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Surfaces
Special Issues
Surface Science and Catalysis of Graphene-Related 2D Materials
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Surface Science and Catalysis of Graphene-Related 2D Materials

A special issue of Surfaces (ISSN 2571-9637).

Deadline for manuscript submissions: closed (31 May 2020) | Viewed by 30939

Special Issue Editors

Prof. Dr. Qiang Fu

E-Mail Website
Guest Editor
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Interests: surface science; heterogeneous catalysis; thin films; interface science
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Gaetano Granozzi

E-Mail Website
Guest Editor
Department of Chemical Science, Universita degli Studi di Padova, Padua, Italy
Interests: ultrathin films; 2D materials; model electrocatalysts; model catalysts; HER, ORR and CRR
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Graphene (G) and other 2D materials (e.g., h-BN, transition metal chalcogenides, phosphorene, 2D carbides, 2D oxides, etc.) are altogether referred to as graphene-related materials (GRMs), and they are gaining great interest for their exceptional properties. Today, the forefront of research has progressed from simple GRM preparation and characterization toward their use in real applications. Whereas in many devices (photonics, optoelectronics, etc.), the goal is the most perfect GRM assemblies with defect-less interfaces, in the case of catalysis (either photo- and electro- and thermal catalysts), energy, and sensor, the quantity and quality of the exposed surfaces and their defectivity play a leading role for the designed functionalities. In these cases, chemically-modified high surface area GRMs hybrid nanoarchitectures (organized in 2D and 3D) are the target. In particular, systems constituted by 2D GRMs, assembled together to form 3D interconnected networks or hybridized with other nano-objects like nanoparticles, nanotubes, and capsules, have the great advantage of maintaining a high surface area while inducing multifunctionality. Very remarkably, the new engineered GRMs systems can be used either as innovative supports for dispersed catalysts or as metal-free catalysts themselves. In addition, they are also effective platforms to anchor molecular active centers, thus combining the activity and selectivity of the homogeneous catalysts with recyclability and stability of the final catalytic system.

The rational design of the chemical properties of such 2D and 3D GRMs requires an equally rational approach. Surface science can provide an effective platform for developing and testing GRMs for catalysis and energy chemistry. The aim of this Special Issue is to offer an open-access forum where researchers in the field of surface science, energy chemistry, and catalysis could join their efforts to rationally develop new 2D and 3D GRMs systems for their application in strategic fields like catalysis and energy conversion.

Prof. Qiang Fu
Prof. Gaetano Granozzi
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Surfaces is an international peer-reviewed open access quarterly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Graphene and related 2D materials (GRMs: e.g., h-BN, layered chalcogenides, phosphorene, carbides, and oxides)
  • Preparation and use of chemically modified 2D and 3D GRMs nanoarchitectures
  • Preparation and use of hybrid GRMs nanoarchitectures (among different GRMs or with other nanoobjects)
  • Structure and chemical properties of GRMs by a surface science-based approach
  • Thermal, electro- and photocatalysis using GRMs
  • GRMs for energy conversion and storage
  • Homogeneous catalysts heterogenized on GRMs
  • Computational studies and modeling

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Published Papers (7 papers)

