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ACS Appl Mater Interfaces 2022 May 26. Epub 2022 May 26.

School of Chemistry and Chemical Engineering, Institute for Innovative Materials and Energy, Yangzhou University, Yangzhou 225009, Jiangsu, P. R. China.

Metal-organic frameworks (MOFs) are promising electrochemical materials that possess large specific surface areas, high porosities, good adjustability, and high activities. However, many conventional MOFs exhibit poor conductivity, which hinders their application in electrochemistry. In recent years, conductive MOFs (cMOFs) have attracted a considerable attention. Read More

ACS Appl Mater Interfaces 2022 May 26. Epub 2022 May 26.

Institute of Physics, Universidade Federal de Mato Grosso do Sul, CP 549, 79070-900 Campo Grande, Mato Grosso do Sul, Brazil.

The combination of energy and chemical conversion can be achieved by designing glycerol fuel cells. However, the anode must promote the reaction at onset potentials low enough to allow a spontaneous reaction, when coupled to the cathodic reaction, and must be selective. Here, we build a three-dimensional (3D)-printed glycerol microfluidic fuel cell that produces power concomitantly to glycolate and formate at zero bias. Read More

ACS Appl Mater Interfaces 2022 May 26. Epub 2022 May 26.

ACS Appl Mater Interfaces 2022 May 26. Epub 2022 May 26.

Institute of Advanced Composite Materials, Korea Institute of Science and Technology, Joellabuk-do 55324, South Korea.

Two-dimensional transition-metal dichalcogenide (TMD) materials have attracted increasing attention in efforts to overcome fundamental issues faced by the complementary metal-oxide-semiconductor industry. Multilayer TMD materials such as MoS can be used for high-performance transistor-based applications; the drive currents are high and the materials handle low-frequency (LF) noise well. We fabricated double-gated multilayer MoS transistors using the h-BN dielectric for the top gate and silicon dioxide for the bottom gate. Read More

ACS Nano 2022 May 26. Epub 2022 May 26.

Institute of Burn Research, State Key Laboratory of Trauma, Burn and Combined Injury, Southwest Hospital, Third Military Medical University (Army Medical University), Chongqing 400038, China.

Excessive extracellular matrix deposition drives fibroblasts into a state of high mechanical stress, exacerbating pathological fibrosis and hypertrophic scar formation, leading to tissue dysfunction. This study reports a minimally invasive and convenient approach to obtaining scarless tissue using a silk fibroin microneedle patch (SF MNs). We found that by tuning the MN size and density only, the biocompatible MNs significantly decreased the scar elevation index in the rabbit ear hypertrophic scar model and increased ultimate tensile strength close to regular skin. Read More

ACS Appl Mater Interfaces 2022 May 26. Epub 2022 May 26.

NanoEngineering Group, Mechanical Engineering Faculty, Technion - Israel Institute of Technology, 32000 Haifa, Israel.

Developing new underwater glue adhesives with robust and repeatable adhesion to various surfaces is promising and useful in marine life and medical treatments. In this work, we developed a novel glue based on a copolymer with a cation--aromatic sequence where the cationic units contain both catechol and positively charged sites. The glue consists of a crosslinked copolymer of poly(2-hydroxy-3-phenoxypropyl acrylate--3-(5-(3,4 dihydroxyphenyl)-4-oxo-3 -pentyl)imidazolium) bromide in dimethyl sulfoxide. Read More

ACS Appl Mater Interfaces 2022 May 26. Epub 2022 May 26.

Chemistry and Physics of Interfaces, Department of Microsystems Engineering - IMTEK, University of Freiburg, 79110 Freiburg, Germany.

Current developments in precision medicine require the simultaneous detection of an increasing number of biomarkers in heterogeneous, complex solutions, such as blood samples. To meet this need, immunoassays on barcoded hydrogel beads have been proposed, although the encoding and decoding of these barcodes is usually complex and/or resource-intensive. Herein, an efficient method for the fabrication of barcoded, functionalized hydrogel beads is presented. Read More

ACS Macro Lett 2020 Nov 20;9(11):1558-1562. Epub 2020 Oct 20.

School of Chemistry and Chemical Engineering, Nantong University, Nantong, Jiangsu 226019, People's Republic of China.

With the rapid progress of nanotechnology, near-infrared (NIR), light-assisted phototherapy as a minimally invasive local cancer therapy, especially photothermal therapy (PTT), has captured broad research attention in recent years. However, combined target molecules with a PTT system through reversible supramolecular interactions has been reported rarely. In this work, we constructed a supramolecular nanosystem combining ATP capture and target PTT based on cationic pillar[5]arene (CWP5)-functionalized CuSe nanoparticles ([email protected] NPs). Read More

ACS Macro Lett 2020 Nov 20;9(11):1552-1557. Epub 2020 Oct 20.

