Mechanically robust and stretchable organic solar cells plasticized by small-molecule acceptors.

Emerging wearable devices would benefit from integrating ductile photovoltaic light-harvesting power sources. In this work, we report a small-molecule acceptor (SMA), also known as a non-fullerene acceptor (NFA), designed for stretchable organic solar cell (-OSC) blends with large mechanical compliance and performance. Blends of the organosilane-functionalized SMA BTP-Si4 with the polymer donor PNTB6-Cl achieved a power conversion efficiency (PCE) of >16% and ultimate strain (ε) of >95%.

Printed Nanomaterials for All-in-One Integrated Flexible Wearables and Bioelectronics.

Recent advancements in printing technologies allow for fabricating various wearable sensors, circuits, and integrated electronics. However, most printing tools have limited ranges of handling ink viscosity, a short working distance, and a limited feature size for developing sophisticated electronics. Here, this paper introduces an all-in-one integrated wearable electronic system via multilayer, multinanomaterial printing.

Effect of Interfacial Electric Field on 2D Metal/Graphene Electrocatalysts for CO Reduction Reaction.

Understanding the influence of local electric fields on electrochemical reactions is crucial for designing highly selective electrocatalysts for CO reduction reactions (CORR). In this study, we provide a theoretical investigation of the effect of the local electric field induced by the negative-biased electrode and cations in the electrolyte on the energetics and reaction kinetics of CORR on 2D hybrid metal/graphene electrocatalysts. Our findings reveal that the electronic structures of the CO molecule undergo substantial modification, resulting in the increased adsorption energy of CO on metal/graphene structures, thus reducing the initial barrier of the CORR mechanism.

Unveiling Competitive Adsorption in TiO Photocatalysis through Machine-Learning-Accelerated Molecular Dynamics, DFT, and Experimental Methods.

The efficient harnessing of solar power for water treatment via photocatalytic processes has long been constrained by the challenge of understanding and optimizing the interactions at the photocatalyst surface, particularly in the presence of nontarget cosolutes. The adsorption of these cosolutes, such as natural organic matter, onto photocatalysts can inhibit the degradation of pollutants, drastically decreasing the photocatalytic efficiency. In the present work, computational methods are employed to predict the inhibitory action of a suite of small organic molecules during TiO photocatalytic degradation of -chlorobenzoic acid (CBA).

Bromine Incorporation Affects Phase Transformations and Thermal Stability of Lead Halide Perovskites.

Mixed-cation and mixed-halide lead halide perovskites show great potential for their application in photovoltaics. Many of the high-performance compositions are made of cesium, formamidinium, lead, iodine, and bromine. However, incorporating bromine in iodine-rich compositions and its effects on the thermal stability of the perovskite structure has not been thoroughly studied.

2D Metal/Graphene and 2D Metal/Graphene/Metal Systems for Electrocatalytic Conversion of CO to Formic Acid.

Efficiently transforming CO into renewable energy sources is crucial for decarbonization efforts. Formic acid (HCOOH) holds great promise as a hydrogen storage compound due to its high hydrogen density, non-toxicity, and stability under ambient conditions. However, the electrochemical reduction of CO (CO RR) on conventional carbon black-supported metal catalysts faces challenges such as low stability through dissolution and agglomeration, as well as suffering from high overpotentials and the necessity to overcome the competitive hydrogen evolution reaction (HER).

Multiscale Modeling Approach for the Aldol Addition Reaction in Multicompartment Micelle-Based Nanoreactor.

Water has emerged as a versatile solvent for organic chemistry in recent years due to its abundance, low cost, and environmental friendliness. However, one of the most important reactions, the aldol reaction, in the presence of excess water exhibits low yields and poor enantioselectivities. In this regard, we have employed a multiscale modeling approach to investigate the aldol addition reaction catalyzed by l-proline in the hydrophobic compartment of multicompartment micelle (MCM) nanoreactor consisting of amphiphilic bottlebrush copolymer, which minimizes the water content at the reactive site.

Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene-Metal-Graphene Sandwich Architecture for Oxygen Reduction Reactions.

Over the past decades, the design of active catalysts has been the subject of intense research efforts. However, there has been significantly less deliberate emphasis on rationally designing a catalyst system with a prolonged stability. A major obstacle comes from the ambiguity behind how catalyst degrades.

Dual-light emitting 3D encryption with printable fluorescent-phosphorescent metal-organic frameworks.

Optical encryption technologies based on room-temperature light-emitting materials are of considerable interest. Herein, we present three-dimensional (3D) printable dual-light-emitting materials for high-performance optical pattern encryption. These are based on fluorescent perovskite nanocrystals (NCs) embedded in metal-organic frameworks (MOFs) designed for phosphorescent host-guest interactions.