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Research

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9 pages, 2514 KiB  
Article
In Situ Monitoring of Growth of Vertically Stacked h-BN/Graphene Heterostructures on Ni Substrates and Their Interface Interaction
by Wei Wei, Guanhua Zhang, Jiaqi Pan, Yi Cui and Qiang Fu
Surfaces 2020, 3(3), 328-336; https://doi.org/10.3390/surfaces3030024 - 14 Jul 2020
Cited by 2 | Viewed by 3188
Abstract
Vertically stacked hexagonal boron nitride (h-BN)/graphene heterostructures present potential applications in electronic, photonic, and mechanical devices, and their interface interaction is one of the critical factors that affect the performances. In this work, the vertical h-BN/graphene heterostructures with high coverage are synthesized by [...] Read more.
Vertically stacked hexagonal boron nitride (h-BN)/graphene heterostructures present potential applications in electronic, photonic, and mechanical devices, and their interface interaction is one of the critical factors that affect the performances. In this work, the vertical h-BN/graphene heterostructures with high coverage are synthesized by chemical vapor deposition (CVD) of h-BN on Ni substrates followed by segregation growth of graphene at the h-BN/Ni interfaces, which are monitored by in situ surface microscopy and surface spectroscopy. We find that h-BN overlayers can be decoupled from Ni substrates by the graphene interlayers. Furthermore, the h-BN domain boundaries exhibit a confinement effect on the graphene interlayer growth and the lower graphene domains are limited within the upper h-BN domains. This work provides new insights into the formation mechanism and interface interaction of the vertical heterostructures. Full article
(This article belongs to the Special Issue Surface Science and Catalysis of Graphene-Related 2D Materials)
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12 pages, 2130 KiB  
Article
In Situ Study of Graphene Oxide Quantum Dot-MoSx Nanohybrids as Hydrogen Evolution Catalysts
by Marco Favaro, Mattia Cattelan, Stephen W. T. Price, Andrea E. Russell, Laura Calvillo, Stefano Agnoli and Gaetano Granozzi
Surfaces 2020, 3(2), 225-236; https://doi.org/10.3390/surfaces3020017 - 16 Jun 2020
Cited by 3 | Viewed by 3999
Abstract
Graphene quantum dots (GOQDs)-MoSx nanohybrids with different MoSx stoichiometries (x = 2 and 3) were prepared in order to investigate their chemical stability under hydrogen evolution reaction (HER) conditions. Combined photoemission/electrochemical (XPS/EC) measurements and operando X-ray absorption spectroscopy (XAS) were employed [...] Read more.
Graphene quantum dots (GOQDs)-MoSx nanohybrids with different MoSx stoichiometries (x = 2 and 3) were prepared in order to investigate their chemical stability under hydrogen evolution reaction (HER) conditions. Combined photoemission/electrochemical (XPS/EC) measurements and operando X-ray absorption spectroscopy (XAS) were employed to determine the chemical changes induced on the MoSx-based materials as a function of the applied potential. This in situ characterization indicates that both MoS2 and MoS3 materials are stable under operating conditions, although sulfur terminal sites in the MoS3 nanoparticles are converted from S-dimer (S22−) to S-monomer (S2−), which constitute the first sites where the hydrogen atoms are adsorbed for their subsequent evolution. In order to complete the characterization of the GOQDs-MoSx nanohybrids, the composition and particle size were determined by X-ray photoemission spectroscopy (XPS), X-ray diffraction (XRD) and Raman spectroscopy; whereas the HER activity was studied by conventional electrochemical techniques. Full article
(This article belongs to the Special Issue Surface Science and Catalysis of Graphene-Related 2D Materials)
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8 pages, 1606 KiB  
Article
Tuning the Catalytic Activity of a Quantum Nutcracker for Hydrogen Dissociation
by Lei Tao, Yu-Yang Zhang, Sokrates T. Pantelides and Shixuan Du
Surfaces 2020, 3(1), 40-47; https://doi.org/10.3390/surfaces3010004 - 20 Jan 2020
Cited by 2 | Viewed by 3168
Abstract
A quantum nutcracker, a recently proposed catalytic system for hydrogen dissociation, consists of two inert components: an organic molecule such as a transition metal phthalocyanine and an inert surface such as Cu or Au. The reaction takes place at the interface between the [...] Read more.
