Electrocatalysis driven by clean electricity has attracted significant interest for its environmentally friendly potential. To this end, high-performance electrocatalysts are required to accelerate reaction rates. Layered materials have attracted considerable research interest for various electrocatalytic reactions and due to their rich crystal structures and flexible electronic structures. Their structural anisotropy and interlayer space between the host layers provide a unique confined microenvironment for accommodating diverse guest species. This review concentrates on the interlayer regulation of layered materials, summarizing the common layered materials and corresponding intercalated species used in electrocatalysis. The influence of interlayer species on the crystal structure, electronic structure, and electrocatalytic performance of layered materials is discussed. In addition, a perspective on future opportunities in the field of interlayer regulation of layered materials in electrocatalysis is highlighted.

Thorium, a radioactive nuclide, commonly accompanies rare earth minerals. The wastewater generated during the mining and processing of these ores poses significant risks to the environment and public health. Therefore, efficient adsorbents for removing thorium are crucial in the recent research. This study synthesized a novel dimethylphosphine functionalized Al-based metal organic framework (CAU-PMIDA) and evaluated its adsorption selectivity for thorium in wastewater. Adsorption mechanism studies have shown that CAU-PMIDA adsorbs thorium mainly through chemical adsorption,and dynamics follow a pseudo second-order model and reach equilibrium within approximately 30 min. Thorium adsorption on CAU-PMIDA fits the Langmuir isotherm, achieving a maximum capacity of 199.50 mg/g at pH 3.5. Coexisting rare earth ions have minimal interference, demonstrating remarkable Th(IV) selectivity. CAU-PMIDA maintains excellent regeneration performance,high adsorption capacity and selectivity under acidic conditions, which indicating significant potential in the treatment especially from acidic rare earth contaminated wastewater.

Triethylamine (TEA) endangers both the environment and public health due to its high toxicity and carcinogenic potential, underscoring the urgent need for effective detection technologies. However, metal oxide semiconductor sensors for TEA detection generally suffer from limitations such as sluggish response and recovery speed, limited selectivity, poor humidity resistance, and ambiguous sensing mechanisms, restricting their practical applications. Herein, SnO2 nanofibers doped with different Cd contents were fabricated via electrospinning and calcination technologies for TEA detection. Among them, the sensor with a Cd content of 3.65 at% exhibited the highest response (Ra/Rg ≈ 32.0@100 ppm TEA), ultra-short response time (3 s), good selectivity, and excellent moisture resistance at 180 °C. The enhanced performance arises from heterovalent Cd doping, which regulates the Fermi level and oxygen vacancies of SnO2, thereby optimizing surface chemisorbed oxygen and enhancing charge transfer efficiency, significantly promoting the gas-sensing reaction. Further, density functional theory (DFT) calculations revealed the interfacial interactions, charge density distributions, and surface adsorption energies between oxygen vacancies and TEA, enabling atomic-scale analysis of the sensing mechanism in Cd-doped SnO2 toward TEA molecules. This work demonstrates Cd-doped SnO2 sensors' significant application potential in environmental monitoring and industrial safety systems.

The development of cost-effective and energy-efficient anode materials is essential for the advancement of industrial water electrolysis. Herein, we report a rapid, ambient-temperature method to prepare largearea nickel mesh electrodes (SFN/NM) via surface functionalization completed within 3 min, without relying on thermal treatments or noble metals. The as-prepared electrodes achieve a high current density of 100 mA/cm(2) at an overpotential of just 300 mV in 6 mol/L KOH, and exhibit remarkable stability over 1600 h of continuous operation. With comparable activity to commercial Raney nickel yet significantly lower processing and material costs (reduced by 50 %-70 %), this approach provides a practical solution for low-energy water splitting. Beyond its industrial relevance, the strategy offers a scalable model for engineering high-performance OER electrodes, inspiring future directions in electrocatalyst design. (c) 2025 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.

