Publications by authors named "Jiayin Yuan"

91 Publications

Ferrocene-Containing Porous Poly(Ionic Liquid) Membranes: Synthesis and Application as Sacrificial Template for Porous Iron Oxide Films.

Macromol Rapid Commun 2021 Jun 1:e2100077. Epub 2021 Jun 1.

Department of Materials and Environmental Chemistry (MMK), Stockholm University, Stockholm, 10691, Sweden.

Herein, the fabrication of iron-containing porous polyelectrolyte membranes (PPMs) via ionic complexation between an imidazolium-based poly(ionic liquid) (PIL) and 1,1-ferrocenedicarboxylic acid is reported. The key parameters to control the microstructure of porous hybrid membranes are investigated in detail. Further aerobic pyrolysis of such porous hybrid membranes at 900 °C can transfer the ferrocene-containing PPMs into freestanding porous iron oxide films. This process points out a sacrificial template function of porous poly(ionic liquid) membranes in the fabrication of porous metal oxide films.
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http://dx.doi.org/10.1002/marc.202100077DOI Listing
June 2021

A transport channel-regulated MXene membrane organic phosphonic acids for efficient water permeation.

Chem Commun (Camb) 2021 Jun 1. Epub 2021 Jun 1.

Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, 10691, Sweden.

A series of organic phosphonic acids (OPAs) were applied as multifunctional spacers to enlarge the inner space of carbide MXene (Ti3C2Tx) laminates. A synergistic improvement in permeance, rejection and stability is achieved via introducing OPA to create pillared laminates. This strategy provides a universal way to regulate transport channels of MXene-based membranes.
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http://dx.doi.org/10.1039/d1cc01464aDOI Listing
June 2021

Large-Area Crystalline Zeolitic Imidazolate Framework Thin Films.

Angew Chem Int Ed Engl 2021 Jun 14;60(25):14124-14130. Epub 2021 May 14.

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Institute of Energy, Hefei Comprehensive National Science Center, CAS Center for Excellence in Nanoscience, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, Department of Chemistry, University of Science and Technology of China, Hefei, 230026, China.

We report that continuous MOF films with highly controlled thickness (from 44 to 5100 nm) can be deposited over length scales greater than 80 centimeters by a facile, fast, and cost-effective spray-coating method. Such success relies on our discovery of unprecedented perfectly dispersed colloidal solutions consisting of amorphous MOF nanoparticles, which we adopted as precursors that readily converted to the crystalline films upon low-temperature in situ heating. The colloidal solutions allow for the fabrication of compact and uniform MOF films on a great deal of substrates such as fluorine-doped tin oxide, glass, SiO , Al O , Si, Cu, and even flexible polycarbonate, widening their technological applications where substrates are essential. Despite the present work focuses on the fabrication of uniform cobalt-(2-methylimidazole) and zinc-(2-methylimidazole) films, our findings mark a great possibility in producing other high-quality MOF thin films on a large scale.
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http://dx.doi.org/10.1002/anie.202104366DOI Listing
June 2021

Electroanalysis of Biomolecules: Rational Selection of Sensor Construction.

Biochemistry (Mosc) 2021 Jan;86(Suppl 1):S140-S151

Laboratory of Bioelectrochemistry, Orekhovich Research Institute of Biomedical Chemistry, Moscow, 119992, Russia.

Methods of electrochemical analysis of biological objects based on the reaction of electro-oxidation/electro-reduction of molecules are presented. Polymer nanocomposite materials that modify electrodes to increase sensitivity of electrochemical events on the surface of electrodes are described. Examples of applications electrochemical biosensors constructed with nanocomposite material for detection of biological molecules are presented, advantages and drawbacks of different applications are discussed.
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http://dx.doi.org/10.1134/S0006297921140108DOI Listing
January 2021

Ultratough and ultrastrong graphene oxide hybrid films via a polycationitrile approach.

Nanoscale Horiz 2021 04 4;6(4):341-347. Epub 2021 Mar 4.

Department of Materials and Environmental Chemistry, Stockholm University, Stockholm 10691, Sweden.

Graphene oxide (GO) is a classic two dimensional (2D) building block that can be used to develop high-performance materials for numerous applications, particularly in the energy and environmental fields. Currently, the precise assembly of GO nanosheets into macroscopic nanohybrids of superior strength and toughness is desirable, and faces challenges and trade-offs. Herein, we exploited the freshly established polycationitrile method as a powerful molecular crosslinking strategy to engineer ultratough and ultrastrong GO/polymer hybrid films, in which a covalent triazine-based network was constructed in a mild condition to reinforce the interface between GO nanosheets. The tensile strength and toughness reached 585 ± 25 MPa and 14.93 ± 1.09 MJ m, respectively, which, to the best of our knowledge, are the current world records in all GO-based hybrid films. As an added merit of the tailor-made polymer crosslinker, the high mechanical performance can be maintained in large part at an extremely high relative humidity of 98%. This emerging interface-engineering approach paves a new avenue to produce integrated strong-and-tough 2D nanohybrid materials that are useful in aerospace, artificial muscle, energy harvesting, tissue engineering and more.
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http://dx.doi.org/10.1039/d1nh00073jDOI Listing
April 2021

"Mix-Then-On-Demand-Complex": Cascade Anionization and Complexation of Graphene Oxide for High-Performance Nanofiltration Membranes.