A quantum nutcracker, a recently proposed catalytic system for hydrogen dissociation, consists of two inert components: an organic molecule such as a transition metal phthalocyanine and an inert surface such as Cu or Au. The reaction takes place at the interface between the two components, which are weakly bonded by Van der Waals (VdW) forces. Here, we explore a method used to tune the reaction barrier in a quantum nutcracker system for hydrogen dissociation. By employing density-functional-theory calculations, we find that the H2 entry barrier, which is the rate-limiting barrier, is reduced by replacing the phthalocyanine by porphyrin derivatives such as octaethylporphyrin (OEP) and tetraphenylporphyrin (TPP). The system remains active if a dissociated H atom is adsorbed on the transition metal ion. Metallic two-dimensional materials such as NbS2 and CoS2 are good candidates for the quantum nutcracker. The present design of a quantum nutcracker for hydrogen dissociation provides new opportunities with which to induce catalytic activity in VdW-bonded systems. Full article
(This article belongs to the Special Issue Surface Science and Catalysis of Graphene-Related 2D Materials)
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10 pages, 3217 KiB  
Article
Hybrid Cathodes Composed of K3V2(PO4)3 and Carbon Materials with Boosted Charge Transfer for K-Ion Batteries
by Xianghua Zhang, Xinyi Kuang, Hanwen Zhu, Ni Xiao, Qi Zhang, Xianhong Rui, Yan Yu and Shaoming Huang
Surfaces 2020, 3(1), 1-10; https://doi.org/10.3390/surfaces3010001 - 11 Jan 2020
Cited by 11 | Viewed by 5307
Abstract
K-ion batteries (KIBs) have emerged as an auspicious alternative to Li-ion batteries (LIBs) owing to their uniform distribution, plentiful reserves, the low cost of K resources, and their similar physicochemical properties to Li resources. The development of KIBs is seriously limited by cathode [...] Read more.
K-ion batteries (KIBs) have emerged as an auspicious alternative to Li-ion batteries (LIBs) owing to their uniform distribution, plentiful reserves, the low cost of K resources, and their similar physicochemical properties to Li resources. The development of KIBs is seriously limited by cathode materials. Here, a hybrid of K3V2(PO4)3 (KVP) particles triple-coated by amorphous carbon, carbon nanotubes (CNTs), and reduced graphene oxide (rGO) nanosheets (KVP/C/CNT/rGO) was fabricated by a facile ball milling process followed by heat treatment. Consequently, a stable capacity of 57 mAh g−1 can be achieved at 0.2C, and a slow capacity decaying rate (0.06% per cycle) is displayed during 500 cycles under a high current density of 5C. The remarkable reversible capacity and excellent long-term cycling life are mainly due to the enhanced interwoven C/CNT/rGO networks and superior KVP crystal structure stability, which can provide multi-channel for fast electron transport and effective K+ diffusion. Full article
(This article belongs to the Special Issue Surface Science and Catalysis of Graphene-Related 2D Materials)
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15 pages, 3534 KiB  
Article
Effect of Ni Doping on the MoS2 Structure and Its Hydrogen Evolution Activity in Acid and Alkaline Electrolytes
by Dario Mosconi, Paul Till, Laura Calvillo, Tomasz Kosmala, Denis Garoli, Doriana Debellis, Alessandro Martucci, Stefano Agnoli and Gaetano Granozzi
Surfaces 2019, 2(4), 531-545; https://doi.org/10.3390/surfaces2040039 - 3 Dec 2019
Cited by 38 | Viewed by 5693
Abstract
We have investigated three-dimensional (3D) MoS2 nanoarchitectures doped with different amount of Ni to boost the hydrogen evolution reaction (HER) in alkaline environment, where this reaction is normally hindered. As a comparison, the activity in acidic media was also investigated to determine [...] Read more.
We have investigated three-dimensional (3D) MoS2 nanoarchitectures doped with different amount of Ni to boost the hydrogen evolution reaction (HER) in alkaline environment, where this reaction is normally hindered. As a comparison, the activity in acidic media was also investigated to determine and compare the role of the Ni sites in both media. The doping of MoS2, especially at high loadings, can modify its structural and/or electronic properties, which can also affect the HER activity. The structural and electronic properties of the Ni doped 3D-MoS2 nanoarchitecture were studied by X-ray diffraction (XRD), Raman spectroscopy, scanning and transmission electronic microscopy (SEM; TEM), and X-ray photoemission Spectroscopy (XPS). XPS also allowed us to determine the Ni-based species formed as a function of the dopant loading. The HER activity of the materials was investigated by linear sweep voltammetry (LSV) in 0.5 M H2SO4 and 1.0 M KOH. By combining the physicochemical and electrochemical results, we concluded that the Ni sites have a different role in the HER mechanism and kinetics in acidic and in alkaline media. Thus, NiSx species are essential to promote HER in alkaline medium, whereas the Ni-Mo-S ones enhance the HER in acid medium. Full article
(This article belongs to the Special Issue Surface Science and Catalysis of Graphene-Related 2D Materials)
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Review

