Surface Adaptive Capillarity Enabling Densified 3D Printing for Ultra‐High Areal and Volumetric Energy Density Supercapacitors

2022-03-29T13:07:33+00:00March 29th, 2022|Categories: Publications|Tags: , , |

Endowing supercapacitors with higher energy density is of great practical significance but remains extremely challenging. In this work, an innovative densified 3D printing enabled by a surface adaptive capillarity strategy is proposed for the first time. The printable ink formulated with pyrrole surface-modified reduced graphene oxide renders the printed electrodes excellent surface tension regulability to the subsequent capillary densification, creating an intensely condensed electrode with well-maintained structural integrity. Furthermore, simultaneous in-situ nitrogen doping and hierarchical micro-meso porosity are readily realized upon post-carbonization, encouraging enhanced capacitance and fast reaction dynamics. As a result, the printed symmetric supercapacitor delivers a double leap in areal and volumetric energy densities in both aqueous and organic electrolytes, a rarely achieved yet gravely desired attribute for 3D printed energy storage devices.

Published in: "Angewandte Chemie International Edition".

Enhanced photocatalytic dye degradation and hydrogen production ability of Bi$_{25}$FeO$_{40}$-rGO nanocomposite and mechanism insight. (arXiv:2202.02508v1 [cond-mat.mtrl-sci])

2022-02-08T05:29:24+00:00February 8th, 2022|Categories: Publications|Tags: , |

A comprehensive comparison between Bi$_{25}$FeO$_{40}$-reduced graphene oxide(rGO) nanocomposite and BiFeO$_{3}$-rGO nanocomposite has been performed to investigate their photocatalytic abilities in degradation of Rhodamine B dye and generation of hydrogen by water-splitting. The hydrothermal technique adapted for synthesis of the nanocomposites provides a versatile temperature-controlled phase selection between perovskite BiFeO$_{3}$ and sillenite Bi$_{25}$FeO$_{40}$. Both perovskite and sillenite structured nanocomposites are stable and exhibit considerably higher photocatalytic ability over pure BiFeO$_{3}$ nanoparticles and commercially available Degussa P25 titania. Notably, Bi$_{25}$FeO$_{40}$- rGO nanocomposite has demonstrated superior photocatalytic ability and stability under visible light irradiation than that of BiFeO$_{3}$-rGO nanocomposite. The possible mechanism behind the superior photocatalytic performance of Bi$_{25}$FeO$_{40}$-rGO nanocomposite has been critically discussed.

Published in: "arXiv Material Science".

Unexpectedly Spontaneous Water Dissociation on Graphene Oxide Supported by Copper Substrate. (arXiv:2202.02746v1 [cond-mat.mtrl-sci])

2022-02-08T05:29:20+00:00February 8th, 2022|Categories: Publications|Tags: , |

Water dissociation is of fundamental importance in scientific fields and has drawn considerable interest in diverse technological applications. However, the high activation barrier of breaking the O-H bond within the water molecule has been identified as the bottleneck, even for the water adsorbed on the graphene oxide (GO). Herein, using the density functional theory calculations, we demonstrate that the water molecule can be spontaneously dissociated on GO supported by the (111) surface of the copper substrate (Copper-GO). This process involves a proton transferring from water to the interfacial oxygen group, and a hydroxide covalently bonding to GO. Compared to that on GO, the water dissociation barrier on Copper-GO is significantly decreased to be less than or comparable to thermal fluctuations. This is ascribed to the orbital-hybridizing interaction between copper substrate and GO, which enhances the reaction activity of interfacial oxygen groups along the basal plane of GO for water dissociation. Our work provides a novel strategy to access water dissociation via the substrate-enhanced reaction activity of interfacial oxygen groups on GO and indicates that the substrate can serve as an essential key to tune the catalytic performance of various two-dimensional material devices.

Published in: "arXiv Material Science".

A multi-interface CoNi-SP/C heterostructure for quasi-solid-state hybrid supercapacitors with a graphene oxide-containing hydrogel electrolyte

2022-02-04T15:21:08+00:00February 4th, 2022|Categories: Publications|Tags: , , , |

J. Mater. Chem. A, 2022, Advance ArticleDOI: 10.1039/D1TA10138B, PaperZixiao Li, Chenchen Ji, Fengjiao Guo, Hongyu Mi, Xiaoqing Zhu, Jieshan QiuA quasi-solid-state HSC was assembled by a reasonable multi-phase hybrid material and a novel high ionic conductivity hydrogel electrolyte, which exhibited excellent energy/power density

Published in: "Journal of Materials Chemistry A".