ACS Nano 2021 Mar 15;15(3):4440-4449. Epub 2021 Feb 15.

Department of Materials and Environmental Chemistry, Stockholm University, Stockholm 10691, Sweden.

Assembling two-dimensional (2D) materials by polyelectrolyte often suffers from inhomogeneous microstructures due to the conventional mixing-and-simultaneous-complexation procedure ("mix-and-complex") in aqueous solution. Herein a "mix-then-on-demand-complex" concept on-demand cascade anionization and ionic complexation of 2D materials is raised that drastically improves structural order in 2D assemblies, as exemplified by classical graphene oxide (GO)-based ultrathin membranes. Specifically, in dimethyl sulfoxide, the carboxylic acid-functionalized GO sheets (COOH-GOs) were mixed evenly with a cationic poly(ionic liquid) (PIL) and upon filtration formed a well-ordered layered composite membrane with homogeneous distribution of PIL chains in it; next, whenever needed, it was alkali-treated to convert COOH-GO into its anionized state COO-GO that immediately complexed ionically with the surrounding cationic PIL chains. This "mix-then-on-demand-complex" concept separates the ionic complexation of GO and polyelectrolytes from their mixing step. By synergistically combining the PIL-induced hydrophobic confinement effect and supramolecular interactions, the as-fabricated nanofiltration membranes carry interface transport nanochannels between GO and PIL, reaching a high water permeability of 96.38 L m h bar at a maintained excellent dye rejection 99.79% for 150 h, exceeding the state-of-the-art GO-based hybrid membranes. The molecular dynamics simulations support the experimental data, confirming the interface spacing between GO and PIL as the water transport channels.
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http://dx.doi.org/10.1021/acsnano.0c08308DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7992131PMC
March 2021

Dual-Cationic Poly(ionic liquid)s Carrying 1,2,4-Triazolium and Imidazolium Moieties: Synthesis and Formation of a Single-Component Porous Membrane.

ACS Macro Lett 2021 Jan 8;10(1):161-166. Epub 2021 Jan 8.

Department of Materials and Environmental Chemistry, Stockholm University, Stockholm 10691, Sweden.

Both imidazolium and 1,2,4-triazolium cations are important functional moieties widely incorporated as building blocks in poly(ionic liquid)s (PILs). In a classical model, a PIL usually contains either imidazolium or 1,2,4-triazolium in its repeating unit. Herein, via exploiting the slight reactivity difference of alkyl bromide with imidazole and 1,2,4-triazole at room temperature, we synthesized dual-cationic PIL homopolymers carrying both imidazolium and 1,2,4-triazolium moieties in the same repeating unit, that is, an asymmetrically dicationic unit. We investigated their fundamental properties, for example, thermal stability and solubility, as well as their unique function in forming supramolecular porous membranes via a water-initiated phase-separation and cross-linking process. With such knowledge, we identified a water-based fabricate strategy toward air-stable porous membranes from single-component PILs. This study will enrich the design tools and chemical structure library of PILs and expand their application spectrum.
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http://dx.doi.org/10.1021/acsmacrolett.0c00784DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7818656PMC
January 2021

Advanced Heteroatom-Doped Porous Carbon Membranes Assisted by Poly(ionic liquid) Design and Engineering.

Acc Mater Res 2020 Oct 25;1(1):16-29. Epub 2020 Sep 25.

Department of Materials and Environmental Chemistry, Stockholm University, 10691 Stockholm, Sweden.

