Cell Reports Physical Science最新文献

Voltage relaxation can be a powerful indicator of lithium-ion battery characteristics, but variations in relaxation times complicate the widespread use of relaxation as an analytical tool. This study investigates the voltage relaxation behavior of commercial lithium-ion batteries, focusing on the impact of depth of discharge, rate, and temperature to gain a better understanding of relaxation and to improve state-of-charge estimation. Most of the data, available in a public dataset, are gathered using a unique protocol derived from intermittent titration techniques with an emphasis on ensuring that every rest is independent of the previous one. The findings demonstrate that relaxation behavior and open-circuit voltage settling times are influenced by depth of discharge, rate, current flow direction, and cell chemistry. In addition, the obtained dataset is used to test the validity of relaxation models to showcase the benefits of having a benchmark relaxation dataset available for validation of future open-circuit voltage forecasting studies.

The weave-based interlocking design has received considerable attention for preparing the patterned linkage of molecules via formation and dissociation of highly non-covalent bonds among molecules. Here, we design the mechanical behavior of a nanoscale pantograph structure in which tetraphenylethene derivatives are interlocked in the form of warp and weft strands in silico. The kinetics related to the width strain of the entire film are evaluated by quantifying the molecular-scale tilting deformation between the warp and weft strands following the inflow and outflow of methanol. The mechanical stiffness, structural durability, and deformation repeatability of the system caused by tightly interlocked molecular strands are investigated together. The cucurbituril hybrids present on the interface are successfully self-assembled into molecular bearings using the in-plane working stroke of the pantograph film.

Silicon heterojunction (SHJ)-solar modules—when encapsulated with ethylene vinyl acetate (EVA)—are known to be extremely sensitive to water ingress. The reason for this is, however, not clear. Here, we explain the root causes of this degradation mechanism specific to SHJ, proposing a detailed microscopic model. The role of EVA is instrumental in facilitating a faster water uptake in the module. However, additional observations led us to consider the role of glass in the degradation process. The moisture at the glass/encapsulant interface promotes a glass corrosion process, releasing sodium (Na) ions that, in combination with water, forms molecular Na hydroxide. This can percolate through the EVA, eventually reaching the solar cell. Na ions may act as recombination centers in the passivating layers or at the a-Si/c-Si interface, reducing the cell’s passivation properties. Finally, we propose strategies to reinforce the water resistance and overall reliability of SHJ solar modules.

The development of photothermal therapy (PTT) as a cancer therapy has been hampered by low photothermal conversion efficiency (PTCE), which reduces its efficacy for this application. Herein, we report the investigation of the photothermal properties of ICG-II, the dimer of indocyanine green (ICG), and show it to have an unexpectedly high PTCE of 95.6%. Based on density functional theory calculations, we attribute the high PTCE of ICG-II to changes in the relative energy levels of the occupied orbitals and a constrained “butterfly” oscillation around the dimer bond that facilitates nonradiative deexcitation. Through in vitro study, we demonstrate ICG-II to be highly biocompatible and stable to irradiation and temperatures needed for photothermal therapy. In vivo experiments show that direct injection of ICG-II followed by 2 min near-infrared (NIR) irradiation can completely eliminate xenograft tumors in mice. This work demonstrates that ICG-II is an attractive candidate for further preclinical development of photothermal agents and serves as a prototype for a class of rotationally constrained molecular rotors for PTT and other photochemical applications.

Cancers of diverse origins exhibit more rapid and greater carbohydrate uptake and consumption compared to normal cells, making carbohydrate an efficient cancer-targeting tool. Here, we report a glycooligomer construction methodology enabling efficient synthesis of sequence-controlled glycooligomers both in solution and on solid support. The uptake of the synthesized glycooligomers by cancerous cells is found to be significantly higher than most normal cells, and the tumor-targeting capability of the sequence-optimized glycooligomers is explored. The efficient cancer cell selectivity and in vivo tumor accumulation indicate its great potential for biomedical applications, such as targeted cancer diagnosis and therapy.