FeCl3-functionalized graphene oxide/single-wall carbon nanotube/silicon heterojunction solar cells with an efficiency of 17.5%

2022-02-04T15:21:02+00:00February 4th, 2022|Categories: Publications|Tags: , |

J. Mater. Chem. A, 2022, Accepted ManuscriptDOI: 10.1039/D2TA00217E, PaperXian-Gang Hu, Qinwei Wei, Yi-Ming Zhao, Peng-Xiang Hou, Wencai Ren, Chang Liu, Hui-Ming ChengSingle-wall carbon nanotube/silicon (SWCNT/Si) heterojunction solar cells are no longer a laboratory curiosity, but the commercial manufacture of devices with a high

Published in: "Journal of Materials Chemistry A".

Fabrication of impermeable dense architecture containing covalently stitched graphene oxide/boron nitride hybrid nanofiller reinforced semi-interpenetrating network for hydrogen gas barrier applications

2022-02-04T15:20:47+00:00February 4th, 2022|Categories: Publications|Tags: , , |

J. Mater. Chem. A, 2022, Advance ArticleDOI: 10.1039/D1TA09486F, PaperSubhabrata Saha, Wansu Son, Nam Hoon Kim, Joong Hee LeeThe GO-BN hybrid nanofiller reinforced TPU/epoxy semi-interpenetrating network provided an excellent H2 barrier coating along with superior adhesion for the nylon 6 based compressed H2 storage

Published in: "Journal of Materials Chemistry A".

Mass transport via in-plane nanopores in graphene oxide membranes. (arXiv:2201.11886v1 [cond-mat.mtrl-sci])

2022-01-31T02:29:17+00:00January 31st, 2022|Categories: Publications|Tags: , |

Angstrom confined solvents in two-dimensional laminates travel through interlayer spacings, gaps between adjacent sheets, and via in plane pores. Among these, experimental access to investigate the mass transport through in plane pores is lacking. Here, we create these nanopores in graphene oxide membranes via ion irradiation with precise control over functional groups, pore size and pore density. Low ion induced pore densities result in mild reduction and increased water permeation for the membranes. Higher pore densities lead to pronounced reduction and complete blockage of pure water however allows permeation of ethanol water mixture due to weakening of hydrogen network. We confirm with simulations, that the attraction of the solvents towards the pores with functional groups and disruption of the angstrom confined hydrogen network is crucial to allow in plane pore transport.

Published in: "arXiv Material Science".

Layered Biomimetic Composites from MXenes with Sequential Bridging

2022-01-20T13:07:51+00:00January 20th, 2022|Categories: Publications|Tags: , |

Layered nanocomposites fabricated by techniques other than layer-by-layer assembly (e.g. vacuum-assisted filtration and blade coating) contain voids in their structure, which reduces their performance. Cheng and co-workers have now found that the problem of voids in Ti3C2T x MXene composites can be solved by sequential bridging of MXEne platelets with sodium carboxymethyl cellulose combined with covalent bridging by borate ions. Abstract Layer-by-layer (LbL) assembly is a widely used technique for the self-assembly of layered nanocomposites from clay sheets, carbon nanotubes, graphene oxide, nanoparticles, and other materials. Other approaches for fabricating layered nanocomposites include vacuum-assisted filtration and blade coating. They are simpler than LbL assembly, but they all introduce voids into the layered structure, thereby reducing the performance of the resulting nanocomposites. A team from Beihang University evaluated the void structure in Ti3C2T x MXene composites and found that the fundamental problem with voids can be solved by the sequential nanoscale bonding of MXEne platelets with sodium carboxymethyl cellulose combined with covalent bridging with borate ions, thereby opening a new path to self-assemble two-dimensional platelets into continuous high-performance layered nanocomposites.

Published in: "Angewandte Chemie International Edition".