Heteroatom-doped porous carbon membranes (HPCMMs) with a tailor-made pore architecture, chemical composition, atomic structural order, and surface state represent an exciting family of porous carbon materials for diverse potential applications in catalysis, water treatment, biofiltration, energy conversion/storage, and so forth. Conventional porous carbon membranes possess intrinsic structural integrity, interconnectivity, and chemical purity across the atomic-to-macro world and have been popularly incorporated into devices as separators or chemically inert conductive supports, circumventing otherwise the inevitable complicated processing and structure weakness of their fine powderous counterpart. Motivated by the distinguished heteroatom-doping effect that revolutionizes the chemical and physical nature of carbon materials, the HPCMM research surges very recently, and focuses not only on the eminent conductive supports or separators but also on electro(co)catalysts in energy devices. Synergy of the porous nature, incorporation of heteroatoms, and the membrane state creates a vivid profile pattern and new task-specific usage. It is also noteworthy that the inherent structural merits of HPCMMs plus a high electron conductivity imbue them as a reliable binder-free model electrode to derive the intrinsic structure-property relationship of porous carbons in electrochemical environments, excluding the complex and adverse factors in association with polymer binders in carbon powder-based electrodes. HPCMMs are of both intense academic interest and practical value because of their well-defined properties endowed by controllable structure and porosity at both atomic and macroscopic scales in a membrane form. The sole aim of this article is to bring this group of porous carbon materials to the forefront so their comprehensive properties and functions can be better understood to serve the carbon community to address pressing materials challenges in our society. In this Account, we highlight the latest discovery and proceedings of HPCMMs, particularly the advancements in how to tailor structures and properties of HPCMMs by rational structure design of porous polymer membranes as sacrificial template built up especially from heteroatom-rich poly(ionic liquid)s (PILs). We will also stress the carbonization craft and the state-of-the-art electrochemical applications for HPCMMs. Key factors and thoughts in heteroatom doping and porous systems in HPCMMs are discussed. A future perspective of the challenges and promising potential of HPCMMs is cast on the basis of these achievements.
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http://dx.doi.org/10.1021/accountsmr.0c00010DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7640738PMC
October 2020

Biomimetic Antigravity Water Transport and Remote Harvesting Powered by Sunlight.

Glob Chall 2020 Nov 6;4(11):2000043. Epub 2020 Sep 6.

Department of Chemistry Tsinghua University Beijing 100084 P. R. China.

Antigravity water transport plays important roles in various applications ranging from agriculture, industry, and environmental engineering. In natural trees, ubiquitous water-flow over 100 m high from roots through the hierarchical xylem to leaves is driven by sunlight-powered continuous evaporation and the negative pressure. Inspired by natural trees, herein an artificial trunk-leaf system is built up to structurally mimic natural trees for a continuous antigravity water delivery. The artificial tree consists of directional microchannels for antigravity water transport, and a top leaf-like hybrid hydrogel that are acts as continuous solar steam evaporator, plus a purposely engineered steam collector. It is found that continuous uniform microchannels of acetylated chitin optimize and enhance capillary rise (≈37 cm at 300 min) and reduce vertical water transport resistance. A remote water harvesting, and purification is performed with a high rate of 1.6 kg m h and 184 cm in height under 1 sun irradiation and the collection efficiency up to 100% by evaporative cooling technique. It is envisioned that the basic design principles underlying the artificial tree can be used to transform solar energy into potential energy.
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http://dx.doi.org/10.1002/gch2.202000043DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7607244PMC
November 2020

Thin Porous Poly(ionic liquid) Coatings for Enhanced Headspace Solid Phase Microextraction.

Polymers (Basel) 2020 Aug 24;12(9). Epub 2020 Aug 24.

Centro de Química Estrutural and Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Avenida Rovisco Pais, 1049-001 Lisboa, Portugal.

In this contribution, thin poly(ionic liquid) (PIL) coatings with a well-defined pore structure built up from interpolyelectrolyte complexation between a PIL and poly(acrylic acid) (PAA) were successfully used for enhanced solid phase microextraction (SPME). The introduction of porosity with tunable polarity through the highly versatile PIL chemistry clearly boosts the potential of SPME in the detection of compounds at rather low concentrations. This work will inspire researchers to further explore the potential of porous poly(ionic liquid) materials in sensing and separation applications.
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http://dx.doi.org/10.3390/polym12091909DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7563990PMC
August 2020

Polymer-Derived Heteroatom-Doped Porous Carbon Materials.

Chem Rev 2020 09 6;120(17):9363-9419. Epub 2020 Aug 6.

Department of Materials and Environmental Chemistry, Stockholm University, 10691 Stockholm, Sweden.

Heteroatom-doped porous carbon materials (HPCMs) have found extensive applications in adsorption/separation, organic catalysis, sensing, and energy conversion/storage. The judicious choice of carbon precursors is crucial for the manufacture of HPCMs with specific usages and maximization of their functions. In this regard, polymers as precursors have demonstrated great promise because of their versatile molecular and nanoscale structures, modulatable chemical composition, and rich processing techniques to generate textures that, in combination with proper solid-state chemistry, can be maintained throughout carbonization. This Review comprehensively surveys the progress in polymer-derived functional HPCMs in terms of how to produce and control their porosities, heteroatom doping effects, and morphologies and their related use. First, we summarize and discuss synthetic approaches, including hard and soft templating methods as well as direct synthesis strategies employing polymers to control the pores and/or heteroatoms in HPCMs. Second, we summarize the heteroatom doping effects on the thermal stability, electronic and optical properties, and surface chemistry of HPCMs. Specifically, the heteroatom doping effect, which involves both single-type heteroatom doping and codoping of two or more types of heteroatoms into the carbon network, is discussed. Considering the significance of the morphologies of HPCMs in their application spectrum, potential choices of suitable polymeric precursors and strategies to precisely regulate the morphologies of HPCMs are presented. Finally, we provide our perspective on how to predefine the structures of HPCMs by using polymers to realize their potential applications in the current fields of energy generation/conversion and environmental remediation. We believe that these analyses and deductions are valuable for a systematic understanding of polymer-derived carbon materials and will serve as a source of inspiration for the design of future HPCMs.
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http://dx.doi.org/10.1021/acs.chemrev.0c00080DOI Listing
September 2020

