2D Carbon Materials Research Articles

Voltammetric measurements of neurotransmitter-acetylcholine through metallic nanoparticles embedded 2-D material

The most generally spread neurotransmitter acetylcholine (Ach) is used as a chemical messenger assisting in conveying signals transversely through the nerve synapse. Herein, two enzymes acetylcholinesterase and choline oxidase were covalently immobilized over the gold nanoparticles (AuNPs) embedded graphene oxide (GO; 2D carbon material) nanocomposite modified ITO coated glass plate. The synergetic and unique properties of AuNPs and GO present in nanocomposite are used to detect the ultra-small concentration of analyte, Ach. The prepared nanocomposites were characterized using different techniques i.e. TEM, XRD, SEM, FTIR, UV–Vis and Raman Spectroscopy. All the electrochemical measurements were performed using 3 electrodes integrated electrochemical system by introducing Ach through varying its concentration from 100 pM to 1000 nM. Cyclic voltammetry curves for different concentrations of Ach indicate the facile charge transfer process over the working electrode. Square wave voltammetry curves indicate the good sensing measurements of the modified electrode at the fixed potential. The limit of detection was found to be as low as 100 pM. In addition to these, selectivity of the electrode towards Ach molecule was confirmed by measuring the response towards other interfering agents. Besides this, the present nano interface is capable of detecting Ach in biological fluid such as serum.

Defect-Rich Graphene Nanomesh Produced by Thermal Exfoliation of Metal-Organic Frameworks for the Oxygen Reduction Reaction.

Although graphene nanomesh is an attractive 2D carbon material, general synthetic routes to produce functional graphene nanomesh in large-scale are complex and tedious. Herein, we elaborately design a simple two-step dimensional reduction strategy for exploring nitrogen-doped graphene nanomesh by thermal exfoliation of crystal- and shape-modified metal-organic frameworks (MOFs). MOF nanoleaves with 2D rather than 3D crystal structure are used as the precursor, which are further thermally unraveled into nitrogen-doped graphene nanomesh by using metal chlorides as the exfoliators and etching agent. The nitrogen-doped graphene nanomesh has a unique ultrathin two-dimensional morphology, high porosity, rich and accessible nitrogen-doped active sites, and defective graphene edges, contributing to an unprecedented catalytic activity for the oxygen reduction reaction (ORR) in acid electrolytes. This approach is suitable for scalable production.

Defect‐Rich Graphene Nanomesh Produced by Thermal Exfoliation of Metal–Organic Frameworks for the Oxygen Reduction Reaction

AbstractAlthough graphene nanomesh is an attractive 2D carbon material, general synthetic routes to produce functional graphene nanomesh in large‐scale are complex and tedious. Herein, we elaborately design a simple two‐step dimensional reduction strategy for exploring nitrogen‐doped graphene nanomesh by thermal exfoliation of crystal‐ and shape‐modified metal‐organic frameworks (MOFs). MOF nanoleaves with 2D rather than 3D crystal structure are used as the precursor, which are further thermally unraveled into nitrogen‐doped graphene nanomesh by using metal chlorides as the exfoliators and etching agent. The nitrogen‐doped graphene nanomesh has a unique ultrathin two‐dimensional morphology, high porosity, rich and accessible nitrogen‐doped active sites, and defective graphene edges, contributing to an unprecedented catalytic activity for the oxygen reduction reaction (ORR) in acid electrolytes. This approach is suitable for scalable production.

Three-dimensional graphene networks modified with acetylenic linkages for high-performance optoelectronics and Li-ion battery anode material

Searching for three-dimensional (3D) semiconducting carbon allotropes with proper bandgaps and excellent optoelectronic properties is always the chasing goal for the new emerging all-carbon optoelectronics. On the other side, 3D carbon materials have also been recognized as promising anode materials superior to commercialized graphite in Li-ion batteries (LIBs). Here, using first-principles calculations, we propose two novel 3D carbon allotropes through acetylenic linkages modification of two structurally intimately correlated 3D carbon structures — carbon kagome lattice (CKL) and interpenetrated graphene network (IGN). The modified CKL is a truly direct-gap semiconductor and possibly possesses the strongest optical transition coefficient amongst of all semiconducting carbon allotropes. The suitable bandgap and small effective masses also imply it can be a good electron transport material (ETM) for perovskite solar cells. As for the modified IGN, it is a topological nodal line semimetal and shows greatly enhanced specific capacity as anode materials in LIBs comparing to that of IGN. Our work not only find two new 3D carbon phases with fabulous physical and chemical properties for high-performance optoelectronics and Li-ion anode material, we also offer a fresh view to create various carbon structures with versatile properties.