Chemically edge-carboxylated graphene enhances thermal conductivity of polyetherimide-graphene nanocomposites. (arXiv:2201.03395v1 [cond-mat.mtrl-sci])

2022-01-11T02:29:49+00:00January 11th, 2022|Categories: Publications|Tags: , |

In this work, we demonstrate that edge-oxidation of graphene nanoplatelets (GnPs) can enable a larger enhancement of effective thermal conductivity (k) in polyetherimide (PEI)-graphene nanocomposites, relative to basal plane functionalization. Edge oxidation is achieved in this work by using a chemical scheme (recently introduced) involving oxidizing graphene in presence of sodium chlorate and hydrogen peroxide, introducing an excess of carboxyl groups on the edge of graphene. Edge oxidation offers the advantage of preserving the high in-plane thermal conductivity of graphene (kin > 2000 W/mK)), while also coupling polymer to this high-in plane thermal conduction pathway of graphene. Carboxyl-moieties on edge-oxidized graphene enhance interfacial thermal transport by interacting with oxygen groups on polyetherimide through hydrogen bonding, resulting in enhancement of overall composite thermal conductivity. Basal-plane oxidation of graphene, on the other hand, achieved through modified Hummers method, distorts sp2 carbon-carbon network of graphene lowering its intrinsic thermal conductivity. The resulting thermal conductivity of edge-oxidized GnP/PEI composite is found to be enhanced by 18%, whereas that of basal-plane functionalized GnP/PEI composite is diminished by 57%, with respect to pristine GnP/PEI composite for 10 weight% filler content. 2-dimensional Raman spectroscopy of individual graphene nanoplatelets is used to confirm and distinguish the location of oxygen functional groups on graphene. Presented results can lead to fundamentally novel pathways for achieving high thermal-conductivity polymer composites.

Published in: "arXiv Material Science".

Frontispiece: Near‐Equilibrium Growth of Chemically Stable Covalent Organic Framework/Graphene Oxide Hybrid Materials for the Hydrogen Evolution Reaction

2022-01-05T13:07:39+00:00January 5th, 2022|Categories: Publications|Tags: , |

Covalent Organic Frameworks Near-equilibrium growth of chemically stable covalent organic framework–graphene oxide hybrid materials for the hydrogen evolution reaction is reported in the Communication by Jianyi Chen, Jichen Dong, Yunqi Liu et al. (e202113067).

Published in: "Angewandte Chemie International Edition".

Covalent Organic Functionalization of Graphene Nanosheets and Reduced Graphene Oxide via 1,3-Dipolar Cycloaddition of Azomethine Ylide. (arXiv:2112.12505v1 [cond-mat.mtrl-sci])

2021-12-24T02:29:31+00:00December 24th, 2021|Categories: Publications|Tags: , , |

Organic functionalization of graphene is successfully performed via 1,3-dipolar cycloaddition of azomethine ylide in the liquid phase. The comparison between 1-methyl-2-pyrrolidinone and N,N-dimethylformamide as dispersant solvents, and between sonication and homogenization as dispersion techniques, proves N,N-dimethylformamide and homogenization as the most effective choice. The functionalization of graphene nanosheets and reduced graphene oxide is confirmed using different techniques. Among them, energy-dispersive X-ray spectroscopy allows to map the pyrrolidine ring of the azomethine ylide on the surface of functionalized graphene, while micro-Raman spectroscopy detects new features arising from the functionalization, which are described in agreement with the power spectrum obtained from ab initio molecular dynamics simulation. Moreover, X-ray photoemission spectroscopy of functionalized graphene allows the quantitative elemental analysis and the estimation of the surface coverage, showing a higher degree of functionalization for reduced graphene oxide. This more reactive behavior originates from the localization of partial charges on its surface due to the presence of oxygen defects, as shown by the simulation of the electrostatic features. Functionalization of graphene using 1,3-dipolar cycloaddition is shown to be a significant step towards the controlled synthesis of graphene-based complex structures and devices at the nanoscale.

Published in: "arXiv Material Science".