Distribution and Transport of CO in Hyperbranched Poly(ethylenimine)-Loaded MCM-41: A Molecular Dynamics Simulation Approach.

Fossil fuel use is accelerating climate change, driving the need for efficient CO capture technologies. Solid adsorption-based direct air capture (DAC) of CO has emerged as a promising mode for CO removal from the atmosphere due to its potential for scalability. Sorbents based on porous supports incorporating oligomeric amines in their pore spaces are widely studied.

Nonorthogonal Cascade Catalysis in Multicompartment Micelles.

Multicompartment micelles (MCMs) containing acid and base sites in discrete domains are prepared from poly(norbornene)-based amphiphilic bottlebrush copolymers in aqueous media. The acid and base sites are localized in different compartments of the micelle, enabling the nonorthogonal reaction sequence: deacetalization - Knoevenagel condensation - Michael addition of acetals to 2-amino chromene derivatives. Computational simulations using dissipative particle dynamics (DPD) elucidated the bottlebrush composition required to effectively site-isolate the nonorthogonal catalysts.

The selective heating effect of microwave irradiation on a binary mixture of water and polyethylene oxide: a molecular dynamics simulation approach.

In this study, we investigate the molecular mechanisms of a microwave-driven selective heating process by performing molecular dynamics simulations for three different systems including pure water, pure polyethylene oxide (PEO), and water-PEO mixed systems in the presence of a microwave with two different intensities of electric field such as 0.001 V Å and 0.01 V Å at a frequency of 100 GHz.

Thermoresponsive Conductivity of Graphene-Based Fibers.

Smart materials are versatile material systems which exhibit a measurable response to external stimuli. Recently, smart material systems have been developed which incorporate graphene in order to share on its various advantageous properties, such as mechanical strength, electrical conductivity, and thermal conductivity as well as to achieve unique stimuli-dependent responses. Here, a graphene fiber-based smart material that exhibits reversible electrical conductivity switching at a relatively low temperature (60 °C), is reported.

Optimal high-throughput virtual screening pipeline for efficient selection of redox-active organic materials.

As global interest in renewable energy continues to increase, there has been a pressing need for developing novel energy storage devices based on organic electrode materials that can overcome the shortcomings of the current lithium-ion batteries. One critical challenge for this quest is to find materials whose redox potential (RP) meets specific design targets. In this study, we propose a computational framework for addressing this challenge through the effective design and optimal operation of a high-throughput virtual screening (HTVS) pipeline that enables rapid screening of organic materials that satisfy the desired criteria.

Catalytically Active Multicompartment Micelles.

This article presents the self-assembly behavior of multicompartment micelles (MCMs) in water into morphologies with multiple segregated domains and their use as supports for aqueous catalysis. A library of poly(norbornene)-based amphiphilic bottlebrush copolymers containing covalently attached l-proline in the hydrophobic, styrene, and pentafluorostyrene domains and a poly(ethylene glycol)-containing repeat unit as the hydrophilic block have been synthesized using ring-opening metathesis polymerization. Interaction parameter (χ) values between amphiphilic blocks were determined using a Flory-Huggins-based computational model.

Graphene Nanoribbon Hybridization of Zeolitic Imidazolate Framework Membranes for Intrinsic Molecular Separation.

Zeolitic imidazolate frameworks (ZIFs) are promising for gas separation membrane, but their molecular cut-off differs from that expected from its intrinsic aperture structure because of their flexibility. Herein, we introduced graphene nanoribbons (GNRs) to rigidify the ZIF framework. Because the sp edge of the GNRs induces strong anchoring effects, the modified layer can be rigidified.

Carbon Quantum Dot Modified Reduced Graphene Oxide Framework for Improved Alkali Metal Ion Storage Performance.

Organic materials with redox-active oxygen functional groups are of great interest as electrode materials for alkali-ion storage due to their earth-abundant constituents, structural tunability, and enhanced energy storage properties. Herein, a hybrid carbon framework consisting of reduced graphene oxide and oxygen functionalized carbon quantum dots (CQDs) is developed via the one-pot solvothermal reduction method, and a systematic study is undertaken to investigate its redox mechanism and electrochemical properties with Li-, Na-, and K-ions. Due to the incorporation of CQDs, the hybrid cathode delivers consistent improvements in charge storage performance for the alkali-ions and impressive reversible capacity (257 mAh g at 50 mA g ), rate capability (111 mAh g at 1 A g ), and cycling stability (79% retention after 10 000 cycles) with Li-ion.

Cooperativity in the Aldol Condensation Using Bifunctional Mesoporous Silica-Poly(styrene) MCM-41 Organic/Inorganic Hybrid Catalysts.

