A kind of ionic liquid, namely deep eutectic solvents, are introduced to load on the surface of porous MOF-808 core as membranes to construct porous core-membrane microstructured nanomaterials for CO₂ capture at room temperature with the sorption mechanism coupling of diffusion, physisorption, and chemisorption. It shows excellent development potential for future application in CO₂ capture.

Abstract

A series of porous core-membrane microstructured nanomaterials, constructed of a deep eutectic solvent (DES) membrane and porous MOF-808 core via liquid surface tensions and electrostatic interactions, are introduced for carbon dioxide capture with the sorption mechanism coupling diffusion, physisorption, and chemisorption. MOF-808 as the porous core considerably improves the diffusion interactions for DES membranes, hence significantly enhancing the sorption performance of DESs. Although the DES consisted by monoethanolamine and tetrapropylammonium chloride (MEA-TPAC-7) has the highest sorption capacity among all DESs, it is only 4.39 mmol g⁻¹ at 2.4 bar and further attenuates by fastidious diffusion interactions when increasing viscosity or dose. The sorption capacities of DES@MOF-120 are 5.18 mmol g⁻¹ at 3.0 bar and 4.78 mmol g⁻¹ at 2.4 bar without apparent sorption hysteresis in pressure swing sorption, which are substantially improved contrasted to MEA-TPAC-7. The sorption isotherms are reconstructed via Sips models considering surface heterogeneity with regression correlation coefficients over 0.9454 to forecast maximum sorption capacity over 6.33 mmol g⁻¹.

Nitroso derivatives with unique characteristics have been extensively studied in various fields, including biology and clinical research. Even though it has been made an intense investigation of "nitrosable" components in many drugs and commonly consumed nutrients, there is still a need for a higher awareness about their formation and characterization. This study demonstrates how these derivatives can be produced through a mechanochemical procedure under solid-state conditions. The results include synthesizing previously unknown compounds with potential biological and pharmaceutical applications, such as a nitrosamine derived from a Diclofenac-like structure.

The increasing need for electrochemical energy storage drives the development of post-lithium battery systems. Among the most promising battery types are sodium-based battery systems. However, like its lithium predecessor, sodium batteries suffer from various issues like parasitic side reactions, which lead to a loss of active sodium inventory, thus reducing the capacity over time. Some problems in sodium batteries arise from an unstable solid electrolyte interphase (SEI) reducing its protective power. While it is known that the electrolyte affects the SEI structure, the exact formation mechanism of the SEI is not yet fully understood. Here we follow the initial SEI formation on sodium metal submerged in propylene carbonate with and without the electrolyte salt sodium perchlorate. We combine X-ray photoelectron spectroscopy, gas chromatography, and density functional theory to unravel the sudden emergence of propylene oxide after adding sodium perchlorate to the solvent.  We identify the formation of a sodium chloride layer as a crucial step in forming propylene oxide by enabling precursors formed from propylene carbonate on the sodium metal surface to undergo a ring-closing reaction. We identify changes in the electrolyte decomposition process, propose a reaction mechanism to form propylene oxide and discuss alternatives based on known synthesis routes.

NH₃ decomposition: The introduction of DBD plasma makes a breakthrough in the temperature of hydrogen production from ammonia decomposition catalyzed by ruthenium-based catalyst, and significantly enhances the NH₃ conversion.

Abstract

The efficient decomposition of ammonia to produce CO_x-free hydrogen at low temperatures has been extensively investigated as a potential method for supplying hydrogen to mobile devices based on fuel cells. In this study, we employed dielectric barrier discharge (DBD) plasma, a non-thermal plasma, to enhance the catalytic ammonia decomposition over supported Ru catalysts (Ru/Y₂O₃, Ru/La₂O₃, Ru/CeO₂ and Ru/SiO₂). The plasma-catalytic reactivity of Ru/La₂O₃ was found to be superior to that of the other three catalysts. It was observed that both the physicochemical properties of the catalyst (such as support acidity) and the plasma discharge behaviours exerted significant influence on plasma-catalytic reactivity. Combining plasma with a Ru catalyst significantly enhanced ammonia conversion at low temperatures, achieving near complete NH₃ conversion over the 1.5 %-Ru/La₂O₃ catalyst at temperatures as low as 380 °C. Under a weight gas hourly space velocity of 2400 mL g_cat ⁻¹ h⁻¹ and an AC supply power of 20 W, the H₂ formation rate and energy efficiency achieved were 10.7 mol g_Ru ⁻¹ h⁻¹ and 535 mol g_Ru ⁻¹ (kWh)⁻¹, respectively, using a 1.5 %-Ru/La₂O₃ catalyst.