Sarin filtration by porous rGO membrane: a molecular dynamics study. (arXiv:2112.03830v1 [cond-mat.mtrl-sci])

2021-12-08T02:29:33+00:00December 8th, 2021|Categories: Publications|Tags: , |

Sarin is a very lethal synthetic organophosphorated compound that inhibits the nervous system muscle control. Although not used as a chemical weapon anymore, it is still worries the authorities regarding possible use by terrorists. Most of the studies about sarin are theoretical/computational, due to its high lethality, and concentrate in its detection and degradation. Few studies are about sarin filtration. Here, the potential of graphene oxide-based membranes to filter sarin molecules is studied by classical molecular dynamics simulations. Membranes formed by one and two nanosheets of porous reduced graphene oxide (rGO) were considered. The passage of sarin and air molecules from a highly concentrated region to an empty one, separated by these membranes, is evaluated as a function of temperature and sarin/air relative concentration. Sarin molecules are shown to be trapped by hydroxyl and carboxyl chemical groups in the nanosheet, while a considerable passage of air molecules (N2, O2 and Ar) through the membranes was verified. These results show the capacity of the rGO membrane systems to retain sarin from passing through, even at high temperatures, thus indicating their potential to be used as a filter for sarin gas.

Published in: "arXiv Material Science".

Modeling of nucleobase/oligonucleotide interaction with graphene and graphene oxide: the role of charging and/or oxidizing the graphene surface. (arXiv:2111.14435v1 [physics.bio-ph])

2021-11-30T04:30:29+00:00November 30th, 2021|Categories: Publications|Tags: , , |

We analyze the influence of the charge and the degree of oxidation of the surface of graphene (Gr) on its interaction with cytosine and oligonucleotide r(C)10. This is a computational study involving DFT calculations and molecular dynamics simulations. It is shown that cytosine interacts stronger with graphene oxide (GO) than with Gr, while the energy of the interaction of cytosine with GO only weakly depends on the degree of the Gr oxidation. A correlation between the shifts of vibrational frequencies of cytosine due to complexation with GO and the degree of the Gr oxidation is found. The adsorption of anionic oligonucleotide r(C)10 onto neutral and positively charged surfaces has a certain conformational similarity to conformations formed with similar van der Waals interactions. Also, for charged surfaces, the Coulombic attraction gives a noticeable contribution to the total interaction energy. For a negatively charged graphene surface the electrostatic repulsion between Gr surface and negatively charged phosphate backbone of oligonucleotide weakens the total binding energy. Competition between the Coulombic repulsion and the van der Waals attraction results in formation of a unique oligonucleotide conformation where all 10 cytosines are stacked onto Gr.

Published : "arXiv Mesoscale and Nanoscale Physics".

DNAzyme‐Functionalized Nanomaterials: Recent Preparation, Current Applications, and Future Challenges

2021-11-26T13:23:47+00:00November 26th, 2021|Categories: Publications|Tags: , , |

Here, DNAzymes functionalized with metal–organic frameworks (MOFs), gold nanoparticles (AuNPs), graphene oxide (GO), and molybdenum disulfide (MoS2) are introduced and summarized in detail. Moreover, the focus is on its biomedical applications, such as bioimaging, biosensor development, drug delivery, and cancer therapy in recent years. Abstract DNAzyme–nanomaterial bioconjugates are a popular hybrid and have received major attention for diverse biomedical applications, such as bioimaging, biosensor development, cancer therapy, and drug delivery. Therefore, significant efforts are made to develop different strategies for the preparation of inorganic and organic nanoparticles (NPs) with specific morphologies and properties. DNAzymes functionalized with metal–organic frameworks (MOFs), gold nanoparticles (AuNPs), graphene oxide (GO), and molybdenum disulfide (MoS2) are introduced and summarized in detail in this review. Moreover, the focus is on representative examples of applications of DNAzyme–nanomaterials over recent years, especially in bioimaging, biosensing, phototherapy, and stimulation response delivery in living systems, with their several advantages and drawbacks. Finally, the perspective regarding the future directions of research addressing these challenges is also discussed and highlighted.

Published in: "Small".

CO2-selective zeolitic imidazolate framework membrane on graphene oxide nanoribbons: experimental and theoretical studies

2021-11-26T13:11:45+00:00November 26th, 2021|Categories: Publications|Tags: , |

J. Mater. Chem. A, 2021, 9,25595-25602DOI: 10.1039/D1TA08340F, PaperEunji Choi, Sung Jun Hong, Junhe Chen, Yeong Jae Kim, Yunkyu Choi, Ohchan Kwon, Kiwon Eum, Ji Il Choi, Seung Soon Jang, Byungchan Han, Dae Woo KimA CO2 selective ZIF-8 membrane can be fabricated on a

Published in: "Journal of Materials Chemistry A".