This work explores the efficacy of silica/organic hybrid catalysts, where the organic component is built from linear aminopolymers appended to the silica support within the support mesopores. Specifically, the role of molecular weight and polymer chain composition in amine-bearing atom transfer radical polymerization-synthesized poly(styrene--2-(4-vinylbenzyl)isoindoline-1,3-dione) copolymers is probed in the aldol condensation of 4-nitrobenzaldehyde and acetone. Controlled polymerization produces protected amine-containing poly(styrene) chains of controlled molecular weight and dispersity, and a grafting-to thiol-ene coupling approach followed by a phthalimide deprotection step are used to covalently tether and activate the polymer hybrid catalysts prior to the catalytic reactions.

Accelerating Solvent Selection for Type II Porous Liquids.

Type II porous liquids, comprising intrinsically porous molecules dissolved in a liquid solvent, potentially combine the adsorption properties of porous adsorbents with the handling advantages of liquids. Previously, discovery of appropriate solvents to make porous liquids had been limited to direct experimental tests. We demonstrate an efficient screening approach for this task that uses COSMO-RS calculations, predictions of solvent p values from a machine-learning model, and several other features and apply this approach to select solvents from a library of more than 11,000 compounds.

Single-Step Fabrication of Polymeric Composite Membrane via Centrifugal Colloidal Casting for Fuel Cell Applications.

Recent interest in polymer electrolyte membranes (PEMs) for fuel cell systems has spurred the development of infiltration technology by which to insert ionomers into mechanically robust reinforcement structures by solution casting in order to produce a cost effective and highly efficient electrolyte. However, the results of the fabrication process often continue to present challenges related to the structural complexity and self-assembly dynamics between the hydrophobic and hydrophilic parts of the constituents which in turn, necessitates additional processing steps and increases production costs. Here, a single-step process is reported for highly compact polymeric composite membranes (PCMs), fabricated using a centrifugal colloidal casting (C3) method.

DFT-Machine Learning Approach for Accurate Prediction of p.

In this study, we propose a novel method of p prediction in a diverse set of acids, which combines density functional theory (DFT) method with machine learning (ML) methods. First, the DFT method with B3LYP/6-31++G**/SM8 is used to predict p, yielding a mean absolute error of 1.85 p units.

Tailored Design of Electrochemically Degradable Anthraquinone Functionality toward Organic Cathodes.

In efforts to design organic cathode materials for rechargeable batteries, a fundamental understanding of the redox properties of diverse non-carbon-based functionalities incorporated into 9,10-anthraquinone is lacking despite their potential impact. Herein, a preliminary investigation of the potential of anthraquinones with halogenated nitrogen-based functionalities reveals that the Li-triggered structural collapse observed in the early stage of discharging can be ascribed to the preference toward the strong Lewis acid-base interaction of N-Li-X (X = F or Cl) over the repulsive interaction of the electron-rich N-X bond. A further study of three solutions (, substitution of NX with (i) BX, (ii) NH, and (iii) BH) to the structural decomposition issue highlights four conclusive remarks.

Distribution and Transport of CO in Hydrated Hyperbranched Poly(ethylenimine) Membranes: A Molecular Dynamics Simulation Approach.

Hyperbranched poly(ethylenimine) (HB-PEI) has been distinguished as a promising candidate for carbon dioxide (CO) capture. In this study, we investigate the distribution and transport of CO molecules in a HB-PEI membrane at various hydration levels using molecular dynamics (MD) simulations. For this, model structures consisting of amorphous HB-PEI membranes with CO molecules are equilibrated at various hydration levels.

Spectral Instability of Layered Mixed Halide Perovskites Results from Anion Phase Redistribution and Selective Hole Injection.

Despite the ability to precisely tune their bandgap energies, mixed halide perovskites (MHPs) suffer from significant spectral instability, which obstructs their utilization for the rational design of light-emitting diodes. Here, we investigate the origin of the electroluminescence peak shifts in layered MHPs containing bromide and iodide. X-ray diffraction and steady-state absorption measurements prove effective integration of iodide into the cubic lattice and the spatially uniform distribution of halides in the ambient environment.

Effect of the Side-Chain Length in Perfluorinated Sulfonic and Phosphoric Acid-Based Membranes on Nanophase Segregation and Transport: A Molecular Dynamics Simulation Approach.

The effect of side-chain length on the nanophase-segregated structure and transport in perfluorinated sulfonic acid (PFSA)-based and perfluorinated phosphoric acid (PFPA)-based membranes is investigated at 20 and 5 wt % water content conditions using a molecular dynamics simulation method. It is found using the pair correlation analysis that the longer side chain leads to more developed local water structures in the water phase at 20 wt % water content, observable in both membrane chemistries albeit more distinct in PFPA-based membranes. It is also confirmed from the structure factor analysis that large-scale nanophase segregation is enhanced with increasing side-chain length for PFPA membranes, whereas no significant change is observed at these scales for PFSA membranes.