Plastics are critical in facilitating the comfort and quality of everyday life. Most plastics are discarded after a single use, wasting the energy and carbon consumed for their production and incurring environmental costs. Thus, closed-loop production and recycling processes are needed to mitigate energy and carbon loss toward a net-zero carbon economy. Here, we show that poly(ethylene terephthalate) (PET) can be efficiently deconstructed into small-molecule α,ω-dialkenenyl terephthalates using organocatalyzed transesterification. The resulting compounds can be polymerized by acyclic diene metathesis (ADMET) polymerization, affording unsaturated semi-aromatic polyesters with thermomechanical properties dependent on the monomer structure and the catalyst used for their synthesis. High-molecular-weight ADMET polymers form free-standing films that are ductile and tough with mechanical properties similar to widely used commodity plastics. Crucially, the ADMET polymers can be deconstructed to monomers using Retro-ADMET and re-polymerized by ADMET polymerization, establishing closed-loop circularity for a unique class of materials.

Electrochemically converting CO₂ to renewable synthons is steadily becoming a globally scalable and important CO₂ utilization technology. Nevertheless, most industrial endeavors employ catalysts based on metallic Ag or Au, with few catalytically competitive alternatives, showing similar activity, high mass activity, and cost efficiency. Similarly, this effort is hindered by insufficient testing of promising materials in application-oriented conditions. We herein present a holistic pathway starting from the conceptualization of different Ag(I)-based molecular catalysts to their complete integration into directly industrially applicable cell assemblies. Notably, optimization of not only the catalyst but also the operational conditions allowed us to achieve CO₂ electrolysis for at least 110 h at 300 mA cm⁻² and 80 h at 600 mA cm⁻² with an FE_CO decay rate of 0.01% h⁻¹. Beyond significant mass activity improvements for CO production, we provide the community with a broad toolbox toward improving catalytic and cell performance directly between different cell sizes.

Due to the upswing in interest in the development of efficient hydroelementation reactions to construct C–heteroatom bonds either stoichiometrically or catalytically, the activation of isocyanates and isothiocyanates has received recent attention. The activation and derivatization of isocyanates and isothiocyanates using earth-abundant and inexpensive group 13 main-group compounds have lately been observed more frequently. In this review, we aim to highlight the activation of the C=N vs. C=O and C=S bonds, the scope of cycloaddition reactions of iso(thio)cyanates with group 13 compounds, and recent findings using frustrated Lewis pairs (FLPs). In addition, the hydroboration and hydroamination reactions of these substrates are also discussed to formulate synthetically important urea/amide or thioamide derivatives.

Transparent solar cells (TSCs) can be used in systems where conventional opaque solar cells cannot be applied, such as in the glass windows of buildings and sunroofs of vehicles. Although extensive research is being conducted on the development of TSCs, some critical limitations remain, including low power conversion efficiency (PCE), reduction in PCE with changes in the angle of incidence of light, and temperature increase in the TSC. In this study, we address these critical issues by selectively applying microscale inverted-pyramidal-structured polydimethylsiloxane to the TSC. As a result, we develop crystalline silicon-based glass-like TSCs with a PCE of 15.8% (at an average visible transmittance of 20%). Furthermore, due to the wide-angle anti-reflection effects, this system maintains a PCE retention of 96% even at an incident angle of 50°, and the film demonstrates a radiative cooling effect that can reduce temperatures of the TSC by up to 16°C.

Amid the growing interest in renewable energy sources and the urgent need for decarbonization in various industries, cost-effective alkaline water electrolysis has emerged as a pivotal technology enabling efficient energy conversion to produce green hydrogen fuel. With the merits of metalloid character, abundant assets, tunable composition, superior conductivity, and cost-effectiveness, transition metal phosphides (TMPs) are recognized as attractive catalytic materials for alkaline electrolyzers. Here, the recent research progress on TMPs (Ni and Co) with their standard synthetic methodology and the roles of mono to bimetallic phosphides (Ni–Co) have been comprehensively summarized. A comparative study of the catalytic hydrogen evolution reaction activity of different phosphides is also included, where the importance of energy efficiency, reaction kinetics, and surface reaction thermodynamics is emphasized. The apt tuning of the electronic and structural properties of TMPs can significantly boost their efficiency to fulfill their tremendous potential in scaling up carbon-neutral hydrogen production via alkaline water electrolysis.