Accelerating Crystallization of Open Organic Materials by Poly(ionic liquid)s.

Angew Chem Int Ed Engl 2020 Dec 4;59(49):22109-22116. Epub 2020 Oct 4.

School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, P. R. China.

The capability to significantly shorten the synthetic period of a broad spectrum of open organic materials presents an enticing prospect for materials processing and applications. Herein we discovered 1,2,4-triazolium poly(ionic liquid)s (PILs) could serve as a universal additive to accelerate by at least one order of magnitude the growth rate of representative imine-linked crystalline open organics, including organic cages, covalent organic frameworks (COFs), and macrocycles. This phenomenon results from the active C5-protons in poly(1,2,4-triazolium)s that catalyze the formation of imine bonds, and the simultaneous salting-out effect (induced precipitation by decreasing solubility) that PILs exert on these crystallizing species.
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http://dx.doi.org/10.1002/anie.202008415DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7756458PMC
December 2020

Crosslinking of a Single Poly(ionic liquid) by Water into Porous Supramolecular Membranes.

Angew Chem Int Ed Engl 2020 Sep 6;59(39):17187-17191. Epub 2020 Aug 6.

Key Laboratory of Functional Polymer Materials of the Ministry of Education, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071, P. R. China.

Reversible regulation of membrane microstructures via non-covalent interactions is of considerable interest yet remains a challenge. Herein, we discover a general one-step approach to fabricate supramolecular porous polyelectrolyte membranes (SPPMs) from a single poly(ionic liquid) (PIL). The experimental results and theoretical simulation suggested that SPPMs were formed by a hydrogen-bond-induced phase separation of a PIL between its polar and apolar domains, which were linked together by water molecules. This unique feature was capable of modulating microscopic porous architectures and thus the global mechanical property of SPPMs by a rational design of the molecular structure of PILs. Such SPPMs could switch porosity upon thermal stimuli, as exemplified by dynamically adaptive transparency to thermal fluctuation. This finding provides fascinating opportunities for creating multifunctional SPPMs.
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http://dx.doi.org/10.1002/anie.202002679DOI Listing
September 2020

Hydrogen bonding and charge transport in a protic polymerized ionic liquid.

Soft Matter 2020 Jul;16(26):6091-6101

Leipzig University, Peter Debye Institute for Soft Matter Physics, Linnéstraße 5, 04103 Leipzig, Germany.

Hydrogen bonding and charge transport in the protic polymerized ionic liquid poly[tris(2-(2-methoxyethoxy)ethyl)ammoniumacryloxypropyl sulfonate] (PAAPS) are studied by combining Fourier transform infrared (FTIR) and broadband dielectric spectroscopy (BDS) in a wide temperature range from 170 to 300 K. While the former enables to determine precisely the formation of hydrogen bonds and other moiety-specific quantized vibrational states, the latter allows for recording the complex conductivity in a spectral range from 10-2 to 10+9  Hz. A pronounced thermal hysteresis is observed for the H-bond network formation in distinct contrast to the reversibility of the effective conductivity measured by BDS. On the basis of this finding and the fact that the conductivity changes with temperature by orders of magnitude, whereas the integrated absorbance of the N-H stretching vibration (being proportional to the number density of protons in the hydrogen bond network) changes only by a factor of 4, it is concluded that charge transport takes place predominantly due to hopping conduction assisted by glassy dynamics (dynamic glass transition assisted hopping) and is not significantly affected by the establishment of H-bonds.
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http://dx.doi.org/10.1039/d0sm00337aDOI Listing
July 2020

A case of planar-type GIST of the sigmoid colon showing diverticular structure with perforation.

World J Surg Oncol 2020 Jun 11;18(1):125. Epub 2020 Jun 11.

Department of Pathology, Hyogo College of Medicine, 1-1 Mukogawa-cho, Nishinomiya, Hyogo, 663-8501, Japan.

Background: Gastrointestinal stromal tumors (GISTs) generally form well-defined mass lesions. However, some cases of the flatly distributed and muscularis propria-replacing GISTs have been reported so far. We experienced an additional case of planar-type GIST of the sigmoid colon accompanied by a diverticulum with perforation.

