A Conceptual Framework to Understand the Self-Assembly of Chemically Active Colloids.

Colloids that generate chemicals, or "chemically active colloids", can interact with their neighbors and generate patterns via forces arising from such chemical gradients. Examples of such assemblies of chemically active colloids are abundant in the literature, but a unified theoretical framework is needed to rationalize the scattered results. Combining experiments, theory, Brownian dynamics, and finite element simulations, we present here a conceptual framework for understanding how immotile, yet chemically active, colloids assemble. This framework is based on the principle of ionic diffusiophoresis and diffusioosmosis and predicts that a chemically active colloid interacts with its neighbors through short- and long-range interactions that can be either repulsive or attractive, depending on the relative diffusivity of the released cations and anions, and the relative zeta potential of a colloidal particle and the planar surface on which it resides. As a result, 4 types of pairwise interactions arise, leading to 4 different types of colloidal assemblies with distinct patterns. Using short-range attraction and long-range attraction (SALR) systems as an example, we show quantitative agreement between the framework and experiments. The framework is then applied to rationalize a wide range of patterns assembled from chemically active colloids in the literature exhibiting other types of pairwise interactions. In addition, the framework can predict what the assembly looks like with minimal experimental information and help infer ionic diffusivity and zeta potential values in systems where these values are inaccessible. Our results represent a solid step toward building a complete theory for understanding and controlling chemically active colloids, from the molecular level to their mesoscopic superstructures and ultimately to the macroscopic properties of the assembled materials.

Conductive polyethersulfone membrane facilely prepared by simultaneous phase inversion method for enhanced anti-fouling and separation under low driven-pressure.

Electrically conductive membranes have been regarded as a new alternative to overcome the crucial drawbacks of membranes, including permeability-selectivity trade-off and fouling. It is still challenging to prepare conductive membranes with good mechanical strength, high conductivity and stable separation performance by reliable materials and methods. This work developed a facile method of simultaneous phase inversion to prepare electrically conductive polyethersulfone (PES) membranes with carboxylic multiwalled carbon nanotubes (MWCNT) and graphene (Gr). The resultant MWCNT/Gr/PES nanocomposite membranes are composed of the upper MWCNT/Gr layer with good conductivity and the base PES layer providing mechanical support. MWCNT as nanofillers effectively turns the insulting PES layers to be electrically conductive. With the dispersing and bridging functions of Gr, the MWCNT/Gr layer shows an enhanced electric conductivity of 0.10 S/cm. This MWCNT/Gr/PES membrane in an electro-filtration cell achieves excellent retention of Cu(II) ions up to 98 % and a high flux of 94.5 L m-2∙h-1∙bar-1 under a low driven-pressure of 0.1 MPa. The conductive membrane also shows improved anti-fouling capability during protein filtration, due mainly to the electrostatic repulsion and hydrogen evolution reaction on the electrode. This facile strategy has excellent potential in electro-assistant membrane filtration for fouling control and effective separation.

Fabrication of hydrolytically stable magnetic core-shell aminosilane nanocomposite for the adsorption of PFOS and PFOA.

Aminosilane materials, with their low cost and ease of modification, have exhibited great potential for the adsorption of perfluorinated compounds (PFCs) from water. However, this kind of material may be facing two drawbacks during its application: low resistance to hydrolysis and difficulties in separation from the water matrix. This work proposed a strategy of grafting N-(2-aminoethyl) aminopropyltrimethoxysilane (AE-APTMS) on the surface of magnetic γ-Fe2O3 nanoparticles by full utilization of the sorption sites provided by the aminosilane and the magnetism by γ-Fe2O3. The FTIR and XRD results verified the formation of the magnetic AE-APTMS nanocomposite. The core-shell nanocomposite showed a superparamagnetic property and an isoelectric point at pH = 8.2. Particularly, compared to the aminopropyltriethoxysilane (APTES) nanocomposite, the AE-APTMS nanocomposite exhibited improved hydrolytic stability with 60% less loss of the amine groups during the 48 h adsorption process, as the longer alkyl chain hindered the aminosilane detachment. The AE-APTMS nanocomposite exhibited a rapid adsorption with the removal efficiency of 78% for perfluorooctane sulfonate (PFOS) and 65% for perfluorooctanoate (PFOA) due to the electrostatic interaction and hydrophobic interaction. The regeneration and reuse of the magnetic AE-APTMS nanocomposite were conveniently realized with the removal efficiency higher than 70% for both PFOS and PFOA even after 15 adsorption-desorption cycles. The stable magnetic aminosilane nanocomposite with the ease of separation may provide a new strategy to achieve the economical and effective removal of typical PFCs from water.

Observation of Coulomb gap in the quantum spin Hall candidate single-layer 1T'-WTe2.

The two-dimensional topological insulators host a full gap in the bulk band, induced by spin-orbit coupling (SOC) effect, together with the topologically protected gapless edge states. However, it is usually challenging to suppress the bulk conductance and thus to realize the quantum spin Hall (QSH) effect. In this study, we find a mechanism to effectively suppress the bulk conductance. By using the quasiparticle interference technique with scanning tunneling spectroscopy, we demonstrate that the QSH candidate single-layer 1T'-WTe2 has a semimetal bulk band structure with no full SOC-induced gap. Surprisingly, in this two-dimensional system, we find the electron-electron interactions open a Coulomb gap which is always pinned at the Fermi energy (EF). The opening of the Coulomb gap can efficiently diminish the bulk state at the EF and supports the observation of the quantized conduction of topological edge states.

Rapid and high-capacity adsorption of PFOS and PFOA by regenerable ammoniated magnetic particle.

Adsorption is well accepted as an effective method for perfluorinated compounds' (PFCs) removal from water among various conventional methods. However, development of adsorbents that combine good performance of PFC removal and regenerability has not yet been realized. This work demonstrated the fabrication and application of an ammoniated magnetic adsorbent for efficient and economical PFOS and PFOA removal. Functional ammonium groups and γ-Fe2O3 were effectively incorporated in the particle with the proposed method. These fabricated magnetic particles presented superior adsorption performance for PFOS and PFOA with short equilibrium time of 120 min and high adsorption capacity. The isotherms revealed that the adsorption process belonged to multilayer sorption with their intricate interactions including anion exchange and hydrophobic interaction. The magnetic particle maintained its removal efficacy over a wide pH range of 3-9 or with coexisting substances. Moreover, the regeneration and reuse of the magnetic particle were successfully carried out with PFOS and PFOA removal efficiency sustained higher than 80% in 15 consecutive treatment cycles. Along with the efficient adsorption and easy separation of adsorbents, we expect that this ammoniated magnetic particle can serve as an excellent alternative for PFOS and PFOA removal from water.

Experimental Observation of Topological Edge States at the Surface Step Edge of the Topological Insulator ZrTe_{5}.

We report an atomic-scale characterization of ZrTe_{5} by using scanning tunneling microscopy. We observe a bulk band gap of ∼80 meV with topological edge states at the step edge and, thus, demonstrate that ZrTe_{5} is a two-dimensional topological insulator. We also find that an applied magnetic field induces an energetic splitting of the topological edge states, which can be attributed to a strong link between the topological edge states and bulk topology. The relatively large band gap makes ZrTe_{5} a potential candidate for future fundamental studies and device applications.