Department of Chemistry, The University of Cincinnati, P.O. Box 210172, Cincinnati, Ohio 45221, United States.

Wavelength-dependent light-responsive seleno-sulfide dynamic covalent bonds were used to prepare organogels with reversible changes in stiffness. The disulfide cross-link organogels prepared from norbornene-terminated poly(ethylene glycol) (PEG-diNB) and poly(2-hydroxypropyl methacrylate--mercaptoethyl acrylate) (PEG-diNB-poly(HPMA--MEMA)) polymers underwent exchange reactions with 5,5'-diselenide-bis(2-aminobenzoic acid) upon irradiation with UV light. Following irradiation with visible light, the seleno-sulfide bonds were cleaved, reforming disulfide cross-links and the 5,5'-diselenide-bis(2-aminobenzoic acid). Read More

ACS Macro Lett 2020 Nov 19;9(11):1547-1551. Epub 2020 Oct 19.

Tianjin Key Laboratory of Molecular Optoelectronic Science, Department of Chemistry, Tianjin University, Tianjin 300354, P. R. China.

A series of Se-Se-linked polystyrenes have been synthesized and subjected to pulse sonication. Comprehensive investigations based on GPC measurements, derivatization experiments, and EPR spectroscopy verify the sonication-induced bond scission and metathesis of these polymeric diselenides. The metathesis kinetics and energy conversion efficiency by different stimuli including heating, light, and sonication are compared, which demonstrate that sonication can offer an alternative way to break the Se-Se bond and realize selective metathesis reactions between diselenide-linked polymers and small molecules. Read More

ACS Macro Lett 2020 Nov 19;9(11):1542-1546. Epub 2020 Oct 19.

Department of Polymer Science, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, People's Republic of China.

Nontraditional polyurethane (PU) has been successfully synthesized by anionic copolymerization of some typical aryl isocyanates and epoxides with ammonium halide onium salt (Lewis base) as the initiator and triisobutylaluminum (Lewis acid) as the activator and the synergistic coordinator. In contrast to the traditional step-growth approach, this chain-growth copolymerization can maintain the anionic propagation site and exhibit some living features with a high activity, by which the copolymers synthesized have narrow molecular weight distributions and discrete end groups. The copolymer is primarily constituted by a urethane linkage, and the byproducts of isocyanurate trimer and oxazolidinone can be effectively suppressed as the polymerization proceeds. Read More

ACS Macro Lett 2020 Nov 14;9(11):1521-1526. Epub 2020 Oct 14.

Department of Physics, Hong Kong University of Science and Technology, Hong Kong, China.

Elastic moduli, , of free-standing polystyrene (PS) single-layers and polystyrene-polydimethylsiloxane (PS-PDMS) bilayers are measured by uniaxial tensile testing at room temperature under different strain rates, γ̇, and for PS thicknesses, , from 8 to 130 nm. As γ̇ increases, increases initially, then approaches the bulk value, , when γ̇ exceeds a characteristic value (≡ τ) that decreases with increasing . The noted variation of with γ̇ shows that stress relaxation occurs in the films during measurement when γ̇τ ≪ 1, while the noted variation of τ with shows that thinner films relax faster. Read More

ACS Macro Lett 2020 Nov 13;9(11):1514-1520. Epub 2020 Oct 13.

School of Chemistry, University of Bristol, Cantock's Close, Bristol, BS8 1TS, United Kingdom.

The formation of colloids with anisotropically patterned surfaces is of growing interest for the creation of hierarchical structures and the templating of nanoparticles. We have recently shown that well-defined two-dimensional platelets with low areal dispersities can be formed by the seeded growth of a blend of homopolymers and block copolymers. Herein we form rectangular platelets containing two block copolymers with different coronal chemistries. Read More

ACS Macro Lett 2020 Nov 13;9(11):1507-1513. Epub 2020 Oct 13.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Center for Advanced Low-Dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

Fiber-based linear actuators (FLAs) are a key module in microrobots and biomimetic devices. It has been a great challenge to develop linear actuators that can balance output stress and output strain and hence provide high working density. Herein, we report the preparation and performance of a FLA system made from commercially available materials and allowed mass production at relatively low cost. Read More

ACS Macro Lett 2020 Nov 8;9(11):1709-1717. Epub 2020 Nov 8.

McKetta Department of Chemical Engineering, The University of Texas at Austin, 200 East Dean Keeton Street, Austin, Texas 78712, United States.

