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1.
Nat Commun ; 14(1): 901, 2023 Feb 17.
Article in English | MEDLINE | ID: mdl-36797272

ABSTRACT

Layered two-dimensional materials can potentially be utilized for organic solvent nanofiltration (OSN) membrane fabrication owing to their precise molecular sieving by the interlayer structure and excellent stability in harsh conditions. Nevertheless, the extensive tortuosity of nanochannels and bulky solvent molecules impede rapid permeability. Herein, nanoporous graphene (NG) with a high density of sp2 carbon domain was synthesized via sequential thermal pore activation of graphene oxide (GO) and microwave-assisted reduction. Due to the smooth sp2 carbon domain surfaces and dense nanopores, the microwave-treated nanoporous graphene membrane exhibited ultrafast organic solvent permeance (e.g., IPA: 2278 LMH/bar) with excellent stability under practical cross-flow conditions. Furthermore, the membrane molecular weight cut-off (MWCO) is switchable from 500 Da size of molecule to sub-nanometer-size molecules depending on the solvent type, and this switching occurs spontaneously with solvent change. These properties indicate feasibility of multiple (both binary and ternary) organic mixture separation using a single membrane. The nanochannel structure effect on solvent transport is also investigated using computation calculations.

2.
ACS Appl Mater Interfaces ; 14(10): 12140-12148, 2022 Mar 16.
Article in English | MEDLINE | ID: mdl-35238550

ABSTRACT

The strong bonding at the interface between the metal and the support, which can inhibit the undesirable aggregation of metal nanoparticles and carbon deposition from reforming of hydrocarbon, is well known as the classical strong metal-support interaction (SMSI). SMSI of nanocatalysts was significantly affected by heat treatment and reducing conditions during catalyst preparation.the heat treatment and reduction conditions during catalyst preparation. SMSI can be weakened by the decrement of metal-doped sites in the supporting oxide and can often deactivate catalysts by the encapsulation of active sites through these processes. To retain SMSI near the active sites and to enhance the catalytic activity of the nanocatalyst, it is essential to increase the number of surficial metal-doped sites between nanometal and the support. Herein, we propose a mild reduction process using dry methane (CH4/CO2) gas that suppresses the aggregation of nanoparticles and increases the exposed interface between the metal and support, Ni and cerium oxide. The effects of mild reduction on the chemical state of Ni-cerium oxide nanocatalysts were specifically investigated in this study. As a result, mild reduction led to form large amounts of the Ni3+ phase at the catalyst surface of which SMSI was significantly enhanced. It can be easily fabricated while the dry reforming of methane (DRM) reaction is on stream. The superior performance of the catalyst achieved a considerably high CH4 conversion rate of approximately 60% and stable operation up to 550 h at a low temperature, 600 °C.

3.
ACS Appl Mater Interfaces ; 14(9): 11779-11788, 2022 Mar 09.
Article in English | MEDLINE | ID: mdl-35192336

ABSTRACT

Hybrids based on carbon nanotubes (CNTs) and graphene nanoribbons (GNRs) are expected to have synergistic effects for various applications. Herein, we demonstrate a simple one-pot synthesis of a CNT/GNR hybrid material by adjusting the oxidation and unzipping conditions of multi-walled CNTs (MWNTs). The MWNT/graphene oxide nanoribbon (GONR) hybrid was dispersed in various solvents, particularly showing the hybrid hydrogel phase in water at a concentration of 40 mg mL-1. The MWNT/GONR hydrogel exhibited shear-thinning behavior, which can be beneficial for coating a large-area MWNT/GONR layer onto a polymeric porous support by using a scalable slot-die coater. The MWNT/GONR membrane exhibited an outstanding nanofiltration performance, with a molecular weight cutoff of 300 Da and a dye/salt diafiltration performance with a separation factor of 1000 and a water flux of 367.8 LMH, far surpassing the upper bound of diafiltration performance of the existing membranes.

4.
Chem Commun (Camb) ; 57(70): 8730-8733, 2021 Sep 11.
Article in English | MEDLINE | ID: mdl-34369528

ABSTRACT

H2 selective dense pores are generated in a graphene oxide (GO) layer by thermal-decomposition of oxygen-functional groups under high pressure. The nanoporous GO membrane shows H2/CO2 selectivity of 12.1 and H2 permeability of 10360 Barrer.

5.
ACS Nano ; 14(9): 12195-12202, 2020 09 22.
Article in English | MEDLINE | ID: mdl-32885959

ABSTRACT

The preparation of carbon materials based hydrogels and their viscoelastic properties are essential for their broad application and scale-up. However, existing studies are mainly focused on graphene derivatives and carbon nanotubes, and the behavior of graphene nanoribbon (GNR), a narrow strip of graphene, remains elusive. Herein, we demonstrate the concentration-driven gelation of oxidized GNR (graphene oxide nanoribbon, GONR) in aqueous solvents. Exfoliated individual GONRs sequentially assemble into strings (∼1 mg/mL), nanoplates (∼20 mg/mL), and a macroporous scaffold (50 mg/mL) with increasing concentration. The GONR hydrogels exhibit viscoelastic shear-thinning behavior and can be shear-coated to form large-area GONR films on substrates. The entangled and stacked structure of the GONR film contributed to outstanding nanofiltration performance under high pressure, cross-flow, and long-term filtration, while the precise molecular separation with 100% rejection rate was maintained for sub-nanometer molecules.

6.
Sci Rep ; 9(1): 3175, 2019 Feb 28.
Article in English | MEDLINE | ID: mdl-30816119

ABSTRACT

First ever transparent bendable secondary zinc-air batteries were fabricated. Transparent stainless-steel mesh was utilized as the current collector for the electrodes due to its reliable mechanical stability and electrical conductivity. After which separate methods were used to apply the active redox species. For the preparation of the anode, zinc was loaded by an electroplating process to the mesh. For the cathode, catalyst ink solution was spray coated with an airbrush for desired dimensions. An alkaline gel electrolyte layer was used for the electrolyte. Microscale domain control of the materials becomes a crucial factor for fabricating transparent batteries. As for the presented cell, anionic exchange polymer layer has been uniquely incorporated on to the cathode mesh as the separator which becomes a key procedure in the fabrication process for obtaining the desired optical properties of the battery. The ionic resin is applied in a fashion where controlled voids exist between the openings of the grid which facilitates light passage while guaranteeing electrical insulation between the electrodes. Further analysis correlates the electrode dimensions to the transparency of the system. Recorded average light transmittance is 48.8% in the visible light region and exhibited a maximum power density of 9.77 mW/cm2. The produced battery shows both transparent and flexible properties while maintaining a stable discharge/charge operation.

7.
RSC Adv ; 9(11): 6320-6327, 2019 Feb 18.
Article in English | MEDLINE | ID: mdl-35517288

ABSTRACT

Methanol is an attractive energy source due to its portability and thermodynamic coke resistance by its oxygen content. In order to operate dry methanol fuel low temperature solid oxide fuel cells (LT-SOFCs), it is important to solve the problems of carbon formation and its low performance. In this study, copper impregnation was selected to decrease the carbon deposition and enhance the performance at low temperature. The interaction of copper, ceria and nickel improves CO oxidation capacity which improves coke tolerance and nano-sized nickel copper alloys improved durability and catalytic performance under methanol feed. It markedly amplified the performance about 0.4 W cm-2 at 550 °C with the durable operation at 1.4 A cm-2 over 50 h. Loading copper nanoparticles is promising method for Ni-ceria based LT-SOFC using methanol fuel with high performance and stable operation.

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