A novel gel polymer electrolyte (GPE) for lithium metal batteries (LMBs) combines two strategies: in-situ formation of GPEs and regulating SEI by adding diluent to manipulate ion pairing. Through a series of experiments and molecular modeling, the fundamental mechanisms of how the diluent TTE affects the ion solvation in the GPE and the formation of SEI on the Li-metal surface were investigated.

Abstract

Gel polymer electrolytes (GPEs) have potential as substitutes for liquid electrolytes in lithium-metal batteries (LMBs). Their semi-solid state also makes GPEs suitable for various applications, including wearables and flexible electronics. Here, we report the initiation of ring-opening polymerization of 1,3-dioxolane (DOL) by Lewis acid and the introduction of diluent 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) to regulate electrolyte structure for a more stable interface. This diluent-blended GPE exhibits enhanced electrochemical stability and ion transport properties compared to a blank version without it. FTIR and NMR proved the effectiveness of monomer polymerization and further determined the molecular weight distribution of polymerization by gel permeation chromatography (GPC). Experimental and simulation results show that the addition of TTE enhances ion association and tends to distribute on the anode surface to construct a robust and low-impedance SEI. Thus, the polymer battery achieves 5 C charge-discharge at room temperature and 200 cycles at low temperature −20 °C. The study presents an effective approach for regulating solvation structures in GPEs, promoting advancements in the future design of GPE-based LMBs.

Single crystal hematite photoanode, Fe-25A/Co−Pi, yields a photocurrent density of 2.67 mA cm⁻² (at 1.23 V vs. RHE) and an incident photon-to-current conversion efficiency incident photon-to-current conversion efficiency (IPCE) value of 50.8 % (380 nm) under AM 1.5G light irradiation, which is much higher than that obtained from the commonly used by thermal dehydration from β-FeO(OH) precursors.

Abstract

In this work, α-Fe₂O₃ photoanode consisted of (110)-oriented α-Fe₂O₃ single crystals were synthesized by a facile hydrothermal method. By using particular additive (C₄MimBF₄) and regulation of hydrothermal reaction time, the Fe-25 consisted of a single-layer of highly crystalline (110)-oriented crystals with fewer grain boundaries, which was vertically grown on the substrate. As a result, the charge separation efficiency and photoelectrochemical (PEC) performance of Fe-25A (Fe-25 after dehydration treatment) have been greatly improved. Fe-25A yields a photocurrent of 1.34 mA cm⁻² (1.23 V vs RHE) and an incident photon-to-current conversion efficiency (IPCE) of 31.95 % (380 nm). With the assistance of cobalt–phosphate water oxidation catalyst (Co−Pi), the PEC performance could be further improved by enhancing the holes transfer at electrode/electrolyte interface and inhibiting surface recombination. Fe-25A/Co−Pi yields a photocurrent of 2.67 mA cm⁻² (1.23 V vs RHE) and IPCE value of 50.8 % (380 nm), which is 3.67 times and 2.39 times as that of Fe-2A/Co−Pi. Our work provides a simple method to fabricate highly efficient Fe₂O₃ photoanodes consist of characteristic (110)-oriented single crystals with high crystallinity and high quality interface contact to enhance charge separation efficiencies.

A novel molecule (PTDM) containing n-type and p-type redox sites was prepared. By exploiting the synergistic advantages of two-type redox sites of PTDM, the aqueous PTDM//Zn cell delivers a high average voltage of ~1.13 V, a decent specific capacity of 118.3 mAh g⁻¹ at 0.1 A g⁻¹ and moderate capacity retention of 65.6 % over 6400 cycles at 1 A g⁻¹.