Gel polymer electrolytes (GPEs), despite their flexibility, non-leakage, and processability as promising candidates of electrolytes for high-energy-density lithium batteries, persistently face the challenge of high desolvation energy caused by robust solvation interactions. Such high desolvation energy compromises interfacial kinetics, resulting in uneven lithium deposition and uncontrollable lithium dendrite growth. In this study, we reveal that the off-domain π-electron cloud of the aromatic ring in the side chains can introduce cation−π interactions to engineer weakly solvated structures, substantially reducing desolvation barriers. In addition, it is demonstrated that cation−π interactions competitively disrupt Li + −solvent coordination, attenuating binding forces between Li + and solvent molecules to promote rapid interfacial kinetics, thereby suppressing the lithium dendrite growth and enhancing interfacial stability. As a result, the cation−π chemistry enables Li||Li symmetric cell to achieve stable lithium plating/stripping over 2000 h, whereas Li||LFP full cell retains 91.6% capacity after 900 cycles at 1 C. Remarkably, 1.0 Ah pouch cell preserves 94.6% capacity after 300 cycles, and the 4.5 Ah pouch cell delivers a stable energy density of 321 Wh kg −1 . This cation−π mediated weak solvation chemistry provides valuable guidance for developing high-performance gel polymer lithium batteries.

Thorium is a promising nuclear fuel; however, even a small amount in nuclear wastewater can cause significant radioactive pollution. Therefore, it is urgent to develop effective adsorbents for the efficient removal of thorium to solve this problem. Herein, the phytic acid modification of carboxylated Zirconium-based metal-organic framework materials (UiO-66-COOH-PA) has been obtained by rapid high-temperature carbonization, which exhibits excellent performance in removing thorium (IV) in acidic aqueous solutions. The maximum adsorption capacity of UiO-66-COOH-PA-2 (with 40% mass ratio of phytic acid) in solution reaches 315.5 mg/g at a pH of 4, which is more than twice that of the unmodified Zr-based metal organic framework (MOF) material. The adsorption kinetics of UiO-66-COOH-PA on thorium has been analyzed using two different isothermal adsorption models, the Langmuir and Freundlich isotherm adsorption models. It turns out that the Freundlich model is more suitable for the data. The thorium adsorption process reaches dynamic equilibrium very quickly, while the adsorption dynamics of UiO-66-COOH-PA on thorium follows the pseudo-second-order adsorption kinetic model. The excellent adsorption performance of UiO-66-COOH-PA-2 at low pH values indicates that adsorption material containing phosphorus is suitable for the removal of thorium especially in acidic systems. It also exhibits excellent selectivity (up to 90.2%) for Th(IV) adsorption in the presence of several coexisting rare-earth ions. Overall, the integration of phosphorus-modified in Zr-MOFs represents a significant advancement in thorium adsorption technology, offering a pathway toward more effective management of radioactive acidic waste liquid.

Proton exchange membrane water electrolyser (PEMWE) possesses great significance for the production of high purity of hydrogen. To expedite the anodic oxygen evolution reaction (OER) that involved multiple electron– proton-coupled process, efficient and stable electrocatalysts are highly desired. Currently, noble-metal Ir-based materials are the benchmark anode due to its corrosion-resistant property and favourable combination of activity/stability. However, the large-scale deployment of PEMWE is usually constrained due to the use of the scarcest element iridium. In this review, we disclose the current research progress towards the non-iridium-based electrocatalysts for OER in acidic media, and then summarize some typical oxides that possesses good catalytic performance. Besides, we also present the unresolved problems and challenges in an attempt to enhance the activity/stability of these catalysts.