Defective synergy of 2D graphitic carbon nanosheets promotes lithium-ion capacitors performance

2D carbon materials show extraordinarily promising prospects in energy storage systems. To improve the performance of lithium-ion capacitors (LICs), it is urgently necessary for addressing the sluggish kinetics behavior of battery-type carbon negative electrode. Herein, novel 2D defective high-graphitic carbon nanosheets (GNS), which is derived from in-situ catalytic graphitization of 1D nanorods precursor, are presented and employed as negative electrode materials in LICs. The effects of defects contained in the as-prepared samples are further explored by the First-principle calculations, revealing that carbonylation and N-doping (particularly pyridine N) manifest synergistic effect on improving the electronic conductivity and regulating the microstructure. The high reversible capacity accompanied with large plateau capacity and superior rate capability in the half-cell test implies that GNS can be a promised candidate as negative electrode for LICs. Excitingly, the fabricated LICs exhibit high energy density of 112 Wh kg−1 and excellent power density of 19,600 W kg−1, together with outstanding energy density retention of 96.5% after 5000 cycles at 5 A g−1. The defects-controlled in-situ catalytic strategy for preparing GNS may provide a brand-new way for materials design for energy storage.

Adenine Derivative Host with Interlaced 2D Structure and Dual Lithiophilic-Sulfiphilic Sites to Enable High-Loading Li-S Batteries.

How to simultaneously restrain the loss of active species and facilitate the conversion reaction under high S loading condition is the key to solve the commercialization of Li-S batteries. For this system, the availability of raw materials and simplicity (high efficiency) of synthetic strategies are also important factors. Herein, we propose an interlaced two-dimensional (2D) carbon material as advanced Li-S cathode host characterized by corrugated monolithic morphology and Co/N dopants as dual lithiophilic-sulfiphilic sites. This 2D structure is derived from a cheap biomass precursor, adenine, with bonding interaction with a MgCl2 hydrate template via a facile ionothermal method. It allows a homogeneous spatial distribution of S/Li2S deposits and strong adsorbability and enhanced conversion kinetics for polysulfides. Benefiting from the synergistic effects ofcorrugated 2D conductive matrix andembedded heteroatom/nanodot catalyst, the resultant sulfur cathode releases a high specific capacity of 1290.4 mA h g-1 at 0.2 C, small capacity fading rate of 0.029% per cycle over 600 cycles at 2 C, superior rate performance up to 20 C, and considerable areal capacity retention of 6.0 mA h cm-2 even under an ultrahigh sulfur loading up to 9.7 mg cm-2.

Decoupling and correlating the ion transport by engineering 2D carbon nanosheets for enhanced charge storage

The high aspect ratio of two-dimensional (2D) carbon materials feature unique superiorities and great potential in supercapacitors. The transport of electrolyte ions inside the 2D carbon electrode that can directly affect the overall electrochemical performance, is a key issue that need to be concerned. Nevertheless, the research regarding this process always lags far behind the material concerns and the intrinsic factors to affect ion transport remain obscure. Here we for the first time focus on and correlate the potential and possible factors for addressing this issue using 2D porous carbon nanosheets with tunable thickness as representative demos. A compromise balance between the thickness and ion transport behavior is presented and investigated. The optimal thickness of nanosheets can effectively avoid curling and stacking of ultrathin nanosheets, shorten the distance of ion transport and accelerate the ion diffusion, which render the material with the low resistance corresponding to minimum Warburg coefficient and maximum ion diffusion coefficient for fast transport of electrolyte. A superior capacitance value of 280 F g−1 can be obtained at 0.5 A g−1, with a retention rate of 81% even at a large current density of 100 A g−1. Besides, the symmetric supercapacitor with 1-ethyl-3-methylimidazolium tetrafluoroborate electrolyte (EMIMBF4) delivers an energy density of 94 Wh kg−1 at 1.8 kW kg−1. This work illustrates the importance for transferring the focus from carbon materials to electrolyte ion transport behavior within electrode and provides a guidance for regulating the ion transport by engineering the microscopic thickness of advanced materials in energy-related fields.

Light-Responsive Actuators Based on Graphene.