Case Presentation: A 68-year-old Japanese male with sudden onset of abdominal pain was clinically diagnosed with gastrointestinal perforation, and an emergency abdominal operation was performed. A diverticulum with rupture was found in the sigmoid colon, but no apparent tumor was observed. Histological examination revealed bland spindle cells flatly proliferating and diffusely replacing the muscularis propria at the diverticular structure. The spindle cells were positive for KIT, DOG1, and CD34. Mutational analysis of the c-kit gene revealed that the lesion had a heterozygous deletion of 2 amino acids at codons 557 and 558 of exon 11. The mutation was not observed in the normal mucosa of the surrounding tissue.

Conclusion: We diagnosed this case as an unusual planar-type GIST. Some similar cases have been reported in the sigmoid colon and other sites. We discuss the mechanism of development of the planar-type GISTs associated with the diverticulum.
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http://dx.doi.org/10.1186/s12957-020-01906-8DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7291680PMC
June 2020

Porous Carbon Membrane-Supported Atomically Dispersed Pyrrole-Type FeN as Active Sites for Electrochemical Hydrazine Oxidation Reaction.

Small 2020 Aug 10;16(31):e2002203. Epub 2020 Jun 10.

Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, 10691, Sweden.

The rational design of catalytically active sites in porous materials is essential in electrocatalysis. Herein, atomically dispersed Fe-N sites supported by hierarchically porous carbon membranes are designed to electrocatalyze the hydrazine oxidation reaction (HzOR), one of the key techniques in electrochemical nitrogen transformation. The high intrinsic catalytic activity of the Fe-N single-atom catalyst together with the uniquely mixed micro-/macroporous membrane support positions such an electrode among the best-known heteroatom-based carbon anodes for hydrazine fuel cells. Combined with advanced characterization techniques, electrochemical probe experiments, and density functional theory calculation, the pyrrole-type FeN structure is identified as the real catalytic site in HzOR.
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http://dx.doi.org/10.1002/smll.202002203DOI Listing
August 2020

Hydrazine-Enabled One-Step Synthesis of Metal Nanoparticle-Functionalized Gradient Porous Poly(ionic liquid) Membranes.

Macromol Rapid Commun 2021 Apr 14;42(8):e2000143. Epub 2020 May 14.

Department of Materials and Environmental Chemistry (MMK), Stockholm University, Stockholm, 10691, Sweden.

In this communication, a one-step synthetic route is reported toward free-standing metal-nanoparticle-functionalized gradient porous polyelectrolyte membranes (PPMs). The membranes are produced by soaking a glass-plate-supported blend film that consists of a hydrophobic poly(ionic liquid) (PIL), poly(acrylic acid), and a metal salt, into an aqueous hydrazine solution. Upon diffusion of water and hydrazine molecules into the blend film, a phase separation process of the hydrophobic PIL and an ionic crosslinking reaction via interpolyelectrolyte complexation occur side by side to form the PPM. Simultaneously, due to the reductive nature of hydrazine, the metal salt inside the polymer blend film is reduced in situ by hydrazine into metal nanoparticles that anchor onto the PPM. The as-obtained hybrid porous membrane is proven functional in the catalytic reduction of p-nitrophenol. This one-step method to grow metal nanoparticles and gradient porous membranes can simplify future fabrication processes of multifunctional PPMs.
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http://dx.doi.org/10.1002/marc.202000143DOI Listing
April 2021

Microstructural and Dynamical Heterogeneities in Ionic Liquids.

Chem Rev 2020 Jul 15;120(13):5798-5877. Epub 2020 Apr 15.

Department of Chemistry, Stanford University, Stanford, California 94305, United States.

Ionic liquids (ILs) are a special category of molten salts solely composed of ions with varied molecular symmetry and charge delocalization. The versatility in combining varied cation-anion moieties and in functionalizing ions with different atoms and molecular groups contributes to their peculiar interactions ranging from weak isotropic associations to strong, specific, and anisotropic forces. A delicate interplay among intra- and intermolecular interactions facilitates the formation of heterogeneous microstructures and liquid morphologies, which further contributes to their striking dynamical properties. Microstructural and dynamical heterogeneities of ILs lead to their multifaceted properties described by an inherent designer feature, which makes ILs important candidates for novel solvents, electrolytes, and functional materials in academia and industrial applications. Due to a massive number of combinations of ion pairs with ion species having distinct molecular structures and IL mixtures containing varied molecular solvents, a comprehensive understanding of their hierarchical structural and dynamical quantities is of great significance for a rational selection of ILs with appropriate properties and thereafter advancing their macroscopic functionalities in applications. In this review, we comprehensively trace recent advances in understanding delicate interplay of strong and weak interactions that underpin their complex phase behaviors with a particular emphasis on understanding heterogeneous microstructures and dynamics of ILs in bulk liquids, in mixtures with cosolvents, and in interfacial regions.
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http://dx.doi.org/10.1021/acs.chemrev.9b00693DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7349628PMC
July 2020

The Effect of Phenyl Substitutions on Microstructures and Dynamics of Tetraalkylphosphonium Bis(trifluoro- methylsulfonyl)imide Ionic Liquids.