A novel graphene-modified molecularly imprinted polymer-based electrochemical sensor (MIP/RGO-GCE) was developed for the sensitive and selective detection of sibutramine in sports doping control. The sensor was fabricated by electropolymerizing o-phenylenediamine on a reduced graphene oxide-modified glassy carbon electrode in the presence of sibutramine as the template molecule. Under optimized conditions, the MIP/RGO-GCE sensor exhibited a wide linear range (0.05 to 20 μM), low detection limit (0.02 μM), high sensitivity (1.27 μA/μM), good precision (RSD < 2.7

Understanding the sensing mechanism of metal oxide semiconductors is imperative to the development of high-performance sensors. The traditional sensing mechanism only recognizes the effect of surface chemisorbed oxygen from the air but ignores surface lattice oxygen. Herein, using in-situ characterizations, we provide direct experimental evidence that the surface chemisorbed oxygen participated in the sensing process can come from lattice oxygen of the oxides. Further density functional theory (DFT) calculations prove that the p-band center of O serves as a state of art for regulating the participation of lattice oxygen in gas-sensing reactions. Based on our experimental data and theoretical calculations, we discuss mechanisms that are fundamentally different from the conventional mechanism and show that the easily participation of lattice oxygen is helpful for the high response value of the materials. Understanding the sensing mechanism of metal oxide semiconductors is imperative for developing high-performance sensors. Here, the participation of lattice oxygen, caused by additional Ge, boosts the hydrogen sensing ability of SnO2.

The oxygen evolution reaction (OER) over a family of metal-doped rutile IrO2 catalysts is theoretically investigated by controlling the species and position of doped elements. The subsurface substitution doping is demonstrated to efficiently regulate the e(g)-filling of surface iridium sites and lower the adsorption strength of oxygen intermediates, improving the catalytic activity for the OER. Finally, based on screening, subsurface Cu- and Li-doped IrO2 models stand near the top of the volcano plot and display high levels of structural stability toward acidic OER.

Schematic illustration of disulfidptosis.Cystine is transported to intracellular compartments by solute carrier family 7 member 11 (SLC7A11).Nicotinamide adenine dinucleotide phosphate (NADPH) is generated in the cytosol through the pentose phosphate pathway (PPP).In the presence of the reducing agent NADPH, one molecule of cystine is reduced to two molecules of cysteine, accompanied by oxidation of NADPH to NADP + .The F-actin cytoskeleton contracts due to aberrant disulfide bonding.Cells can survive if the reduced form of NADPH counteracts the accumulation of intracellular disulfides.Disulfidptosis is induced if the balance between cystine and NADPH/NADP + is disrupted.

The poor catalyst stability, stemming from serious cationdissolutionand uncontrollable amorphization, remains an outstanding problem inthe acidic oxygen evolution reaction (OER). Herein, we report thesynthesis and characterization of honeycomb layered strontium iridate(SrIr2O6) and demonstrate its potential as anefficient OER electrocatalyst with robust structural stability inacid. In contrast to the vast majority of iridate catalysts, SrIr2O6 can keep both bulk and surface structures crystallineduring OER, as opposed to forming an amorphous active phase. The edgesof SrIr2O6 are highly catalytically active forOER by following the adsorbate evolution mechanism, but the basalplanes are catalytically inert. SrIr2O6 exhibits similar to 10-fold higher intrinsic activity than the benchmark catalystIrO(2), affords an extremely low total iridium leaching level(similar to 0.03%) during OER, and retains its catalytic activity formore than 300 h.

The acidic oxygen evolution reaction underpins several important electrical-to-chemical energy conversions, and this energy-intensive process relies industrially on iridium-based electrocatalysts. Here, phase-selective synthesis of metastable strontium iridates with open-framework structure and their unexpected transformation into a highly active, ultrastable oxygen evolution nano-electrocatalyst are presented. This transformation involves two major steps: Sr2+ /H+ ion exchange in acid and in situ structural rearrangement under electrocatalysis conditions. Unlike its dense perovskite-structured polymorphs, the open-framework iridates have the ability to undergo rapid proton exchange in acid without framework amorphization. The resulting protonated iridates further reconstruct into ultrasmall, surface-hydroxylated, (200) crystal plane-oriented rutile nanocatalyst, instead of the common amorphous IrOx Hy phase, during acidic oxygen evolution. Such microstructural characteristics are found to benefit both the oxidation of hydroxyls and the formation of OO bonds in electrocatalytic cycle. As a result, the open-framework iridate derived nanocatalyst gives a comparable catalytic activity to the most active iridium-based oxygen evolution electrocatalysts in acid, and retains its catalytic activity for more than 1000 h.