As a typical 2D carbon material, graphene, that possesses outstanding physical/chemical properties, has revealed great potential for developing soft actuators. Especially, the unique properties of graphene, including the excellent light absorption property, softness, and thermal conductivity, play very important roles in the development of light-responsive graphene actuators. At present, various light-driven actuators have been successfully developed based on graphene and its derivatives. In this mini review, we reviewed the recent advances in this field. The unique properties of graphene or graphene-related materials that are of benefit to the development of light-driven actuators have been summarized. Typical smart actuators based on different photothermal/photochemical effects, including photothermal expansion, photothermal desorption, photoisomerization, and photo-triggered shape memory effect, have been introduced. Besides, current challenges, and future perspective have been discussed. The rapid progress of light-responsive actuators based on graphene has greatly stimulated the development of graphene-based soft robotics.

Ultra-thin, highly graphitized carbon nanosheets into three-dimensional interconnected framework utilizing a ball mill mixing of precursors

Constructing two-dimensional (2D) carbon nanosheets into a three-dimensional (3D) framework can prevent restacking and increase the accessible surface area, which is promising to broaden the range of applications of 2D carbon materials. Here we report a facile preparation of an ultrathin, highly graphitized carbon nanosheets framework (UGCF) by directly carbonizing a gel composite of resol, FeCl3·6H2O, and F127 block polymer prepared by ball milling. During the carbonization process, the presence of FeCl3·6H2O in the resol-F127-Fe composite benefits the formation of highly graphitized structure, while F127 helps to introduce the porous architecture, resulting in an interconnected framework of carbon nanosheets. The unique carbon nanostructure of this UGCF has major advantages for electrochemical applications, owing to the large accessible geometrical surface, the rapid diffusion paths for ions, and the continuous transfer path for electrons through the graphitic framework. When used as anode in lithium-ion batteries, the UGCF shows excellent electrochemical performance in terms of capacity, rate performance, and cycle stability. This work provides a convenient and simple scale-up method to prepare highly graphitized carbon nanosheets with 3D nanoarchitecture.

Two-Dimensional Carbon-Based Auxetic Materials for Broad-Spectrum Metal-Ion Battery Anodes.

Auxetic materials possess special applications due to their unique negative Poisson's ratios (NPRs). As a classic 2D carbon material, the NPR of graphene is still deliberated. Introducing the NPR in graphene would increase its extraordinary properties, and the NPR together with other properties would bring more significant applications for graphene. In this Letter, on the basis of first-principles calculations, we reconfigure the structure of graphene, and, as an example, we propose a new 2D planar carbon allotrope, xgraphene, which is constructed by 5-6-7 carbon rings. Our theoretical calculations indicate that xgraphene has an NPR and constitutes a broad spectrum of metal ion battery anodes with high performance. Its maximum storage capacities are 930/1302/744/1488 mAh/g for Li/Na/K/Ca-ion batteries. It has low metal-ion diffusion energy barriers (≤0.49 eV) and low average open-circuit voltages (≤0.53 V). Our density functional theory results also showed that it is intrinsically metallic and possesses dynamic, thermal, and mechanical stabilities. Its intrinsic NPR, which stems from the weakness of coupling of carbon-carbon bonds, is found upon loading the uniaxial strain along the armchair direction. This work not only opens up a new direction for the design of the next-generation broad-spectrum energy-storage materials with low cost and high performance but also offers a class application for auxetic materials.

Hexagonal phase NiS octahedrons co-modified by 0D-, 1D-, and 2D carbon materials for high-performance supercapacitor

It's crucial to improve the electronic conductivity, active sites and structural stability of transition-metal sulfides for better performance. Herein, hexagonal-phase NiS octahedrons were obtained through phase transition and co-modified by multidimensional carbon, i.e. 0D carbon QDs, 1D CNTs, and 2D reduced graphene oxide (NiS@C QDs-CNTs-rGO). It delivers a significantly enhanced specific capacity of 241 mAh g−1 at a current density of 1 A g−1 and capacity of 149 mAh g−1 at 20 A g−1, superior to its counterparts with other phases NiS2@CNTs-rGO (154 mAh g−1 at 1 A g−1, 52 mAh g−1 at 20 A g−1) and Ni7S6@CNTs-rGO (167 mAh g−1 at 1 A g−1, 124 mAh g−1 at 20 A g−1). Furthermore, asymmetric supercapacitors (ASC) assembled by NiS@C QDs-CNTs-rGO and graphene hydrogel achieve a remarkable cycling stability (capacity retention of 82% after 5000 cycles). XPS results confirm that strong CS bonds exist between carbon matrix and NiS NPs, which stabilizes structural stability and thus leading to excellent long-term cycling stability. The excellent electrochemical performance could be ascribed to the improved conductivity and structural stability, the co-modified 0D, 1D, and 2D carbon structures, and strong CS bonds between active material and carbon matrix.

