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Jiayin Yuan

Publications and source records attributed to Jiayin Yuan.

At least 19 recordsLinked to original sources
arXiv2019

Efficient Electrocatalytic Reduction of CO2 by Nitrogen-Doped Nanoporous Carbon-Carbon Nanotube Membranes - A Step Towards the Electrochemical CO2 Refinery

The search for earth abundant, efficient and stable electrocatalysts that can enable the chemical reduction of CO2 to value-added chemicals and fuels at an industrially relevant scale, is a high priority for the development of a global network of renewable energy conversion and storage systems that can meaningfully impact greenhouse gas induced climate change. Here we introduce a straightforward, low cost, scalable and technologically relevant method to manufacture an all-carbon, electroactive, nitrogen-doped nanoporous carbon-carbon nanotube composite membrane, dubbed "HNCM-CNT". The membrane is demonstrated to function as a binder-free, high-performance electrode for the electrocatalytic reduction of CO2 to formate. The Faradaic efficiency for the production of formate is 81%. Furthermore, the robust structural and electrochemical properties of the membrane endow it with excellent long-term stability.

physics.chem-ph↗
arXiv2019

Ambient Electro-Synthesis of Ammonia - Electrode Porosity and Composition Engineering

Ammonia, key precursor for fertilizer production, convenient hydrogen carrier and emerging clean fuel, plays a pivotal role in sustaining life on earth. Currently, the main route for NH3 synthesis is via the heterogeneous catalytic Haber-Bosch process (N2+3H2 - 2NH3), which proceeds under extreme conditions of temperature and pressure with a very large carbon footprint. Herein we report that a pristine nitrogen-doped nanoporous graphitic carbon membrane (NCM) can electrochemically convert N2 into NH3 in an aqueous acidic solution under ambient conditions. The Faradaic efficiency and rate of production of NH3 on the NCM electrode reach 5.2% and 0.08 g m-2 h-1, respectively. After functionalization of the NCM with Au nanoparticles (Au NPs) these performance metrics are dramatically enhanced to 22% and 0.36 g m-2 h-1, respectively. These efficiencies and rates for the production of NH3 at room temperature and atmospheric pressure are unprecedented. As this system offers the potential to be scaled to industrial proportions there is a high likelihood it might displace the century old Haber-Bosch process.

physics.chem-ph↗
arXiv2019

Templated synthesis of cyclic poly(ionic liquid)s

Charged cyclic polymers, e.g. cyclic DNAs and polypeptides, play enabling roles in organisms, but their synthesis was challenging due to the well known polyelectrolyte effect. To tackle the challenge, we developed a templated method to synthesize a library of imidazolium and pyridinium based cyclic poly(ionic liquid)s. Cyclic templates, cyclic polyimidazole and poly(2-pyridine), were synthesized first through ring-closure method by light-induced Diels-Alder click reaction. Through quaternization of cyclic templates followed by anion metathesis, the cyclic poly(ionic liquid)s were synthesized, which paired with varied counter anions.

cond-mat.soft↗
arXiv2019

Ionic Organic Cage-encapsulating Phase-transferable Metal Clusters

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 via ligand-binding may perturb MC 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 (less than 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 MCs(at)I-Cage hybrid serves as a recyclable, reaction-switchable catalyst featuring high activity in liquid-phase catalysis.

physics.chem-ph↗
arXiv2019

Poly(ionic liquid)-derived N-doped carbons with hierarchical porosity for lithium and sodium ion batteries

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 porous N-doped 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 were first prepared and then decorated by a thin PIL coating before carbonization. The resulting NPCs reached a satisfactory specific surface area of up to 561 m2/g and a hierarchically meso- and macroporous structure while keeping a nitrogen content of 2.6 wt %. Such NPCs delivered a high reversible charge/discharge capacity of 1013 mA h/g over 200 cycles at 0.4 A/g for lithium ion batteries (LIBs), and showed a good capacity of 204 mA h/g over 100 cycles at 0.1 A/g for sodium ion batteries (SIBs).

physics.app-ph↗
arXiv2019

Fine Tuning Hydrophobicity of Counter-Anions to Tailor Pore Size in Porous All-Poly(ionic liquid) Membranes

