Graphene-Based Microbots for Toxic Heavy Metal Removal and Recovery from Water

Heavy metal contamination in water is a serious risk to the public health and other life forms on earth. Current research in nanotechnology is developing new nanosystems and nanomaterials for the fast and efficient removal of pollutants and heavy metals from water. Here, we report graphene oxide-based microbots (GOx-microbots) as active self-propelled systems for the capture, transfer, and removal of a heavy metal (i.e., lead) and its subsequent recovery for recycling purposes. Microbots’ structure consists of nanosized multilayers of graphene oxide, nickel, and platinum, providing different functionalities. The outer layer of graphene oxide captures lead on the surface, and the inner layer of platinum functions as the engine decomposing hydrogen peroxide fuel for self-propulsion, while the middle layer of nickel enables external magnetic control of the microbots. Mobile GOx-microbots remove lead 10 times more efficiently than nonmotile GOx-microbots, cleaning water from 1000 ppb down to below 50 ppb in 60 min. Furthermore, after chemical detachment of lead from the surface of GOx-microbots, the microbots can be reused. Finally, we demonstrate the magnetic control of the GOx-microbots inside a microfluidic system as a proof-of-concept for automatic microbots-based system to remove and recover heavy metals

Graphene-Based Microbots for Toxic Heavy Metal Removal and Recovery from Water

Heavy metal contamination in water is a serious risk to the public health and other life forms on earth. Current research in nanotechnology is developing new nanosystems and nanomaterials for the fast and efficient removal of pollutants and heavy metals from water. Here, we report graphene oxide-based microbots (GOx-microbots) as active self-propelled systems for the capture, transfer, and removal of a heavy metal (i.e., lead) and its subsequent recovery for recycling purposes. Microbots’ structure consists of nanosized multilayers of graphene oxide, nickel, and platinum, providing different functionalities. The outer layer of graphene oxide captures lead on the surface, and the inner layer of platinum functions as the engine decomposing hydrogen peroxide fuel for self-propulsion, while the middle layer of nickel enables external magnetic control of the microbots. Mobile GOx-microbots remove lead 10 times more efficiently than nonmotile GOx-microbots, cleaning water from 1000 ppb down to below 50 ppb in 60 min. Furthermore, after chemical detachment of lead from the surface of GOx-microbots, the microbots can be reused. Finally, we demonstrate the magnetic control of the GOx-microbots inside a microfluidic system as a proof-of-concept for automatic microbots-based system to remove and recover heavy metals

Graphene-Based Microbots for Toxic Heavy Metal Removal and Recovery from Water

Heavy metal contamination in water is a serious risk to the public health and other life forms on earth. Current research in nanotechnology is developing new nanosystems and nanomaterials for the fast and efficient removal of pollutants and heavy metals from water. Here, we report graphene oxide-based microbots (GOx-microbots) as active self-propelled systems for the capture, transfer, and removal of a heavy metal (i.e., lead) and its subsequent recovery for recycling purposes. Microbots’ structure consists of nanosized multilayers of graphene oxide, nickel, and platinum, providing different functionalities. The outer layer of graphene oxide captures lead on the surface, and the inner layer of platinum functions as the engine decomposing hydrogen peroxide fuel for self-propulsion, while the middle layer of nickel enables external magnetic control of the microbots. Mobile GOx-microbots remove lead 10 times more efficiently than nonmotile GOx-microbots, cleaning water from 1000 ppb down to below 50 ppb in 60 min. Furthermore, after chemical detachment of lead from the surface of GOx-microbots, the microbots can be reused. Finally, we demonstrate the magnetic control of the GOx-microbots inside a microfluidic system as a proof-of-concept for automatic microbots-based system to remove and recover heavy metals

Novel Temperature/pH/CO₂/Redox-Quadruple-Responsive Ferrocene-Containing Homopolymers and Their Self-Assembly Behavior

