ACS Materials Letters最新文献

Ultralong room-temperature phosphorescence (URTP) materials have been widely studied due to their broad applications. However, achieving phosphorescent materials with ultralong lifetimes is engaging and challenging. In this work, the indolo[3,2,1-j,k]carbazole (ICZ) with excellent planarity is obtained through twice single-bond locking on triphenylamine (TPA). Doping ICZ into a rigid matrix, URTP materials with a lifetime of 3.24 s and a photoluminescence quantum yield of 37.37% is successfully prepared.. The analysis of single-crystal, temperature-dependent photophysical characterization, Huang–Rhys factor, and theoretical calculations demonstrates that it is possible to make the molecules more planar and rigid by single-bond locking, which can inhibit the structural relaxation of the excited state and thus reduce the nonradiative transition to generate URTP. In addition, we achieve full-color afterglow by energy transfer. The potential applications of anticounterfeiting and optoelectronic information display of these URTP materials have been conducted. This work is an important reference for the construction of URTP materials.

The development of cathodes for lithium–sulfur (Li–S) batteries requires optimizing a variety of interacting and competing variables, with the early technology readiness level (TRL) of Li–S relative to Li-ion batteries presenting researchers with a wide parameter space. Given the interactions between the positive electrode design and the electrolyte, the development of Li–S electrodes requires comprehensive reporting of parameters to enable a comparison of developments. By developing a tool to aggregate synthesis parameters with cell performance, we summarize the frequency with which different components and electrochemical testing conditions are used, including data from 100 articles. Grouping reported capacity data by composite carbon type, C rate, and sulfur content revealed widespread variation in the maximum capacity and rate of degradation. We hope that the tool developed here will provide a facile workflow and promote consistent reporting across the literature, while also pointing toward routes to improve the design of Li–S positive electrodes.

Bulk metallic oxides with abundant surface oxygen vacancies are promising for the electrocatalytic carbon dioxide reduction reaction (CO₂RR). However, the obscure quantification of oxygen-release behavior has hindered the development of highly active and robust electrocatalysts. Herein, based on theoretical guidance, graphene confined SnO_x nanodots (rGO@SnO_x ND) holding the capacity for in situ formation of reaction-induced oxygen vacancies were prepared and taken as the model catalyst. Operando X-ray absorption fine structure (XAFS) quantitatively analyzed the reversible oxygen-released behavior, promoting the SnO_x lattice modulation of the adsorption of *OCHO intermediate. These structure changes further facilitate the exceptional performance, yielding a peak j_formate of 567 mA cm^–2, a selectivity of 92.5% and a 50 h long-term stability of rGO@SnO_x ND. The findings significantly advance the comprehensive understanding of the quantitative relationship between controllable oxygen vacancies and reaction activity, highlighting the capabilities of operando spectroscopy toward much wider metallic oxide-based electrochemical systems.

Inspired by the diversity of natural metalloenzymes, we designed microgels incorporating metal centers that mimic carbonic anhydrase for efficient CO₂ capture and detection, even in aqueous environments. These microgels demonstrate high sensitivity, detecting CO₂ at concentrations as low as 300 ppm, surpassing conventional methods. The metal centers in the microgels can be constructed by coordinating with metal ions such as Mn²⁺, Cr³⁺, Ni²⁺, Cu²⁺, and Zn²⁺. Upon absorption of CO₂, the system becomes weakly acidic, enabling multifunctional applications. Notably, Cu²⁺-based microgels display catalytic versatility, acting as carbonic anhydrase in neutral to alkaline conditions and as laccase or peroxidase in neutral to acidic environments. This versatility highlights their potential for transforming water pollutants across a broad pH range, offering significant promise for environmental remediation.