Charged porous polymer membranes (CPMs) emerging as a multifunctional platform for diverse applications in chemistry, materials science, and biomedicine have been attracting widespread attention. Fabrication of CPMs in a controllable manner is of particular significance for optimizing their function and maximizing practical values. Herein, we report the fabrication of CPMs exclusively from poly(ionic liquid)s (PILs), and their pore size and wettability were precisely tailored by rational choice of the counteranions. Specifically, stepwise subtle increase in hydrophobicity of the counteranions by extending the length of fluorinated alkyl substituents, i.e. from bis(trifluoromethane sulfonyl)imide (Tf2N) to bis(pentafluoroethane sulfonyl)imide (Pf2N) and bis(heptafluoropropane sulfonyl)imide (Hf2N), decreases the average pore size gradually from 1546 nm to 157 nm and 77 nm, respectively. Meanwhile, their corresponding water contact angles increased from 90 degree to 102 degree and 120o. The exquisite control over the porous architectures and surface wettability of CPMs by systematic variation of the anion's hydrophobicity provides a solid proof of the impact of the PIL anions on CPMs' structure.

physics.app-ph↗
arXiv2019

"Cooking carbon in a solid salt": Synthesis of porous heteroatom-doped carbon foams for enhanced organic pollutant degradation under visible light

Porous heteroatom-doped carbons are desirable for catalytic reactions due to their tunable physicochemical properties, low cost and metal-free nature. Herein, we introduce a facile general bottom-up strategy, so-called "cooking carbon in a solid salt", to prepare hierarchically porous heteroatom-doped carbon foams by using poly(ionic liquid) as precursor and common inorganic salts as structural template. The obtained carbon foams bear micro-/meso-/macropores, large specific surface area and rich nitrogen dopant. The combination of these favorable features facilitates the catalytic degradation of aqueous organic pollutants by persulfate under visible light irradiation, in which they prevail over the state-of-the-art metal-/carbon-based catalysts.

physics.chem-ph↗
arXiv2019

Poly(ionic liquid)s: platform for CO2 capture and catalysis

Capture and conversion of CO2 are of great importance for environment-friendly and sustainable development of human society. Poly(ionic liquid)s (PILs) combine some unique properties of ILs with that of polymers and are versatile materials for CO2 utilization. In this contribution, we briefly outline innovative poly(ionic liquid)s emerged over the past few years, such as polytriazoliums, deep eutectic monomer (DEM) based PILs, and polyurethane PILs. Additionally, we discuss their advantages and challenges as materials for Carbon Capture and Storage (CCS), and the fixation of CO2 into useful materials.

physics.chem-ph↗
arXiv2019

Precise Micropatterning of a Porous Poly(Ionic Liquid) via Maskless Photolithography for High-Performance Non-Enzymatic H2O2 Sensing

Porous poly(ionic liquid)s (PILs) recently have been actively 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 to photo-pattern 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 designs 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.

physics.chem-ph↗
arXiv2019

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

Herein we firstly 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 being as photothermal membranes exhibited excellent performance for solar seawater desalination, representing a promising strategy to construct advanced functional nanomaterials for portable water production technologies.

physics.app-ph↗
arXiv2018

Molecular dynamics and charge transport in highly conductive Polymeric Ionic Liquids

Glassy dynamics and charge transport are studied for the polymeric Ionic Liquid (PIL) poly(tris(2-(2-methoxyethoxy)ethyl)ammonium acryloxypropylsulfonate) (PAAPS) with varying molecular weight (9700, 44200, 51600 and 99500 g per mol) by Broadband Dielectric Spectroscopy (BDS) in a wide frequency (0.01 - 10E7 Hz) and temperature range (100 - 400 K) and by DSC- and AC-chip calorimetry. The dielectric spectra are characterized by a superposition of (i) relaxation processes, (ii) charge transport and (iii) electrode polarization. The relaxation processes (i) are assigned to the dynamic glass transition and a secondary relaxation. Charge transport (ii) can be described by the random free-energy barrier model as worked out by Dyre et al.; the Barton-Namikawa-Nakajima (BNN) relationship is well fulfilled over more than 8 decades. Electrode polarization (iii) follows the characteristics as analyzed by Serghei et al.; with deviations on the low frequency side. The proportionality between the relaxation rate of the dynamic glass transition and the charge carrier hopping rate reflects the nature of charge transport as glass transition assisted hopping. Hereby, the PIL under study exposes the highest dc-conductivity values observed for this class of materials below 100 oC so far, and for the first time a conductivity increase by rising degree of polymerization. The comparison of the polymeric Ionic Liquids under study with others implies conclusions on the design of novel highly conductive PILs.

cond-mat.soft↗
arXiv2018

Poly(ionic liquid)-Derived Carbon with Site-Specific N-Doping and Biphasic Heterojunction for Enhanced CO2 Capture and Sensing