Treatment of nontraditional source waters (e.g., produced water, municipal and industrial wastewaters, agricultural runoff) offers exciting opportunities to expand water and energy resources via water reuse and resource recovery. Read More

ACS Macro Lett 2020 Nov 28;9(11):1638-1654. Epub 2020 Oct 28.

Department of Chemistry, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States.

The thermomechanical properties exhibited by synthetic macromolecules can be directly linked to their tacticity, or the relative stereochemistry of repeat units. The development of stereoselective coordination-insertion polymerization, for example, led to the discovery of isotactic polypropylene, now one of the most widely produced commodity plastics in the world. Widespread interest in controlling polymer tacticity has led to a variety of stereoselective polymerization methodologies; however, this area of polymer science has lagged behind when compared to the ability to control molecular weight, dispersity, and composition. Read More

ACS Macro Lett 2020 Nov 5;9(11):1590-1603. Epub 2020 Nov 5.

Department of Chemical and Biomolecular Engineering, Rice University, Houston, Texas 77005, United States.

Bioelectronics brings together the fields of biology and microelectronics to create multifunctional devices with the potential to address longstanding technological challenges and change our way of life. Microbial electrochemical devices are a growing subset of bioelectronic devices that incorporate naturally occurring or synthetically engineered microbes into electronic devices and have broad applications including energy harvesting, chemical production, water remediation, and environmental and health monitoring. The goal of this Viewpoint is to highlight recent advances and ongoing challenges in the rapidly developing field of microbial bioelectronic devices, with an emphasis on materials challenges. Read More

ACS Macro Lett 2020 Nov 16;9(11):1527-1541. Epub 2020 Oct 16.

Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang, Korea 790-784.

Scientific research on advanced polymer electrolytes has led to the emergence of all-solid-state energy storage/transfer systems. Early research began with acid-tethered polymers half a century ago, and research interest has gradually shifted to high-precision polymers with controllable acid functional groups and nanoscale morphologies. Consequently, various self-assembled acid-tethered block polymer morphologies have been produced. Read More

ACS Macro Lett 2020 Nov 12;9(11):1494-1506. Epub 2020 Oct 12.

School of Chemistry, University of Birmingham, Edgbaston, Birmingham B15 2TT, United Kingdom.

The current global materials economy has long been inefficient due to unproductive reuse and recycling efforts. Within the wider materials portfolio, plastics have been revolutionary to many industries but they have been treated as disposable commodities leading to their increasing accumulation in the environment as waste. The field of chemistry has had significant bearing in ushering in the current plastics industry and will undoubtedly have a hand in transforming it to become more sustainable. Read More

ACS Macro Lett 2020 Nov 3;9(11):1687-1692. Epub 2020 Nov 3.

Institute for Frontier Materials, Deakin University, Geelong, Victoria 3216, Australia.

Hypoxia-activated prodrugs (HAPs) have emerged as important candidates for chemotherapy due to their efficient killing of hypoxic cancer cells. Traditional small molecule agents, such as tirapazamine (TPZ) and its derivatives, have shown unsatisfactory therapeutic effect in clinical trials due to poor bioavailability in hypoxic tumor regions. Herein, an amphiphilic macromolecular prodrug with hypoxia-specific activity, named as hypoxia-activated macromolecular prodrug (HAMP), is prepared from poly{[poly(ethylene glycol) methacrylate]--(methacrylic acid)} [poly(PEGMA--MAA)], containing pendant TPZ residues. Read More

ACS Macro Lett 2020 Nov 3;9(11):1681-1686. Epub 2020 Nov 3.

Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an China, 710000.

Hydrogel tubes as one kind of perfusable tubular materials, show promising applications in a wide spectrum of fields. However, there is still a great challenge to design a rapid, biocompatible, and straightforward strategy for one-step engineering tough hydrogel tubes, which have excellent mechanical properties, unique resilience, and multiple functions. Herein, we explore visible-light-mediated orthogonal photochemistry to achieve the fabrication of tough hydrogel tubes with double networks via a coaxial-nozzle spinning technique under short blue-light irradiation (∼20 s). Read More

ACS Macro Lett 2020 Nov 2;9(11):1674-1680. Epub 2020 Nov 2.

Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States.

We have directly observed the in situ self-assembly kinetics of polyelectrolyte complex (PEC) micelles by synchrotron time-resolved small-angle X-ray scattering, equipped with a stopped-flow device that provides millisecond temporal resolution. A synthesized neutral-charged diblock polycation and homopolyanion that we have previously investigated as a model charge-matched, core-shell micelle system were selected for this work. The initial micellization of the oppositely charged polyelectrolytes was completed within the dead time of mixing of 100 ms, followed by micelle growth and equilibration up to several seconds. Read More

ACS Macro Lett 2020 Nov 30;9(11):1667-1673. Epub 2020 Oct 30.

Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.

We present a molecular dynamics simulation study investigating the phase behavior of lamellae-forming diblock copolymers with a single ionic junction on the backbone. Our results show qualitative agreement with experimental findings regarding enhanced microphase separation with the introduction of an ionic junction at the conjunction point, while further revealing nonmonotonic changes in domain spacing and order-disorder transition as a function of the electrostatic interaction strength. This highlights the dominant roles of entropic and binding effects of counterions under weak and strong ionic correlations, respectively. Read More

ACS Macro Lett 2020 Nov 30;9(11):1662-1666. Epub 2020 Oct 30.

Department of Chemistry, University of Tennessee, 1416 Circle Drive, Knoxville, Tennessee 37996, United States.

Postsynthetic modification is a powerful strategy for tuning soft materials. While methods for side-chain functionalization abound, modifications of backbone structural elements can be difficult to achieve. This challenge arises, in part, from a lack of intrinsically reactive motifs that can be installed in the main chain of a polymer. Read More

ACS Macro Lett 2020 Nov 28;9(11):1655-1661. Epub 2020 Oct 28.

Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China.

The strength and toughness are two trade-off properties of a material, yet can achieve strong and tough materials by introducing sacrificial bonds into a system. Here, we present a four-component multiblock copolymer (mBCP) approach toward strong and tough elastic fibers, by introducing terpyridine moieties into poly(ether ester) mBCP elastomers. After coordination with Fe(II), supramolecular cross-links are formed within the physically cross-linked thermoplastic elastomers. Read More

ACS Macro Lett 2020 Nov 27;9(11):1632-1637. Epub 2020 Oct 27.

Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.

A paradigm for enhanced magnetorheological elastic materials is introduced and experimentally established. We show that a nonlinearly stiffening polymer matrix can be exploited to achieve anomalous magneto-elastomer stiffening exceeding standard magneto-elastomer theory and experiment in terms of percentage stiffness change and sensitivity to applied magnetic flux. Using a model system of a semiflexible fibrin network embedded with micron sized carbonyl iron particles, we demonstrate that even at a modest particle volume fraction (0. Read More

ACS Macro Lett 2020 Nov 27;9(11):1625-1631. Epub 2020 Oct 27.

Department of Physics, Emory University, Atlanta, Georgia 30322, United States.

Profiles in the local glass transition temperature () within polystyrene (PS) next to polydimethylsiloxane (PDMS) domains were determined using a localized fluorescence method. By changing the base to cross-linker ratio, we varied the cross-link density and, hence, the Young's modulus of PDMS (Sylgard 184). The local () in PS at a distance of = 50 nm away from the PS/PDMS interface was found to shift by 40 K as the PDMS modulus was varied from 0. Read More

ACS Macro Lett 2020 Nov 26;9(11):1617-1624. Epub 2020 Oct 26.

Department of Chemical Engineering, University of California, Santa Barbara, California 93106, United States.

We report the first simulations of nonsolvent-induced phase separation (NIPS) that predict membrane microstructures with graded asymmetric pore size distribution. In NIPS, a polymer solution film is immersed in a nonsolvent bath, enriching the film in nonsolvent, and leading to phase separation that forms a solid polymer-rich membrane matrix and polymer-poor membrane pores. We demonstrate how mass-transfer-induced spinodal decomposition, thermal fluctuations, and glass-transition dynamics-implemented with mobility contrast between the polymer-rich and polymer-poor phases-are essential to the formation of asymmetric membrane microstructures. Read More

ACS Macro Lett 2020 Nov 23;9(11):1611-1616. Epub 2020 Oct 23.

State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, The Key Laboratory for Chemical Biology of Fujian Province, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian 361005, China.

Here, we report a distinct mechanism for harnessing CO-responsiveness through enhancing CO capture ability. The finding is demonstrated on the microgels that are composed of oligo(ethylene glycol) and sulfonate moieties. Laser light scattering studies on dilute aqueous dispersion of these microgels indicated a low CO-responsivity, which can be significantly enhanced by adding NaCl and other salts. Read More

ACS Macro Lett 2020 Nov 23;9(11):1604-1610. Epub 2020 Oct 23.

Materials Physics Center, CSIC-UPV/EHU, Paseo Manuel Lardizábal 5, 20018 Donostia-San Sebastián, Spain.

Cyclic polymers behave different than linear polymers due to the lack of end groups and smaller coil dimensions. Herein, we demonstrate that cyclic polyethylene glycol (PEG) can be used as an alternative of classical linear PEG ligands for gold nanoparticle (AuNP) stabilization. We observed that the brush height of cyclic PEG on AuNPs of diameter 4. Read More