Chemphyschem 2020 06 21;21(11):1202-1214. Epub 2020 Apr 21.

Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91, Stockholm, Sweden.

Extensive atomistic simulations demonstrated that a gradual substitution of hexyl chains with phenyl groups in tetraalkylphosphonium cations results in remarkable changes in hydrogen bonding interactions, liquid structures and scattering structural functions, and rotational dynamics of hexyl chains and phenyl groups in tetraalkylphosphonium bis(trifluoromethylsulfonyl)imide ionic liquids. Hydrogen donor sites in hexyl chains present competitive characteristics with those in phenyl groups in coordinating anions, as well as their continuous and intermittent hydrogen bonding dynamics. Cation-cation and anion-anion spatial correlations show concomitant shift to short distances with decreased peak intensities with variations of cation structures, whereas cation-anion correlations have a distinct shift to large radial distances due to decreased associations of anions with neighboring cations. These microstructural changes are qualitatively manifested in shifts of prominent peaks for prevalent charge alternations and adjacency correlations between ion species in scattering structural functions. Meanwhile, rotational dynamics of hexyl chains speed up, which, in turn, slow down rotations of phenyl groups, whereas anions exhibit imperceptible changes in their rotational dynamics. These computational results are intrinsically correlated with conformational flexibilities, molecular sizes, and steric hindrance effects of phenyl groups in comparison with hexyl chains, and constrained distributions of anions around cations in heterogeneous ionic environments.
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http://dx.doi.org/10.1002/cphc.201901206DOI Listing
June 2020

β-Cyclodextrin-derived Room Temperature Macromolecular Ionic Liquids by PEGylated Anions.

Macromol Rapid Commun 2020 Apr 13;41(8):e1900576. Epub 2020 Mar 13.

Stockholm University, Svante Arrheniusvag 16C, 10691, Stockholm, Sweden.

A series of cyclodextrin-derived room temperature macromolecular ionic liquids carrying rather low glass transition temperatures of -20 to -40 °C are synthesized via sequential esterification, quaternization, and anion metathesis reactions. In addition to being ionic in nature, they are viscous liquids at room temperature with more fluidic behavior at elevated temperatures. They serve as a solvent for organic dyes or iodine separation via a liquid-liquid extraction approach. This strategy is useful for the development of various sugar (macro)molecule-based functional ionic liquids as well as macromolecular ionic liquids.
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http://dx.doi.org/10.1002/marc.201900576DOI Listing
April 2020

Poly(ionic liquid) composites.

Chem Soc Rev 2020 Mar 25;49(6):1726-1755. Epub 2020 Feb 25.

School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, P. R. China.

Poly(ionic liquid)s (PILs), as an innovative class of polyelectrolytes, are composed of polymeric backbones with IL species in each repeating unit. The combined merits of the polymers and ILs make them promising materials for composites in materials science. Particularly, the integration of PILs with functional substances (PIL composites) opens up a new dimension in utilizing ionic polymers by offering novel properties and improved functions, which impacts multiple subfields of our chemical society. This review summarizes recent developments of PIL composites with a special emphasis on the preparation techniques that are based on the intrinsic properties of the PILs and the synergistic effects between the PILs and substances of interest for diverse applications.
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http://dx.doi.org/10.1039/c8cs00938dDOI Listing
March 2020

Poly(Ionic Liquid)-Derived Graphitic Nanoporous Carbon Membrane Enables Superior Supercapacitive Energy Storage.

ACS Nano 2019 Sep 13;13(9):10261-10271. Epub 2019 Sep 13.

Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, School of Chemistry and Chemical Engineering , Huazhong University of Science and Technology , Wuhan , 430074 , China.

High energy/power density, capacitance, and long-life cycles are urgently demanded for energy storage electrodes. Porous carbons as benchmark commercial electrode materials are underscored by their (electro)chemical stability and wide accessibility, yet are often constrained by moderate performances associated with their powdery status. Here controlled vacuum pyrolysis of a poly(ionic liquid) membrane template, advantageous features including good conductivity (132 S cm at 298 K), interconnected hierarchical pores, large specific surface area (1501 m g), and heteroatom doping are realized in a single carbon membrane electrode. The structure synergy at multiple length scales enables large areal capacitances both for a basic aqueous electrolyte (3.1 F cm) and for a symmetric all-solid-state supercapacitor (1.0 F cm), together with superior energy densities (1.72 and 0.14 mW h cm, respectively) without employing a current collector. In addition, theoretical calculations verify a synergistic heteroatom co-doping effect beneficial to the supercapacitive performance. This membrane electrode is scalable and compatible for device fabrication, highlighting the great promise of a poly(ionic liquid) for designing graphitic nanoporous carbon membranes in advanced energy storage.
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http://dx.doi.org/10.1021/acsnano.9b03514DOI Listing
September 2019

Atomically Dispersed Semimetallic Selenium on Porous Carbon Membrane as an Electrode for Hydrazine Fuel Cells.