CO2 capture is a pressing global environmental issue that drives scientists to develop creative strategies for tackling this challenge. The concept in this contribution is to produce site specific nitrogen doping in microporous carbon fibers. It creates a carbon/carbon heterojunction by using poly(ionic liquid) (PIL) as soft activation agent that deposits nitrogen species exclusively on the skin of commercial microporous carbon fibers. Such carbon-based biphasic heterojunction amplifies the interaction between carbon fiber and CO2 molecule for unusually high CO2 uptake and resistive sensing.

physics.app-ph↗
arXiv2018

Main-chain poly(ionic liquid)-derived nitrogen-doped micro/mesoporous carbons for CO2 capture and selective aerobic oxidation of alcohols

Sustainable development and the recent fast growing global demands for energy and functional chemicals urgently call for effective methods for CO2 remediation and efficient metal-free catalysts for selective oxidation of aromatic alcohol. Herein, a unique main-chain poly(ionic liquid) (PIL) is employed as the precursor to prepare nitrogen doped micro and mesoporous carbons via simultaneous carbonization and activation, which bear high yield, large specific surface area above 1700 m2 per g and rich nitrogen dopant. The porous carbon products deliver a high CO2 adsorption capacity up to 6.2 mmol per g at 273 K and 1 bar with outstanding reversibility and satisfactory selectivity. Besides, they work excellently as metal free carbocatalysts for the selective aerobic oxidation of benzyl alcohol to benzaldehyde with high selectivity. It is believed that this work not only provides a facile approach to prepare nitrogen-doped porous carbon, but also advances the related research in the fields of environment and catalysis.

physics.chem-ph↗
arXiv2018

General Synthetic Route Towards Highly Dispersed Metal Clusters Enabled by Poly(ionic liquid)s

The capability to synthesize a broad spectrum of metal clusters (MCs) with their size controllable in a subnanometer scale presents an enticing prospect for exploring nanosize-dependent properties. Here we report an innovative design of a capping agent from a polytriazolium poly(ionic liquid) (PIL) in a vesicular form in solution that allows for crafting a variety of MCs including transition metals, noble metals, and their bimetallic alloy with precisely controlled sizes (~ 1 nm) and record-high catalytic performance. The ultrastrong stabilization power is result of an unusual synergy between the conventional binding sites in the heterocyclic cations in PIL, and an in-situ generated polycarbene structure induced simultaneously to the reduction reaction. INTRODUCTION

cond-mat.soft↗
arXiv2017

Hierarchically Arranged Helical Fiber Actuators Derived from Commercial Cloth

The first hygroscopic tunable cloth actuator is realized via modification of commercial cloth template by a 3D nanoporous polymer hybrid. The nanoporous hybrid guarantees fast water diffusion and amplifies deformation. The cloth actuator achieves a large-scale size production, tunable motion, high tensile strength and mechanical flexibility with a breadth of utilities (e.g., electric generator and smart materials).

physics.app-ph↗
arXiv2017

Main-chain Polyimidazolium Polymers by One-pot Synthesis and Application as Nitrogen-doped Carbon Precursors

This paper reports on the one-pot synthesis of main-chain imidazolium-containing polymers, some of which show unusually high thermal stability. The imidazolium polymers were obtained by modified Debus-Radziszewski reactions for the chain build-up from simple organic compounds, here pyruvaldehyde, formaldehyde, acetic acid, and a variety of diamines. The reactions were performed in aqueous media at ambient conditions, being synthetically elegant, convenient and highly efficient. Finally, a simple anion-metathesis reaction was conducted to replace the acetate anion with dicyanamide, and the thermal properties of the main-chain polyimidazoliums before and after anion exchange were studied in detail, which demonstrated chain cross-linking by the counterion and a coupled unusually high carbonization yield of up to 66 wt% at 900 oC.

cond-mat.soft↗
arXiv2017

Plants to Polyelectrolytes: Theophylline Polymers and their Microsphere Synthesis

To extend fossil oil supplies, sustainable feed stocks for the production of useful reagents and polymers should be harnessed. In this regard, chemicals derived from plants are excellent candidates. While the vast majority of plant sources used for polymer science only contain CxHyOz, alkaloids such as caffeine, nicotine, and theophylline possess nitrogen functionality that can provide new functions for bio-derived polymers and their synthesis. In this context, we exploited the chemistry of theophylline, a natural product found in chocolate and tea, to create a cationic poly(theophylline) in a straightforward fashion for the first time. We demonstrate how this new polymer can be synthesized and used for the creation of narrowly disperse cationic microspheres.

cond-mat.soft↗