Confined Synthesis of 2D Nanostructured Materials toward Electrocatalysis

2D nanostructured materials have shown great application prospects in energy conversion, owing to their unique structural features and fascinating physicochemical properties. Developing efficient approaches for the synthesis of well‐defined 2D nanostructured materials with controllable composition and morphology is critical. The emerging concept, confined synthesis, has been regarded as a promising strategy to design and synthesize novel 2D nanostructured materials. This review mainly summarizes the recent advances in confined synthesis of 2D nanostructured materials by using layered materials as host matrices (also denoted as “nanoreactors”). By virtue of the space‐ and surface‐confinement effects of these layered hosts, various well‐organized 2D nanostructured materials, including 2D metals, 2D metal compounds, 2D carbon materials, 2D polymers, 2D metal‐organic frameworks (MOFs) and covalent‐organic frameworks (COFs), as well as 2D carbon nitrides are successfully synthesized. The wide employment of these 2D materials in electrocatalytic applications (e.g., electrochemical oxygen/hydrogen evolution reactions, small molecule oxidation, and oxygen reduction reaction) is presented and discussed. In the final section, challenges and prospects in 2D confined synthesis from the viewpoint of designing new materials and exploring practical applications are commented, which would push this fast‐evolving field a step further toward greater success in both fundamental studies and ultimate industrialization.

Two-dimensional graphyne-like carbon nitrides: Moderate band gaps, high carrier mobility, high flexibility and type-II band alignment

Two-dimensional (2D) carbon nitrides are drawing increasing interests due to the structural diversities and unique electronic properties, superiors to the pure 2D carbon materials. Motivated by the recent experimental progresses, we investigated from first-principles a new family of 2D carbon nitrides composed of sp- and sp2-hybridized carbon atoms and with kagome, rhombic and hexagonal lattices. The kagome and rhombic lattices exhibit moderate electronic band gaps (0.98–3.34 eV), high carrier mobility in the order of 3 × 105 cm2V−1s−1, high flexibility with critical strain up to 44%–47%, and type-II band alignment which are desired for applications in electronic devices and solar cells. Our findings are expected to offer theoretical bases for synthesis and applications of these novel 2D carbon nitrides and promote the following experimental exploration.

Magnetic Properties of One- and Two-Dimensional Functional Materials: Oxygen Molecules Encapsulated in Single-Walled Carbon Nanotubes and Copper Ions Embedded into Phthalocyanine Sheets

Background: In this paper, we report on the topics of one-dimensional (1D) and two-dimensional (2D) functional materials. Single-Walled Carbon Nanotubes (SWCNTs) are seamless hollow cylinders made of hexagonal lattice graphite sheets. The SWCNTs have attracted considerable attention due to the applicability of their enclosed nanospaces to engineering, and many types of guest materials are encapsulated inside their 1D space, expecting unusual properties. The poly Transition Metal (TM) phthalocyanine, in which phthalocyanine units are extended in two dimensions by sharing benzene rings, is one of the examples of the TM containing 2D carbon materials. Because of strong correlation between localized d-electrons in the TM atom and delocalized π-electrons on the poly phthalocyanine frame, it is expected that spin-polarized conduction, which is useful for the spintronic applications. Objectives: The objective of the first work is to synthesize SWCNTs encapsulating oxygen molecules having spin one, whose O-O bond directions are aligned to the longitudinal direction of the SWCNTs. The objective of the second work is to synthesize Poly Cu Phthalocyanine (PCuPc) through a bottom-up method by using copper octacyanophthalocyanine as a building block and to elucidate its crystal structure and magnetic properties. Methods: SWCNTs with inner diameter of ca 0.8 nm were prepared by the CoMoCAT method, and encapsulated together with oxygen molecules (~400 Torr) into a high-purity quartz tube. To subtract the background signals of the SWCNTs and the quartz tube, we prepared the same SWCNTs inducing He gas after evacuating oxygen molecules. Magnetization measurements of these SWCNTs samples were conducted by means of a SQUID magnetometer and a pulse magnet using an induction method. PCuPc were synthesized by a solid state reaction of octacyanophthalocyanine, tetracyanobenzene, and CuCl2·2H2O in glass ampoules sealed after evacuation. The as-synthesized samples were characterized using XRD analysis and TEM microscopy. Magnetization measurement of the samples were done by using a SQUID magnetometer. Results: The intrinsic magnetization data from oxygen molecules inside the SWCNTs (temperature and magnetic field dependence) show magnetic properties typical of the spin-one Heisenberg antiferromagnet named a Haldane magnet. PCuPc and its half-filling counterpart were obtained by solid state reaction. Both magnetic susceptibility and magnetization of PCuPc are larger than those of half-filling PCuPc, but the magnitudes of the former sample are about 1.5 times larger than those of the latter one, which is expected to be twice from the geometric superlattice structure. Conclusion: We have studied magnetic properties (magnetic susceptibility and magnetization) of oxygen molecules encapsulated into Single Walled Carbon Nanotubes (SWCNTs) with diameters of about 0.8 nm, regarded as a 1D functional magnetic material, and Poly Copper Phthalocyanine (PCuPc) and poly half-filling copper phthalocyanine (half-filling PCuPc), regarded as 2D functional magnetic materials.

