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Markus Antonietti

Publications and source records attributed to Markus Antonietti.

10 recordsLinked to original sources

Rainbows in a bottle: Realizing microoptic effects by polymerizable multiple emulsion particle design

In nature, structural colour generation is based on discriminative light propagation associated with physical structures in the range of the wavelengths of light1. These iridescent structural colours are of immense significance2 but not easy to control experimentally and therefore difficult to exploit for applications. In this work, we employ microfluidics to produce polymerizable double emulsions that can not only induce the already known lensing effect3 but also result in the spectral separation of white light. Here, liquids of varying refractive in-dex that constitute the emulsions resulted in patterns of iridescent colours. After polymerization, the inner emulsion cores collapse and this results in curved concave surfaces on these polymeric microspheres. Interestingly, the light propagation along the curved surfaces undergo total internal reflection, followed by near-field interference along exit structures on the polymerized microspheres4. These structured polymeric particles that are able to generate colour dispersions can be exploited for optical devices, displays and even sensing technologies.

physics.optics

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

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

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

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

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

Nitrogen-doped Nanoporous Carbon Membranes Functionalized with Co/CoP Janus-type nanocrystals as Hydrogen Evolution Electrode in Both Acid and Alkaline Environment

Self-supported electrocatalysts being generated and employed directly as electrode for energy conversion has been intensively pursued in the fields of materials chemistry and energy. Herein, we report a synthetic strategy to prepare freestanding hierarchically structured, nitrogen-doped nanoporous graphitic carbon membranes functionalized with Janus-type Co/CoP nanocrystals (termed as HNDCM-Co/CoP), which were successfully applied as a highly-efficient, binder-free electrode in hydrogen evolution reaction (HER). Benefited from multiple structural merits, such as high degree of graphitization, three-dimensionally interconnected micro-/meso-/macropores, uniform nitrogen-doping, well-dispersed Co/CoP nanocrystals as well as the confinement effect of the thin carbon layer on the nanocrystals, HNDCM-Co/CoP exhibited superior electrocatalytic activity and long-term operation stability for HER under both acid and alkaline conditions. As a proof-of-concept of practical usage, a macroscopic piece of HNDCM-Co/CoP of 5.6 cm x 4 cm x 60 um in size was prepared in our laboratory. Driven by a solar cell, electroreduction of water in alkaline condition (pH 14) was performed, and H2 has been produced at a rate of 16 ml/min, demonstrating its potential as real-life energy conversion systems.

physics.chem-ph

Synthesis of Single-crystal-like Nanoporous Carbon Membranes and Their Applications in Overall Water Splitting

Nanoporous graphitic carbon membranes with defined chemical composition and pore architecture are novel nanomaterials that are actively pursued. Compared to easy-to-make porous carbon powders that dominate the porous carbon research and applications in energy generation/conversion and environmental remediation, porous carbon membranes are synthetically more challenging though rather appealing from an application perspective due to their structural integrity, interconnectivity and purity. Here we report a simple bottom-up approach to fabricate large-size, freestanding, porous carbon membranes that feature an unusual single-crystal-like graphitic order and hierarchical pore architecture plus favorable nitrogen doping. When loaded with cobalt nanoparticles, such carbon membranes serve as high-performance carbon-based non-noble metal electrocatalyst for overall water splitting.

cond-mat.mtrl-sci

Nanoporous ionic organic networks: from synthesis to materials applications

The past decade has witnessed the rapid progress in synthesizing nanoporous organic networks or polymer frameworks for various potential applications. Generally speaking, functionalization of porous networks to add extra properties and enhance materials performance could be achieved either during the pore formation (thus a concurrent approach) or post-synthetic modification (a sequential approach). Nanoporous organic networks which include ion pairs in a covalent manner are of special importance and possess extreme application profiles. Within these nanoporous ionic organic networks (NIONs), here with a pore size in the range from sub-1 nm to 100 nm, we observe a synergistic coupling of the electrostatic interaction of charges, the nanoconfinement within pores and the addressable functional units in soft matter resulting in a wide variety of functions and applications, above all catalysis, energy storage and conversion, as well as environmental operations. This review aims to highlight the recent progress in this area, and seeks to raise original perspectives that will stimulate future advancements at both the fundamental and applied level.

cond-mat.mtrl-sci

From Filter Paper to Functional Actuator by Poly(ionic liquid)-Modified Graphene Oxide

A commercially available membrane filter paper composed of mixed cellulose esters bearing typically an interconnected pore structure was transformed into a stimuli-responsive bilayer actuator by depositing a thin film of poly(ionic liquid)-modified graphene oxide sheets (GO-PIL) onto the filter paper. In acetone vapor, the as-synthesized bilayer actuator bent readily into multiple loops at a fast speed with the GO-PIL top film inwards. Upon pulling back into air the actuator recovered their original shape. The asymmetric swelling of the top GO-PIL film and the bottom porous filter paper towards organic vapor offers a favorably synergetic function to drive the actuation. The PIL polymer chains in the hybrid film were proven crucial to enhance the adhesion strength between the GO sheets and the adjacent filter paper to avoid interfacial delamination and thus improve force transfer. The overall construction allows a prolonged lifetime of the bilayer actuator under constant operation, especially when compared to that of the GO/filter paper bilayer actuator without PIL.

cond-mat.mtrl-sci