of magnetic CNTs as next generation of sustainable catalyst supports that can improve production of hydrogen and reduce the use of precious metals.

Carbon nanotubes have emerged as unique carbon allotropes that bear very interesting prospects in catalysis. Their use is mostly related to that of supports for inorganic metal catalysts, including molecular catalysts, metal nanoparticles, metal oxides or even more complex hierarchical hybrids. However, several reports have shown that they can intriguingly act as metal-free catalysts, with performance often superior to that of other carbon materials, in particular when ad hoc organic functional groups are attached prior to catalytic screening. The range of catalytic reactions is quite wide, and it includes standard organic synthesis, electrocatalysis, photocatalysis as well as other important industrial processes. In the last few years, the energy sector has acquired a dominant role as one of the most sought-after fields of application, given its ever-increasing importance in society.

Ceria (CeO 2 ) is enjoying increasing popularity in catalytic applications, and in some cases has established itself as an irreplaceable component. The reasons for such success stem from the intrinsic structural and redox properties of ceria. Reducing the ceria particles to the nanoscale has a profound impact on the catalytic behavior. The proliferation of improved synthetic methods that allow control over the final morphology and size of the nano-structures is opening new possibilities in terms of catalytic potential, particularly for energy-related applications.

The unique morphological characteristics of carbon nanotubes (CNTs) present the intriguing opportunity of exploiting the inner cavity for carrying out chemical reactions. Such reactions are catalysed either by the individual tubes that function both as catalysts and nanoreactors or by additional catalytic species that are confined within the channel. Such confinement creates what is called “confinement effect”, which can result in different catalytic features affecting activity, stability and selectivity. The review highlights the recent major advancements of catalysis conducted within the CNTs, starting from the synthesis of the catalytic composite, and discussing the most notable catalytic processes that have been reported in the last decade.

Carbon nanostructures (e.g., fullerenes, CNTs, graphene, nanohorns, nanodiamonds) play a key role in the development of nanomedicines. Here we analyze opportunities and barriers for their application in clinical settings. In particular, we discuss the unique properties of certain carbon nanostructures that allow for innovative solutions in theranostics, as well as current pitfalls around clinical applications of the EPR effect, the formation of the protein corona, and how functionalization of CNTs is a key tool to modulate their biodistribution and toxicity.

Considering the depletion of fossil-fuel reserves and their negative environmental impact, new energy schemes must point towards alternative ecological processes. Efficient hydrogen evolution from water is one promising route towards a renewable energy economy and sustainable development. Here we show a tridimensional electrocatalytic interface, featuring a hierarchical, co-axial arrangement of a palladium/titanium dioxide layer on functionalized multi-walled carbon nanotubes. The resulting morphology leads to a merging of the conductive nanocarbon core with the active inorganic phase. A mechanistic synergy is envisioned by a cascade of catalytic events promoting water dissociation, hydride formation and hydrogen evolution. The nanohybrid exhibits a performance exceeding that of state-of-the-art electrocatalysts (turnover frequency of 15000 H2 per hour at 50 mV overpotential). The Tafel slope of ∼130 mV per decade points to a rate-determining step comprised of water dissociation and formation of hydride. Comparative activities of the isolated components or their physical mixtures demonstrate that the good performance evolves from the synergistic hierarchical structure., Hydrogen evolution by water electrolysis is a promising route to 'green energy', but efficiency is still an issue. Here, the authors make mixed organic/inorganic hierarchical nanostructures with high hydrogen evolution activity, identifying synergic effects in the material contributing to enhanced efficiency.

Hydrogen evolution is among the most investigated catalytic processes given the importance of H2 from an industrial and an energy perspective. Achieving H2 production through green routes, such as water splitting or more realistically photoreforming of alcohols, is particularly desirable. In this work, we achieve a remarkable H2 productivity through photoreforming of either ethanol or glycerol as a sacrificial electron donor by employing a hybrid nanocatalyst where the properties of multi-walled carbon nanotubes (MWCNTs), Pd nanoparticles and crystalline TiO2 are optimally merged through appropriate engineering of the three components and an optimised synthetic protocol. Catalysts were very active both under UV (highest activity 25 mmol g−1 h−1) and simulated solar light (1.5 mmol h−1 g−1), as well as very stable. Critical to such high performance is the intimate contact of the three phases, each fulfilling a specific task synergistically with the other components.