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36 pages, 17347 KiB  
Review
Catalysis Mediated by 2D Black Phosphorus Either Pristine or Decorated with Transition Metals Species
by Matteo Vanni, Maria Caporali, Manuel Serrano-Ruiz and Maurizio Peruzzini
Surfaces 2020, 3(2), 132-167; https://doi.org/10.3390/surfaces3020012 - 1 Apr 2020
Cited by 12 | Viewed by 4616
Abstract
Among the novel class of mono-elemental two-dimensional (2D) materials, termed Xenes, phosphorene is emerging as a great promise for its peculiar chemical and physical properties. This review collects a selection of the recent breakthroughs that are related to the application of phosphorene in [...] Read more.
Among the novel class of mono-elemental two-dimensional (2D) materials, termed Xenes, phosphorene is emerging as a great promise for its peculiar chemical and physical properties. This review collects a selection of the recent breakthroughs that are related to the application of phosphorene in catalysis and electrocatalysis. Noteworthy, thanks to its intrinsic Lewis basic character, pristine phosphorene turned out to be more efficient and more selective than other non-metal catalysts, in chemical processes as the electroreduction of nitrogen to ammonia or the alkylation of nucleophiles with esters. Once functionalized with transition metals nanoparticles (Co, Ni, Pd, Pt, Ag, Au), its catalytic activity has been evaluated in several processes, mainly hydrogen and oxygen evolution reactions. Under visible light irradiation, it has shown a great improvement of the activity, demonstrating high potential as a photocatalyst. Full article
(This article belongs to the Special Issue Surface Science and Catalysis of Graphene-Related 2D Materials)
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14 pages, 2391 KiB  
Review
Overview of Rational Design of Binary Alloy for the Synthesis of Two-Dimensional Materials
by Hongyan Zhu, Chao Zhang, Xuefu Zhang, Zhiyuan Shi, Tianru Wu and Guanghui Yu
Surfaces 2020, 3(1), 26-39; https://doi.org/10.3390/surfaces3010003 - 15 Jan 2020
Viewed by 3815
Abstract
Two-dimensional (2D) materials attracted widespread interest as unique and novel properties different from their bulk crystals, providing great potential for semiconductor devices and applications. Recently, the family of 2D materials has been expanded including but not limited to graphene, hexagonal boron nitride ( [...] Read more.
Two-dimensional (2D) materials attracted widespread interest as unique and novel properties different from their bulk crystals, providing great potential for semiconductor devices and applications. Recently, the family of 2D materials has been expanded including but not limited to graphene, hexagonal boron nitride (h-BN), transition metal carbides (TMCs), and transition metal dichalcogenides (TMDCs). Metal-catalyzed chemical vapor deposition (CVD) is an effective method to achieve precise synthesis of these 2D materials. In this review, we focus on designing various binary alloys to realize controllable synthesis of multiple CVD-grown 2D materials and their heterostructures for both fundamental research and practical applications. Further investigations indicated that the design of the catalytic substrate is an important issue, which determines the morphology, domain size, thickness and quality of 2D materials and their heterostructures. Full article
(This article belongs to the Special Issue Surface Science and Catalysis of Graphene-Related 2D Materials)
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