Electrochemical reduction of thin graphene-oxide films in aqueous solutions: restoration of conductivity. (arXiv:2111.10081v1 [physics.app-ph])

2021-11-22T02:29:19+00:00November 22nd, 2021|Categories: Publications|Tags: , , |

Graphene oxide finds applications in different fields of science, including energy conversion. Electrochemical reduction of graphene oxide (GO) significantly improves its conductivity. However, the kinetics of this process depends on the solvent, supporting electrolyte, pH, and numerous other factors. Most studies report the macroscopic views and ex-situ properties of reduced GO. To expand the knowledge about GO reduction, in this study, we used cyclic voltammetry (CV), simultaneous 2 points and 4 points resistance measurement (s24), conductive atomic force microscopy (AFM), and theoretical calculations. Using CV, we demonstrated that the choice of supporting electrolyte (KCl or LiCl) influences the potential range in which electrochemical GO reduction occurs. The activation energy of this process was estimated to be below 30 kJ mol-1 in both electrolytes, being significantly lower than that required for thermal reduction of GO. Simultaneous in situ s24 resistance measurements suggest that GO films reach a highly conductive state at deep negative potentials, with an abrupt, irreversible switch from non-conductive to the conductive state. However, conductive AFM presents a more exact picture of this process: the reduction of GO films starts locally while the formed conductive islands grow during the reduction. This mechanism was confirmed by theoretical calculations indicating that the reduction starts on isolated oxygen-functional groups over the GO basal plane, while clustered OH groups are more difficult to reduce. The presented results can help in tailoring reduced GO for a particular electrochemical application by precisely controlling the reduction degree and percentage of the conductive area of the reduced

Published in: "arXiv Material Science".

Chlorine-free electrochemical disinfection using graphene sponge electrodes. (arXiv:2111.05252v1 [cond-mat.mtrl-sci])

2021-11-10T02:29:23+00:00November 10th, 2021|Categories: Publications|Tags: , |

Graphene sponge electrodes were employed for chlorine-free inactivation of Escherichia coli from low conductivity water. The nitrogen-doped reduced graphene oxide (NRGO) sponge anode bearing more positive charge achieved complete E. coli inactivation (i.e., 5 log removal) in the anode-cathode configuration at 115 A m-2, versus 2.6 log removal using boron-doped reduced graphene oxide sponge anode. The bacteria were mainly inactivated via electrosorption and electroporation, as confirmed by the scanning electron microscopy. Storage of the electrochemically treated samples revealed further killing of the bacteria due to the damaged cell membranes. When using real tap water, 5.5 log E. coli removal required 5.70 kWh m-3, which was drastically lowered to 1.38 kWh m-3 using intermittent current and thus exploiting the capacitive properties of graphene. The developed graphene sponge anode does not form any chlorine, chlorate, or perchlorate, and holds great promise for efficient electro-disinfection without forming toxic disinfection byproducts.

Published in: "arXiv Material Science".

Nonmonotonic magnetic field dependence of remanent ferroelectric polarization in reduced-graphene-oxide-BiFeO$_3$ nanocomposite. (arXiv:2110.06519v1 [cond-mat.mtrl-sci])

2021-10-14T02:29:32+00:00October 14th, 2021|Categories: Publications|Tags: , , |

In a nanocomposite of reduced graphene oxide (RGO) and BiFeO$_3$ (BFO), the remanent ferroelectric polarization is found to follow nonmonotonic magnetic field dependence at room temperature as the applied magnetic field is swept across 0-20 kOe on a pristine sample. The remanent ferroelectric polarization is determined both from direct electrical measurements on an assembly of nanoparticles and powder neutron diffraction patterns recorded under 0-20 kOe field. The nanosized ($sim$20 nm) particles of BFO are anchored onto the graphene sheets of RGO via Fe-C bonds with concomitant rise in covalency in the Fe-O bonds. The field-dependent competition between the positive and negative magnetoelectric coupling arising from magnetostriction due to, respectively, interface and bulk magnetization appears to be giving rise to the observed nonmonotonic field dependence of polarization. The emergence of Fe-C bonds and consequent change in the magnetic and electronic structure of the interface region has influenced the coupling between ferroelectric and magnetic properties remarkably and thus creates a new way of tuning the magnetoelectric properties via reconstruction of interfaces in nanocomposites or heterostructures of graphene/single-phase-multiferroic systems.

Published in: "arXiv Material Science".

Some say, that 2D Research is the best website in the world.