Novel heteroarchitectures made of graphitic carbon nitride (g-C3N4) and halloysite nanotubes (HNTs) were prepared by a facile and soft self-assembly strategy. The morphological, structural and electronic properties of the HNTs/g-C3N4 nanocomposites were determined by means of a plethora of techniques including N-2 physisorption, XRD, FT-IR, TEM, UV-Vis absorption, XPS, zeta potential and photoluminescence (PL). Their photocatalytic activity was evaluated under both simulated solar light and pure visible light irradiation against the photodegradation of neutral, positively and negatively charged pollutants, namely phenol, methylene blue (MB) and methyl orange (MO), respectively. The prepared HNTs/g-C3N4 nanocomposites were proven to be durable and significantly more efficient than the pure g-C3N4 reference for the degradation of positively charged and neutral organics. The nanocomposites presented increased charge carrier formation and reduced recombination rates due to the tight contact between the two components. The enhanced photoactivity was attributed to the dual function of HNTs enhancing (a) the abundance and stability of the photogenerated e(-) and h(+) pairs and (b) the adsorption of positively charged organics on the nanocomposite. Both functions originate from the charged surface of HNTs.

Production of molecular hydrogen (H-2) is becoming an increasingly prominent process, due to high expectations as a new green energy carrier and key reagent for many industrial processes. Herein we report the high efficiency of H-2 production via photoreforming of ethanol using a catalyst based on hierarchical carbon nanocones hybridised with an inorganic layer of nanocrystalline TiO2 containing Pd nanoparticles.

The utilization of grown or deposited graphene on solid substrates offers key benefits for functionalization processes, but especially to attain structures with a high level of control for electronics and "smart" materials. In this review, we will initially focus on the nature and properties of graphene on substrates, based on the method of preparation. We will then analyze the most relevant literature on the functionalization of graphene on substrates. In particular, we will comparatively discuss radical reactions, cycloadditions, halogenations, hydrogenations, and oxidations. We will especially address the question of how the reactivity of graphene is affected by its morphology (i.e., number of layers, defects, substrate, curvature, etc.).

An efficient method is presented for preparing hierarchical catalysts composed of multi-walled carbon nanotubes (MWCNTs) and Pd@CeO2 core–shell nanoparticles. These materials were then examined for the water gas shift reaction (WGSR), which demonstrated intimate contact between the constituent parts. The integration of the carbonaceous support improves the stability of the nanoparticles by ordering the dispersion of the inorganic phase and increases the activity by suppressing the deactivation of the active phase that is commonly observed in conventional Pd–CeO2 under reducing conditions, e.g. WGSR conditions. An optimum MWCNTs:Pd@CeO2 ratio exists that affords totally homogeneous structures and provides the best catalytic properties.

Covalent functionalization of carbon nanotubes (CNTs) is the attachment of chemical moieties to the CNT tubular structure via the formation of covalent bonds, which share at least one pair of electrons between the CNT and the introduced chemical moiety. The typical scope of covalent sidewall functionalization is to increase not only the dispersibility and processability of CNTs but often also their reactivity. As a result, CNT physicochemical properties can be fine-tuned for intended applications, thus opening the way to the assembly of functional advanced materials, including nanotube-based composites or hybrids.

The rise of carbon nanotubes (CNTs) in the development of new functional materials for the most diverse applications seems to be tightly cuffed to their chemical functionalization. The reasons are multifaceted as functionalization can 1) improve solubility of CNTs, 2) provide them with anchor points for post-modification with application-dependant functional molecules 3) decrease their toxicity for medicinal and biological applications.

Short peptide hydrogels are attractive biomaterials but typically suffer from limited mechanical properties. Inclusion of other nanomaterials can serve the dual purpose of hydrogel reinforcement and of conferring additional physicochemical properties (e.g., self-healing, conductivity), as long as they do not hamper peptide self-assembly. In particular, nanocarbons are ideal candidates, and their physicochemical properties have demonstrated great potential in nanocarbon-polymer gel biomaterials for tissue engineering or drug delivery. Recently, increasing interest in supramolecular hydrogels drove research also on their enhancement with nanocarbons. However, little is known on the effect of nanocarbon morphology on the self-assembly of short peptides, which are among the most popular hydrogel building blocks. In this work, three different oxidized nanocarbons (i.e., carbon nanotube or CNT as 1D material, graphene oxide sheet or GO as 2D material, and carbon nanohorn or CNH as 3D material) were evaluated for their effects on the self-assembly of the unprotected tripeptide Leu-DPhe-DPhe at physiological conditions. Supramolecular hydrogels were obtained in all cases, and viscoelastic properties were clearly affected by the nanocarbons, which increased stiffness and resistance to applied stress. Notably, self-healing behavior was observed only in the case of CNTs. Tripeptide–nanotube interaction was noted already in solution prior to self-assembly, with the tripeptide acting as a dispersing agent in phosphate buffer. Experimental and in silico investigation of the interaction between peptide and CNTs suggests that the latter acts as nucleation templates for self-assembly and reassembly. Overall, we provide useful insights for the future design of composite biomaterials with acquired properties.