Hierarchically porous nanosheets-constructed 3D carbon network for ultrahigh-capacity supercapacitor and battery anode

An advanced hierarchically porous nanosheets-constructed three-dimensional (3D) carbon material (HPNSC) is prepared by using low-cost agricultural waste-nelumbium seed-pods as the precursor, and potassium hydroxide (KOH) as the activator. The as-prepared HPNSC material has a hierarchically porous nanosheets-constructed structure with 3D carbon nanosheet network morphology, which can enable fast and efficient transfer of Li+/Na+/H+ during charge–discharge process. The assembled HPNSC//HPNSC symmetric supercapacitors exhibit an improved energy density of 41.3 W h kg−1 with a power density of 180 W kg−1 in 1 mol l−1 Na2SO4 electrolyte. The energy density can still be maintained at 16.3 W h kg−1 even if the power density is increased to 9000 W kg−1. When acting as the reversible electrode for lithium ion batteries, this HPNSC material can achieve a high specific capacity of 1246 mA h g−1 at 0.1 A g−1. Moreover, sodium ion battery with HPNSC electrode exhibits excellent cycling performance of 161.8 mA h g−1 maintained even after being cycled 3350 times. The electrochemical performances clearly indicate that the HPNSC developed in this work is a very promising energy storage electrode material, and can further provide new insights for designing and developing highly porous materials for energy storage in other fields.

Intensified C≡C Stretching Vibrator and Its Potential Role in Monitoring Ultrafast Energy Transfer in 2D Carbon Material by Nonlinear Vibrational Spectroscopy.

In this work, an intensity-enhanced C≡C stretching infrared (IR) absorption is observed in hexakis[(trimethylsilyl)ethynyl]benzene (HTEB), whose IR transition dipole magnitude becomes comparable to that of a typical C═O stretch, and the enhancement is believed to be due to a joint effect of π-π conjugation and hyperconjugation associated with a terminal trimethylsilyl group. Using dynamical time-dependent two-dimensional infrared (2D IR) spectroscopy, a picosecond intramolecular energy redistribution process is observed between two nondegenerate C≡C stretching modes, whose symmetry breaking is attributed to a noncovalent halogen-bonding interaction between HTEB and solvent CH2Cl2. The rigid structure of HTEB and limited structural dynamics are also inferred from the insignificant initial spectral diffusion value extracted from the 2D IR spectra. This work provides the first nonlinear infrared investigation of the conventionally weak C≡C stretch. The methods outlined are particularly important for detailed understanding of the structure-related processes such as vibrational energy transfer in novel C≡C species containing materials such as graphdiyne.

Pure nitrogen-doped graphene aerogel with rich micropores yields high ORR performance

How good can the oxygen reduction reaction (ORR) performance of metal-free 3D carbon material be, if the ratio of micropores to all the micropores and mesopores in it can be greatly increased? To answer this question, a nitrogen doped graphene aerogel (NGA) with rich micropores is prepared by a facial one-pot assembly. Pores especially rich micropores introduced by the dense packing of graphene oxide (GO) precursor with small size facilitated by the crosslinking agent dopamine (DA) in walls of NGA with a large specific surface area (1631 m2/g) shorten the diffusion time and decrease the transport distance of O2 inside the pores; a high N content (7.21 at%) increases the adsorption and diffusion of O2 in NGA; consequently increase the ORR speed, rendering so far the largest ORR current density of NGA among reported metal-free carbon catalysts and Pt-based catalysts, promising for applications in fuel cells.