Abstract The sluggish kinetics of oxygen evolution reaction (OER) and high iridium loading in catalyst coated membrane (CCM) are the key challenges for practical proton exchange membrane water electrolyzer (PEMWE). Herein, we demonstrate high-surface-area nano-metal diborides as promising supports of iridium-based OER nanocatalysts for realizing efficient, low-iridium-loading PEMWE. Nano-metal diborides are prepared by a novel disulphide-to-diboride transition route, in which the entropy contribution to the Gibbs free energy by generation of gaseous sulfur-containing products plays a crucial role. The nano-metal diborides, TaB2 in particular, are investigated as the support of IrO2 nanocatalysts, which finally forms a TaOx/IrO2 heterojunction catalytic layer on TaB2 surface. Multiple advantageous properties are achieved simultaneously by the resulting composite material (denoted as IrO2@TaB2), including high electrical conductivity, improved iridium mass activity and enhanced corrosion resistance. As a consequence, the IrO2@TaB2 can be used to fabricate the membrane electrode with a low iridium loading of 0.15 mg cm−2, and to give an excellent catalytic performance (3.06 A cm−2@2.0 V@80 oC) in PEMWE―the one that is usually inaccessible by unsupported Ir-based nanocatalysts and the vast majority of existing supported Ir-based catalysts at such a low iridium loading.

为满足稳态强磁场实验装置(SHMFF)日益增长的液氦供应需求,研制一台基于两级串联透平膨胀机修正克劳特(Claude)循环且带有液氮预冷的氦液化装置.完成了氦液化流程设计及冷箱系统集成,并对降温液化过程进行测试与分析.结果表明,两级透平膨胀机能够稳定运行于额定转速,氦液化装置在降温15 h时进入液化阶段,在产液4.5 h后能达到100 L/h的液化速率,满足设计要求.

The large-scale application of proton exchange membrane water electrolysis technology requires the development of high-performance oxygen evolution electrocatalysts with as little iridium (Ir) as possible. Ir-based double perovskite oxides (A2B'IrO6; A = alkaline, alkaline-earth, or rare-earth elements; B' = transition metal or rare-earth elements) represent a class of oxides with great potential to replace the commercial catalyst IrO2. However, the structural evolution of Ir-based double perovskite oxides in electrolytes is incompletely understood, and foundational knowledge of the design principle of the “ideal” material is lacking. In this work, we report the unexpected phenomenon of instant Ir leaching from Ir-based double perovskite oxides in acid under non-catalytic conditions and discuss the implications of this phenomenon for mechanism investigation and material identification. Some well-known Ir-based double perovskite oxides, such as Ba2PrIrO6 and Sr2YIrO6, undergo instantaneous Ir leaching when they come into contact with acidic electrolytes. The Ir-leaching process is found to be non-persistent and non-thermodynamically determined, and its extent is correlated with the leaching of other B'-site elements in the perovskite oxides. Based on this observation, we revisit the Ir dissolution-precipitation process for surface IrOx formation during the perovskite-electrolyzed oxygen evolution reaction, emphasizing the non-negligible role of Ir species owing to acid corrosion in the electrolyte. Finally, we modify a screening protocol for low-Ir oxygen evolution electrocatalysts and propose an instant acid corrosion test as an indispensable process to evaluate the structural stability of potential catalysts.