Angew Chem Int Ed Engl 2019 Sep 30;58(38):13466-13471. Epub 2019 Jul 30.

Key Laboratory of Functional Polymer Materials (Ministry of Education), Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071, P. R. China.

Electrochemically functional porous membranes of low cost are appealing in various electrochemical devices used in modern environmental and energy technologies. Herein we describe a scalable strategy to construct electrochemically active, hierarchically porous carbon membranes containing atomically dispersed semi-metallic Se, denoted SeNCM. The isolated Se atoms were stabilized by carbon atoms in the form of a hexatomic ring structure, in which the Se atoms were located at the edges of graphitic domains in SeNCM. This configuration is different from that of previously reported transition/noble metal single atom catalysts. The positively charged Se, enlarged graphitic layers, robust electrochemical nature of SeNCM endow them with excellent catalytic activity that is superior to state-of-the-art commercial Pt/C catalyst. It also has long-term operational stability for hydrazine oxidation reaction in practical hydrazine fuel cell.
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http://dx.doi.org/10.1002/anie.201907752DOI Listing
September 2019

Poly(Ionic Liquid) Nanoparticles Selectively Disrupt Biomembranes.

Adv Sci (Weinh) 2019 Feb 17;6(4):1801602. Epub 2018 Dec 17.

Department of Theory & Bio-Systems Max Planck Institute of Colloids and Interfaces Science Park Golm 14424 Potsdam Germany.

Polymer-based nanoparticles have an increasing presence in research due to their attractive properties, such as flexible surface functionality design and the ability to scale up production. Poly(ionic liquid) (PIL) nanoparticles of size below 50 nm are very unique in terms of their high charge density and internal onion-like morphology. The interaction between PIL nanoparticles and giant unilamellar vesicles (GUVs) of various surface charge densities is investigated. GUVs represent a convenient model system as they mimic the size and curvature of plasma membranes, while simultaneously offering direct visualization of the membrane response under the microscope. Incubating PIL nanoparticles with GUVs results in poration of the lipid membrane in a concentration- and charge-dependent manner. A critical poration concentration of PILs is located and the interactions are found to be analogous to those of antimicrobial peptides. Microbial mimetic membranes are already affected at submicromolar PIL concentrations where contrast loss is observed due to sugar exchange across the membrane, while at high concentrations the collapse of vesicles is observed. Finally, a confocal microscopy-based approach assessing the particle permeation through the membrane is reported and a mechanism based on bilayer frustration and pore stabilization via particle integration in the membrane is proposed.
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http://dx.doi.org/10.1002/advs.201801602DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6382306PMC
February 2019

Organic Molecule-Driven Polymeric Actuators.

Macromol Rapid Commun 2019 Apr 27;40(7):e1800896. Epub 2019 Feb 27.

Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, 10691, Sweden.

Inspired by the motions of plant tissues in response to external stimuli, significant attention has been devoted to the development of actuating polymeric materials. In particular, polymeric actuators driven by organic molecules have been designed due to their combined superiorities of tunable functional monomers, designable chemical structures, and variable structural anisotropy. Here, the recent progress is summarized in terms of material synthesis, structure design, polymer-solvent interaction, and actuating performance. In addition, various possibilities for practical applications, including the ability to sense chemical vapors and solvent isomers, and future directions to satisfy the requirement of sensing and smart systems are also highlighted.
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http://dx.doi.org/10.1002/marc.201800896DOI Listing
April 2019

Ionic organic cage-encapsulating phase-transferable metal clusters.

Chem Sci 2019 Feb 19;10(5):1450-1456. Epub 2018 Nov 19.

Department of Materials and Environmental Chemistry , Stockholm University , 10691 Stockholm , Sweden . Email:

Exploration of metal clusters (MCs) adaptive to both aqueous and oil phases without disturbing their size is promising for a broad scope of applications. The state-of-the-art approach ligand-binding may perturb MCs' size due to varied metal-ligand binding strength when shuttling between solvents of different polarity. Herein, we applied physical confinement of a series of small noble MCs (<1 nm) inside ionic organic cages (I-Cages), which by means of anion exchange enables reversible transfer of MCs between aqueous and hydrophobic solutions without varying their ultrasmall size. Moreover, the [email protected] hybrid serves as a recyclable, reaction-switchable catalyst featuring high activity in liquid-phase NHBH (AB) hydrolysis reaction with a turnover frequency (TOF) of 115 min.
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http://dx.doi.org/10.1039/c8sc04375bDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6354838PMC
February 2019

Three birds, one stone - photo-/piezo-/chemochromism in one conjugated nanoporous ionic organic network.