PCF-Graphene: A 2D sp2-Hybridized Carbon Allotrope with a Direct Band Gap

Motivated by the recent progress in synthesizing graphene by using aromatic benzene molecules as precursors, herein, we propose a new two-dimensional (2D) carbon allotrope by using nonaromatic molecule cyclooctatetraene as the precursor from a bottom-up approach. In this structure, all the carbon atoms are threefold coordinated, similar to the sp2-hybridized atoms in graphene; thus, we name the poly-cyclooctatetraene framework as PCF-graphene. First-principles calculations reveal that although PCF-graphene is metastable compared with graphene, it is thermally, mechanically, and dynamically stable. Different from graphene with a single-atomic thickness and zero band gap, PCF-graphene has a finite thickness of 2.45 Å and is a semiconductor with a direct band gap of 0.77 eV. It exhibits anisotropies in mechanical properties, carrier mobility, and optical adsorption because of its anisotropic lattice. This study not only sheds insights into the design of 2D carbon materials from some simple organic molecules but also expands the 2D purely three-coordinated carbon family from a single-atomic layer to a finite thickness. PCF-graphene can be used as a rung in the ladder to stabilize three-dimensional three-coordinated carbon system that remains elusive currently.

Assembling Carbon Pores into Carbon Sheets: Rational Design of Three-Dimensional Carbon Networks for a Lithium-Sulfur Battery.

The conversion reaction-based lithium-sulfur battery features an attractive energy density of 2600 W h/kg. Nevertheless, the unsatisfied performance in terms of poor discharge capacity and cycling stability still hinders its practical applications. Recently, porous carbon materials have been widely reported as promising sulfur reservoirs to promote the sluggish reaction kinetics of sulfur conversion, tolerate volume expansion of sulfur, and suppress polysulfide shuttling. However, porous carbon with a simply designed nanostructure is hard to satisfy all of these aspects simultaneously. Herein, we have applied a dual-template strategy that assembles carbon pores into carbon sheets to prepare three-dimensional (3D) nitrogen-doped porous carbon nanosheets (N-PCSs) as the multifunctional sulfur host for the Li-S battery. By arranging carbon pores within an interconnected 3D architecture, the porous carbon sheets enable rapid electron/ion transfer. Moreover, the micro/mesopores and nitrogen dopant in N-PCS provide both physical and chemical restrictions to polysulfide species. With these advances, the N-PCS/S cathode delivers a large initial discharge capacity of 1360 mA h/g at 0.1 C. When performed at 0.5 C for 1000 cycles, the cathode can still remain ∼50% of its capacity with a low decay rate of 0.05% per cycle, showing the important role of the 3D carbon material in the Li-S battery.

Graphdiyne bearing pillar[5]arene-reduced Au nanoparticles for enhanced catalytic performance towards the reduction of 4-nitrophenol and methylene blue.

Graphdiyne (GD), a novel two dimensional (2D) carbon material, has earned a lot of attention in recent years. Constructing a novel hybrid nanomaterial based on GD, macrocyclic host and Au nanoparticles is an effective strategy for heterogeneous catalysis applications. While tremendous advancements in the preparation of two dimensional (2D) materials anchoring Au nanoparticles have been made, it is an urgent requirement to explore a green, efficient and facile approach for obtaining small-sized Au nanoparticles. The use of the 2D material graphdiyne (GD) presents more-promising candidates for constructing excellent sites for loading metal nanoparticles. In this study, a novel 2D heterogeneous hybrid nanomaterial (P5A-Au-GD) based on GD and pillar[5]arene (P5A)-reduced Au nanoparticles (P5A-Au) was successfully prepared. In this strategy, the P5A can reduce HAuCl4 with the aid of NaOH in the dispersion of GD. Accordingly, the generated P5A-Au can immediately interact with GD to form the P5A-Au-GD hybrid nanomaterial without any harsh reduced materials or other energies. The Au nanoparticles with average diameter of 2–3 nm are homogeneously dispersed on the surface of GD. The heterogeneous 2D catalyst of P5A-Au-GD shows high catalytic performances in the reduction of 4-nitrophenol and methylene blue by comparing commercial Pd/C catalyst. Meanwhile, the unique 2D heterogeneous hybrid material P5A-Au-GD exhibits durable recyclability and stability during the catalytic reaction. Considering the outstanding merits of the heterogeneous 2D catalyst of P5A-Au-GD as well as the simple and green preparation, this study might not only present enormous opportunities for the stabilized, high-performance and sustainable catalysts but also be applied in other frontier studies of sustainable functionalized nanocomposites and advanced materials.