The oxygen evolution reaction (OER) is an electrochemical bottleneck half-reaction in some important energy conversion systems (e.g., water splitting), which is traditionally mediated by iridium oxides in acidic environment. Perovskite-structured Ir-containing oxides (e.g., SrIrO3) are a family of striking electrocatalysts due to their high specific activity, but this excellent quality is difficultly transferred to a nano-electrocatalyst with large active surface and good structural stability. Here, we present a synthesis method that produces a 2D ultrathin {001}-faceted SrIrO3 perovskite (2D-SIO) with a thickness of similar to 5 nm and high surface area (57.6 m(2) g (1)). We show that 2D-SIO can serve as a highly active and stable electrocatalytic nanomaterial for OER under acidic conditions. This perovskite nanomaterial produces 10 mA cm (2) current density at a low overpotential (eta, 243 mV), and maintains its catalytic activity after 5000 continuous cyclic measurements. Besides ultrathin structure and large surface area, the exposed {001} facets are found to be the most crucial and unique structural factor for achieving high catalytic activity and structural stability. Our joint experimental and theoretical results demonstrate that these advantageous microstructural features of 2D-SIO endow it with a strong capability to generate the key O* intermediates, and thereby facilitate O-O bond formation and the OER. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

The concept of single-atom catalysts (SACs) takes our understanding of active sites of heterogeneous catalysts to greater heights. 'While the knowledge about the SACs containing isolated metal centers has rapidly enriched over the last decade, a few examples of the SACs that feature single-nonmetal centers are studied, and their application potentials are also poorly explored. Herein, we report a family of 358 model surfaces featuring metal-coordinated single-boron sites for investigating the effects of boron-centered local environment on N-2-to-NH3 catalytic conversion. We demonstrate these model surfaces with (001) surfaces of antiperovskite borides (M3M'B, M, and M' represent different metal atoms), where the surface-isolated boron atoms are spacially separated by M atoms, but they do not directly bond to M' atoms. The surface-isolated boron atoms are found to be necessary for the adsorption and activation of dinitrogen, and the types of M atoms determine dinitrogen adsorption configurations. When M atoms are the late transition metals (e.g., Ni), dinitrogen prefers to adsorb on the top-site of the surface B atom with an end-on configuration; when M atoms are alkaline-earth metals, early transition metals and lanthanide elements (e.g., Sr, Zr, and La) and dinitrogen bonds to M-B-M three-center site with a side-on configuration. Additionally, during the catalytic conversion of dinitrogen to ammonia, the M atoms cooperate with the isolated boron atom to costabilize NxHy intermediates (x = 1, 2; y = 0-4), and the M' atoms finely regulate the electronic structure of B - M ensembles and thereby tune the adsorption property and catalytic activity. Furthermore, the adsorption free energy of *N is found to be applied as a descriptor of the limiting potential of dinitrogen reduction reaction, and its value is correlated with orbital hybridization between M and B atoms apart from the inherent electronic properties of M and B atoms. Finally, we predict Rh3GeB, Rh3SbB, and Ni3LiB to be promising ammonia synthesis catalysts with high activity that exceed that of the stepped Ru(0001) surface, a prominent benchmarking surface for ammonia synthesis.

Ir-based perovskite oxides show great promise for next-generation oxygen evolution reaction (OER) electrocatalysts in an acidic medium, but they are generally stuck with their uncontrollable surface amorphization and thus structural instability (e.g., serious Ir leaching) during OER. Herein, we report the high-yield chemical exfoliation of Ruddlesden-Popper layered perovskite Sr2IrO4 into protonated colloidal nanosheets with an undamaged perovskite framework. We further demonstrate the potential of protonated perovskite nanosheets to evade the trade-off between OER activity and structural stability. The 2D morphological benefit and nice monodispersity of these protonated perovskite nanosheets enable the facile fabrication of an ultralow-Ir-loading catalyst film (30 mu g cm(-2)), which exhibits about 10 times higher activity than the IrO2 catalyst film and undergoes almost as much Ir leaching during OER. Our joint experimental and theoretical results also reveal that structural hydroxyl groups on the surface of protonated nanosheets participate in the catalytic cycle of OER, and the protonated layered perovskite framework represents an example of OER electrocatalyst that works with a non-traditional adsorbate evolution mechanism.