J Mater Chem C Mater 2018 Sep 24;6(34):9065-9070. Epub 2018 May 24.

Max-Planck-Institute of Colloids and Interfaces , D-14476 Potsdam , Germany . Email:

A nanoporous material bearing a high ion density and inherent organic radical character was synthesized by a facile one-pot process, which exhibits photo-, piezo- and chemochromism, driven by the diverse electron transfer processes between the acceptor framework and different electron donors. The responsive behavior is useful for its sensing application, as demonstrated here for pressure, anion and gas sensing.
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http://dx.doi.org/10.1039/c8tc01324aDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6333276PMC
September 2018

Precise Micropatterning of a Porous Poly(ionic liquid) via Maskless Photolithography for High-Performance Nonenzymatic HO Sensing.

ACS Nano 2018 12 10;12(12):12551-12557. Epub 2018 Dec 10.

Max Planck Institute of Colloids and Interfaces , Department of Colloid Chemistry , D-14424 Potsdam , Germany.

Porous poly(ionic liquid)s (PILs) recently have been serving as a multifunctional, interdisciplinary materials platform in quite a few research areas, including separation, catalysis, actuator, sensor, and energy storage, just to name a few. In this context, the capability of photopatterning PIL microstructures in a porous state on a substrate is still missing but is a crucial step for their real industrial usage. Here, we developed a method for in situ rapid patterning of porous PIL microstructures via a maskless photolithography approach coupled with a simple electrostatic complexation treatment. This breakthrough enables design of miniaturized sensors. As exemplified in this work, upon loading Pt nanoparticles into porous PIL microstructures, the hybrid sensor showed outstanding performance, bearing both a high sensitivity and a wide detection range.
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http://dx.doi.org/10.1021/acsnano.8b07069DOI Listing
December 2018

All-Poly(ionic liquid) Membrane-Derived Porous Carbon Membranes: Scalable Synthesis and Application for Photothermal Conversion in Seawater Desalination.

ACS Nano 2018 Nov 8;12(11):11704-11710. Epub 2018 Nov 8.

Key Laboratory of Functional Polymer Materials, Ministry of Education, Institute of Polymer Chemistry, College of Chemistry , Nankai University , Tianjin 300071 , P.R. China.

Herein, we introduce a straightforward, scalable, and technologically relevant strategy to manufacture charged porous polymer membranes (CPMs) in a controllable manner. The pore sizes and porous architectures of CPMs are well-controlled by rational choice of anions in poly(ionic liquid)s (PILs). Continuously, heteroatom-doped hierarchically porous carbon membrane (HCMs) can be readily fabricated via morphology-maintaining carbonization of as-prepared CPMs. These HCMs, as photothermal membranes, exhibited excellent performance for solar seawater desalination, representing a promising strategy to construct advanced functional nanomaterials for portable water production technologies.
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http://dx.doi.org/10.1021/acsnano.8b07526DOI Listing
November 2018

Poly(ionic liquid)-Derived N-Doped Carbons with Hierarchical Porosity for Lithium- and Sodium-Ion Batteries.

Macromol Rapid Commun 2019 Jan 3;40(1):e1800545. Epub 2018 Oct 3.

Dr. W. Alkarmo, Dr. F. Ouhib, Dr. A. Aqil, Dr. J.-M. Thomassin, Dr. C. Detrembleur, Prof. C. Jérôme, Centre for Education and Research on Macromolecules, CESAM Research Unit, University of Liege, Sart-Tilman B6a, 13allée du 6 août,, B-4000, Liège, Belgium.

The performance of lithium- and sodium-ion batteries relies notably on the accessibility to carbon electrodes of controllable porous structure and chemical composition. This work reports a facile synthesis of well-defined N-doped porous carbons (NPCs) using a poly(ionic liquid) (PIL) as precursor, and graphene oxide (GO)-stabilized poly(methyl methacrylate) (PMMA) nanoparticles as sacrificial template. The GO-stabilized PMMA nanoparticles are first prepared and then decorated by a thin PIL coating before carbonization. The resulting NPCs reach a satisfactory specific surface area of up to 561 m g and a hierarchically meso- and macroporous structure while keeping a nitrogen content of 2.6 wt%. Such NPCs deliver a high reversible charge/discharge capacity of 1013 mA h g over 200 cycles at 0.4 A g for lithium-ion batteries, and show a good capacity of 204 mA h g over 100 cycles at 0.1 A g for sodium-ion batteries.
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http://dx.doi.org/10.1002/marc.201800545DOI Listing
January 2019