Androgenic alopecia (AGA) is a prevalent progressive hair loss condition. The main therapeutic drug, minoxidil, is limited by its poor efficacy and side effects such as contact dermatitis and hypertrichosis. Nitric oxide (NO), an endothelial-derived relaxing factor, promotes angiogenesis and accelerates blood flow, enhancing nutrient supply similar to minoxidil. Accordingly, we utilized a poly(vinyl alcohol) film (PVA) loaded with hyaluronic acid (HA) liposomes to construct a multistage transdermal NO delivery system (PVA@HL/NONOate) for the treatment of AGA. The HA liposomes provided efficient NO loading and extended release, while the PVA film improved skin penetration and sustained NO release, increasing NO bioavailability. Low-concentration NO effectively enhanced hair follicle vitality and repaired blood vessels. Mechanistically, low-concentration NO could treat AGA mainly by regulating the HIF-1 signaling pathway to promote angiogenesis, reducing inflammation by downregulating the expression of TNFRSF9 and IL-6, repairing hair follicles by downregulating the expression of genes in the CXCL5-IL-17 inflammatory axis.

The rational design of organic ligands is crucial in the development of new metal–organic frameworks (MOFs) to enrich the structural diversity and application potential of MOFs. For example, tuning the ligand symmetry has been widely utilized in the construction of new MOFs with specific properties. Herein, a novel Y-based MOF (denoted as NU-60) was generated by selecting a tritopic carboxylate ligand with reduced symmetry. Compared with its tritopic counterpart with relatively high symmetry, NU-60 has a new (3,12)-connected topology, highlighting the power of the ligand desymmetrization method to enrich MOF structural diversity. Gas adsorption studies demonstrated that NU-60 is a propane-selective adsorbent for efficient propane/propylene separation.

Direct estimation of the reaction environment, e.g., local pH at the anode side of a membrane electrode assembly (MEA) of zero gap electrolyzer, is essential to understand possible key factors, which are influencing the sustainable operation of industrial electrolyzers. Herein, we demonstrate a scanning electrochemical microscopy-based strategy to measure the local pH in the close vicinity of an operating MEA. Local proton concentration changes during the oxygen evolution reaction were monitored in the nonzero gap electrolyzer and MEA systems. The measurements constitute a methodology to evaluate the ion transport efficiency of the MEA. The strategy was extended to investigate the effect of an activation process, buffering of the electrolyte, and poisoning effect on the change in proton transport efficiency. This novel strategy enables the estimation of the actual pH of the MEA system during operation and is of great relevance in understanding the process conditions during sustainable fuel production.

Direct estimation of the reaction environment, e.g., local pH at the anode side of a membrane electrode assembly (MEA) of zero gap electrolyzer, is essential to understand possible key factors, which are influencing the sustainable operation of industrial electrolyzers. Herein, we demonstrate a scanning electrochemical microscopy-based strategy to measure the local pH in the close vicinity of an operating MEA. Local proton concentration changes during the oxygen evolution reaction were monitored in the nonzero gap electrolyzer and MEA systems. The measurements constitute a methodology to evaluate the ion transport efficiency of the MEA. The strategy was extended to investigate the effect of an activation process, buffering of the electrolyte, and poisoning effect on the change in proton transport efficiency. This novel strategy enables the estimation of the actual pH of the MEA system during operation and is of great relevance in understanding the process conditions during sustainable fuel production.

The electrochemical CO₂ reduction reaction (CO₂RR) paved the way to carbon neutrality while producing value-added chemicals and fuels. While Cu-based catalysts show potential, they suffer from inadequate faradaic efficiency. In this study, we explore Cu(100) surface-based dual atom alloy (DAA) catalysts for the CO₂RR to produce C₁ and C₂ products. Three distinct doping patterns involve two identical or different transition metals across 27 candidates. Machine learning (ML) based models were developed with high accuracy to predict the catalytic activity of unknown catalysts. The scaling relation between the adsorption energies of *CO and *CHO is circumvented by regulating the local environment with preferential dual atom doping. The integrated DFT+ML approach identifies 14 and 8 most suitable DAAs for C₁ and C₂ product formation, respectively. Feature importance analysis underscores the significance of valence d-orbital electrons in *CO adsorption. Additionally, PDOS analysis reveals atom-like electronic states in doped metals, characterized by highly localized d-states.