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The preparation of dense Si3N4-based ceramics has attracted great attention because of the achievable improvements in their mechanical properties and high-temperature oxidation resistance. In this work, advanced dense boron-containing α/β-Si3N4/Si monoliths were prepared via a high pressure‒high temperature technique in which polymer-derived amorphous SiBN powders were used as raw materials. The crystallization behavior and phase transformation of the polymer-derived amorphous samples were studied in the temperature range from 1400 to 1800 °C. The results demonstrate that the incorporation of boron in the Si3N4 matrix suppresses the phase transformation from α-Si3N4 to β-Si3N4. Furthermore, the mechanical properties of the as-prepared samples were measured, and the maximum hardness and fracture toughness of boron-rich SiBN samples reached 14.8 GPa and 7.96 MPa·m1/2, respectively. The hardness of the obtained boron-rich SiBN samples is stable up to 300 °C. In addition, the oxidation behavior of the samples prepared at 1400 and 1600 °C was investigated at 1400 °C for 50 h. The results show that the incorporation of boron significantly improved the oxidation resistance of the samples because of the formation of borosilicate/cristobalite. This work provides guidance for the synthesis of boron-containing α/β-Si3N4-based ceramics with excellent mechanical properties and oxidation resistance.

Abstract Luminescent materials that simultaneously embody bright singlet and triplet excitons hold great potential in optoelectronics, signage, and information encryption. However, achieving high-performance white-light emission is severely hampered by their inherent unbalanced contribution of fluorescence and phosphorescence. Herein, we address this challenge by pressure treatment engineering via the hydrogen bonding cooperativity effect to realize the mixture of n–π*/π–π* transitions, where the triplet state emission was boosted from 7% to 40% in isophthalic acid (IPA). A superior white-light emission based on hybrid fluorescence and phosphorescence was harvested in pressure-treated IPA, and the photoluminescence quantum yield was increased to 75% from the initial 19% (blue-light emission). In-situ high-pressure IR spectra, X-ray diffraction, and neutron diffraction reveal continuous strengthening of the hydrogen bonds with the increase of pressure. Furthermore, this enhanced hydrogen bond is retained down to the ambient conditions after pressure treatment, awarding the targeted IPA efficient intersystem crossing for balanced singlet/triplet excitons population and resulting in efficient white-light emission. This work not only proposes a route for brightening triplet states in organic small molecules, but also regulates the ratio of singlet and triplet excitons to construct high-performance white-light emission.

Large-volume presses (LVPs) providing large volumes, liquid media, deformation capability, jump compression, and in situ measurements are in great demand for high-pressure research, particularly in the fields of geoscience, condensed matter physics, material science, chemistry, and biology. A high-pressure and high-temperature (HPHT) platform with different LVP subsystems, both solid-state and liquid environments, and nonequilibrium subsystems, has been constructed at the Synergetic Extreme Condition User Facility, Jilin University. This article describes the construction of the different subsystems and provides an overview of the capabilities and characteristics of the different HPHT subsystems. A large sample volume (1000 mm3) at 20 GPa is achieved through the use of a belt-type apparatus in the solid-state subsystem. HPHT conditions (1.8 GPa and 1000 K) are realized in the liquid subsystem through the use of a piston–cylinder-type LVP with optical diamond windows for in situ spectroscopic measurements. A maximum pressure jump to 10.2 GPa can be reached within 20 ms in the nonequilibrium subsystem with the use of an improved bladder-pressurization jump press. Some typical results obtained with different LVPs are briefly reviewed to illustrate the applications and advantages of these presses. In summary, the platform described here has the potential to contribute greatly to high-pressure research and to innovations in high-pressure technology.

Abstract Superconductivity at room temperature and near‐ambient pressures is a highly sought‐after phenomenon in physics and materials science. A recent study reported the presence of this phenomenon in N‐doped lutetium hydride [Nature 615, 244 (2023)], however, subsequent experimental and theoretical investigations have yielded inconsistent results. This study undertakes a systematic examination of synthesis methods involving high temperatures and pressures, leading to insights into the impact of the reaction path on the products and the construction of a phase diagram for lutetium hydrides. Notably, the high‐pressure phase of face‐centered cubic LuH3 (fcc‐LuH3) is maintained to ambient conditions through a high‐temperature and high‐pressure method. Based on temperature and anharmonic effects corrections, the lattice dynamic calculations demonstrate the stability of fcc‐LuH3 at ambient conditions. However, no superconductivity is observed above 2 K in resistance and magnetization measurements in fcc‐LuH3 at ambient pressure. This work establishes a comprehensive synthesis approach for lutetium hydrides, thereby enhancing the understanding of the high‐temperature and high‐pressure method employed in hydrides with superconductivity deeply.