Abstract

Aqueous zinc ion batteries (AZIBs) are gaining popularity as advanced energy storage devices that are economical, safe, and use resource-abundant storage options. In this study, we have synthesized a bipolar phenothiazine organic scaffold known as 3,7-bis(melaminyl)phenothiazin-5-ium iodide (PTDM), which is obtained by undergoing nucleophilic substitution through phenothiazinium tetraiodide hydrate (PTD) and melamine. Electrochemical results indicate that PTDM can act as a high-potential cathode material for rechargeable AZIBs. In detail, the aqueous PTDM//Zn full cell exhibits a high average voltage of approximate 1.13 V, along with a specific capacity of 118.3 mAh g⁻¹ at 0.1 A g⁻¹. Furthermore, this demonstrated cell displays moderate long-term cycling stability over 6400 cycles, which is encouraging and suggests potential for developing advanced organic electrode materials for rechargeable AZIBs.

“Heterogeneous electrocatalytic water oxidation is a complicate reaction… This and more about the story behind the research that inspired the Cover image is presented in the Cover Profile. Read the full text of the corresponding research at 10.1002/cssc.202300709. View the Front Cover here: 10.1002/cssc.202301261.

Abstract

Invited for this month′s cover is the group of Rui Cao at Shaanxi Normal University. The image shows the interface between Co₃O₄ and β-Mo₂C can be regulated to boost the electrocatalytic performance of water oxidation. The Research Article itself is available at 10.1002/cssc.202300709.

Phase is different: Recent progress on low dimensional perovskite materials based on Ruddlesden-Popper and Dion-Jacobson phases is reviewed and the key link between the phase difference and the optoelectronic performance is critically summarized.

Abstract

Layered low-dimensional halide perovskites (LDPs) with multiple quantum well structure have shown increasing research interest in photovoltaic solar cell applications owing to their intrinsic moisture stability and favorable photophysical properties in comparison with their three-dimensional (3D) counterparts. The most common LDPs are Ruddlesden-Popper (RP) phases and Dion-Jacobson (DJ) phases, both of which have made significant research advances in efficiency and stability. However, distinct interlayer cations between RP and DJ phase lead to disparate chemical bonds and different perovskite structures, which endow RP and DJ perovskite with distinctive chemical and physical properties. Plenty of reviews have reported the research progress of LDPs but no summary has elaborated from the perspective of the merits and drawbacks of the RP and DJ phases. Herein, in this review, we offer a comprehensive expound on the merits and promises of RP and DJ LDPs from their chemical structure, physicochemical properties, and photovoltaic performance research progress aiming to provide a new insight into the dominance of RP and DJ phases. Then, we reviewed the recent progress on the synthesis and implementation of RP and DJ LDPs thin films and devices, as well as their optoelectronic properties. Finally, we discussed the possible strategies to resolve existing toughs to realize the desired high-performance LDPs solar cells.

Developing high-performance photocatalysts to selectively catalyze bio-platform molecules remains a challenge. In this work, PI with moderate photooxidation capability showed high-performance photooxidation of 5-hydroxymethylfurfural (HMF) to 2, 5-diformylfuran (DFF) with a high selectivity of 91 % and a high apparent quantum efficiency of 1.13 %.

Abstract

Solar-driven high-value utilization of biomass and its derivatives has attracted tremendous attention in replacing fossil sources to generate chemicals. Developing high-performance photocatalysts to selectively catalyze bio-platform molecules remains a challenge. Herein, biomass-based 5-hydroxymethylfurfural (HMF) was efficiently and selectively photooxidized to 2, 5-diformylfuran (DFF) using a metal-free polyimide (PI). PI with moderate photooxidation capacity delivered high DFF selectivity of 91 % and high apparent quantum efficiency of 1.13 %, nearly 7 times higher than that of graphitic carbon nitride. Experimental measurements and theoretical calculations revealed that the band structure and photooxidation capability of PI can be continuously modulated by varying the molar ratio of amine and anhydride. Mechanism analysis depicted that holes and superoxide radicals play crucial roles in the efficient photooxidation of HMF to DFF. This work provides guidance on designing efficient polymeric photocatalysts for oxidating biomass and its derivatives to value-added chemicals.