A series of temperature/pH/CO2/redox-quadruple-responsive ferrocene-containing homopolymers were prepared for the first time. These homopolymers contain hydrophilic ethoxy group, amino group, and hydrophobic ferrocene (Fc) and were synthesized by reversible addition–fragmentation chain transfer (RAFT) polymerization. They showed four different stimuli responses. (1) They exhibit an upper critical solution temperature (UCST) in n-propyl alcohol and n-butanol, which can be adjusted by the molecular structure, molecular weight, and concentration. (2) They have a critical pH in aqueous solution and are affected by molecular structure, molecular weight, and concentration. (3) The CO2 response of the homopolymers was confirmed by cyclic bubbling CO2/N2 to the solution. (4) The redox response of homopolymers was demonstrated by adding a chemical oxidant (FeCl3)/reductant (VC) or electrical stimulation to the solution of homopolymers. In addition, these homopolymers are amphiphilic, and their self-assembly behavior in solution was investigated. It was found that they have different critical micelle concentrations (cmc) and can form lamella, sphere, and agglomerated sphere in solution, and the morphology can be reversibly changed by applying stimulation. Finally, the release behavior of micelles of the homopolymer was explored by wrapping Nile Red (NR), which proved that they had good release efficiency. These temperature/pH/CO2/redox-quadruple-responsive ferrocene-containing homopolymers expand the types of multistimuli-responsive homopolymers and have excellent application prospects in the fields of self-assembly, drug delivery, and electrode materials

Self-Assembly Evolution of <i>N</i>‑Terminal Aromatic Amino Acids with Transient Supramolecular Chirality

Deep understanding and fine tailoring of spontaneous structural evolution of self-assembled arrays are pivotal in the rational design of advanced soft materials. However, an indistinct structure–property relationship and pathway complexity in self-assembly lead to a considerable challenge. Herein, we reveal the self-assembly pathway complexity in spontaneous aggregation of several N-terminated aromatic amino acids. By primarily tuning the incubation time, building blocks appended with alanine and serine selectively form 1:1 hydrated clathrates, enabling the microfiber to transition to crystals. The dynamic water intercalation process was studied by incubation time-dependent morphological changes, powder X-ray diffraction, and single-crystal structure analysis. A pronounced amino acid residue effect on the self-assembly evolution was reflected by supramolecular chirality inversion of the building block having the phenylalanine residue, accomplishing dynamic M- to P-helicity transition within a confined time scale

Covalent Organic Frameworks Formed with Two Types of Covalent Bonds Based on Orthogonal Reactions

Covalent organic frameworks (COFs) are excellent candidates for various applications. So far, successful methods for the constructions of COFs have been limited to a few condensation reactions based on only one type of covalent bond formation. Thus, the exploration of a new judicious synthetic strategy is a crucial and emergent task for the development of this promising class of porous materials. Here, we report a new orthogonal reaction strategy to construct COFs by reversible formations of two types of covalent bonds. The obtained COFs consisting of multiple components show high surface area and high H₂ adsorption capacity. The strategy is a general protocol applicable to construct not only binary COFs but also more complicated systems in which employing regular synthetic methods did not work

A Highly Active Catalyst System for Suzuki–Miyaura Coupling of Aryl Chlorides

A series of new Pd­(II) complexes with simple structures were designed and synthesized for Suzuki–Miyaura coupling reactions of aryl chlorides. The new Pd­(II) complexes contain bidentate amine ligands, and their structures were characterized by single-crystal X-ray diffraction. They are highly efficient for Suzuki–Miyaura coupling reactions of aryl chlorides with low catalyst loadings (0.01 mol %) in aqueous media at room temperature. Two possible reaction pathways involving a PdII/0/II and a PdII/IV/II catalytic cycle are proposed, and the mechanism was further investigated using density functional theory (DFT) calculations

Integrating Suitable Linkage of Covalent Organic Frameworks into Covalently Bridged Inorganic/Organic Hybrids toward Efficient Photocatalysis

Covalent organic frameworks (COFs) are excellent platforms with tailored functionalities in photocatalysis. There are still challenges in increasing the photochemical performance of COFs. Therefore, we designed and prepared a series of COFs for photocatalytic hydrogen generation. Varying different ratios of β-ketoenamine to imine moieties in the linkages could differ the ordered structure, visible light harvesting, and bandgap. Overall, β-ketoenamine-linked COFs exhibited much better photocatalytic activity than those COFs having both β-ketoenamine and imine moieties on account of a nonquenched excited state and more favorable HOMO level in the photoinduced oxidation reaction from the former. Specifically, after in situ growth of β-ketoenamine-linked COFs onto NH2–Ti3C2Tx MXene via covalent connection, the heterohybrid showed an obvious improvement in photocatalytic H2 evolution because of strong covalent coupling, electrical conductivity, and efficient charge transfer. This integrated linkage evolution and covalent hybridization approach advances the development of COF-based photocatalysts