The temperature-dependent magnetic susceptibility combined with first-principle calculations was conducted to unravel the magnetic structure and the magnetic interaction of the laminar structure of manganese diboride (MnB2). MnB2 showed weak ferromagnetic, antiferromagnetic, and paramagnetic behavior with increased temperature. Its weak ferromagnetic property below 135.6 K Curie temperature (TC) originated from the spin canting antiferromagnetic magnetic structure. The exotic kink of temperature-dependent magnetic susceptibility at 330 K Néel temperature (TN) correlated with the transition from antiferromagnetic to paramagnetic structure. First-principle calculation show that the antiferromagnetic ordering show lower energy, and suggest a canting anti-ferromagnetic ordering for its ferromagnetic behavior. The peculiar magnetic behavior of MnB2 may be due to the insertion of the honeycomb boron layers into the host matrix of manganese atoms. The honeycomb boron layers played a key role in the exchange between two manganese layers. This study resolved the longstanding puzzle of the magnetic structure of MnB2 and provided a typical laminar magnetic structure prototype.

Purity metallic materials are increasingly demanded in modern manufacturing industries, but their applications are limited owing to their poor wear resistance and mechanical properties. Therefore, exploring an efficient hardening method to significantly enhance the hardness of pure metals is emergent in materials science. In this work, a series of high pressure and high temperature (HPHT) quenching experiments were carried out on several pure metals, with a maximum hardening factor exceeding 10. The results indicated that pressure has an unusual effect on refining grains and increasing the Hall–Petch coefficient ky. The ky value of pure Fe is 49.5 GPa*μm1/2 with a quenching pressure of 5 GPa, which is two orders higher than that of the untreated polycrystalline sample (0.2 GPa*μm1/2). In addition, we report an extreme hardness of 8.34 GPa in pure Ti induced by HPHT quenching, and the unprecedented hardening comes from the formation of the twin and lath martensitic substructures. The hardening mechanism of the HPHT quenching method is a combination of Hall–Petch hardening and work-hardening. Our results provide a practical route to achieve attractive mechanical properties in pure metals and shine a light on the hardening mechanism of metallic materials.

The hardness of materials is a complicated physical quantity, and the hardness models that are widely used do not function well for transition metal light element (TMLE) compounds. The overestimation of actual hardness is a common phenomenon in hardness models. In this work, high-quality Mn3N2 bulk samples were synthesized under high temperature and high pressure (HTHP) to investigate this issue. The hardness of Mn3N2 was found to be 9.9 GPa, which was higher than the hardness predicted using Guo’s model of 7.01 GPa. Through the combination of the first-principle simulations and experimental analysis, it was found that the metal bonds, which are generally considered helpless to the hardness of crystals, are of importance when evaluating the hardness of TMLE compounds. Metal bonds were found to improve the hardness in TMLEs without strong covalent bonds. This work provides new considerations for the design and synthesis of high-hardness TMLE materials, which can be used to form wear-resistant coatings over the surfaces of typical alloy materials such as stainless steels. Moreover, our findings provide a basis for establishing a more comprehensive theoretical model of hardness in TMLEs, which will provide further insight to improve the hardness values of various alloys.

High-quality P6322 Mn2N0.86 samples were synthesised using a high-pressure metathesis reaction, and the properties of the material were investigated. The measurements revealed that the Vickers hardness was 7.47 GPa, which is less than that predicted by commonly used theoretical models. At low air pressure, Mn2N0.86 and MnO coexist at 500 to 600 °C, and by excluding air, we succeeded in producing Mn4N by heating Mn2N0.86 in nitrogen atmosphere; we carefully studied this process with thermogravimetry and differential scanning calorimetry (TG-DSC). This gives a hint that to control temperature, air pressure and gas concentration might be an effective way to prepare fine Mn-N-O catalysis. Magnetic measurements indicated that ferromagnetism and antiferromagnetism coexist within Mn2N0.86 at room temperature and that these magnetic properties are induced by nitrogen vacancies. Ab intio simulation was used to probe the nature of the magnetism in greater detail. The research contributes to the available data and the understanding of Mn2N0.86 and suggests ways to control the formation of materials based on Mn2N0.86.

Transition metal borides (TMBs) are promising catalysts for hydrogen evolution reaction (HER). While the commercially available TMBs indicate poor HER performance due to powder electrode and low activity sites density, optimizing commercial TMBs for better HER performance is urgent. To break through the challenge, a new strategy is proposed to compose integral bulk electrodes with needle surfaces in TMBs. The integral bulk electrodes in TiB2, ZrB2, and HfB2 are formed under high pressure and high temperature (HPHT), and the nanoneedle morphology is constructed by chemical etching. In the three materials, the smallest overpotential is 346 mV at 10 mA cm−2 in the HCl etched bulk TiB2 electrode, which is about 61.9% higher than commercial TiB2 powder. Better performance arises from better conductivity of the integral bulk electrode, and the nano morphology exposes the edge sides of the structure which have high activity site density. This work is significant for developing new kinds of bulk TMBs catalysts.