Highly active, stable, and cheap Pt-free catalysts for the hydrogen evolution reaction (HER) are facing increasing demand as a result of their potential use in future energy-conversion systems. However, the development of HER electrocatalysts with Pt-like or even superior activity, in particular ones that can function under alkaline conditions, remains a significant challenge. Here, the synthesis of a novel carbon-loaded ruthenium nanoparticle electrocatalyst (Ru@CQDs) for the HER, using carbon quantum dots (CQDs), is reported. Electrochemical tests reveal that, even under extremely alkaline conditions (1 m KOH), the as-formed Ru@CQDs exhibits excellent catalytic behavior with an onset overpotential of 0 mV, a Tafel slope of 47 mV decade , and good durability. Most importantly, it only requires an overpotential of 10 mV to achieve the current density of 10 mA cm . Such catalytic characteristics are superior to the current commercial Pt/C and most noble metals, non-noble metals, and nonmetallic catalysts under basic conditions. These findings open a new field for the application of CQDs and add to the growing family of metal@CQDs with high HER performance.
Cesium-based trihalide perovskites have been demonstrated as promising light absorbers for photovoltaic applications due to their superb composition stability. However, the large energy losses (E ) observed in inorganic perovskite solar cells has become a major hindrance impairing the ultimate efficiency. Here, an effective and reproducible method of modifying the interface between a CsPbI Br absorber and polythiophene hole-acceptor to minimize the E is reported. It is demonstrated that polythiophene, deposited on the top of CsPbI Br, can significantly reduce electron-hole recombination within the perovskite, which is due to the electronic passivation of surface defect states. In addition, the interfacial properties are improved by a simple annealing process, leading to significantly reduced energy disorder in polythiophene and enhanced hole-injection into the hole-acceptor. Consequently, one of the highest power conversion efficiency (PCE) of 12.02% from a reverse scan in inorganic mixed-halide perovskite solar cells is obtained. Modifying the perovskite films with annealing polythiophene enables an open-circuit voltage (V ) of up to 1.32 V and E of down to 0.5 eV, which both are the optimal values reported among cesium-lead mixed-halide perovskite solar cells to date. This method provides a new route to further improve the efficiency of perovskite solar cells by minimizing the E .
Metal halide perovskites (MHPs) are of great interest for optoelectronics because of their high quantum efficiency in solar cells and light-emitting devices. However, exploring an effective strategy to further improve their optical activities remains a considerable challenge. Here, we report that nanocrystals (NCs) of the initially nonfluorescent zero-dimensional (0D) cesium lead halide perovskite Cs4PbBr6 exhibit a distinct emission under a high pressure of 3.01 GPa. Subsequently, the emission intensity of Cs4PbBr6 NCs experiences a significant increase upon further compression. Joint experimental and theoretical analyses indicate that such pressure-induced emission (PIE) may be ascribed to the enhanced optical activity and the increased binding energy of self-trapped excitons upon compression. This phenomenon is a result of the large distortion of [PbBr6]4− octahedral motifs resulting from a structural phase transition. Our findings demonstrate that high pressure can be a robust tool to boost the photoluminescence efficiency and provide insights into the relationship between the structure and optical properties of 0D MHPs under extreme conditions.
Recently, an experimental work reported a very high Tc of ~190K in hydrogen sulphide (H2S) at 200 GPa. The search of new superconductors with high superconducting critical temperatures in hydrogen-dominated materials has attracted significant attention. Here we predict a candidate phase of MgH6 with a sodalite-like framework in conjunction with firstprinciples electronic structure calculations. The calculated formation enthalpy suggests that it is thermodynamically stable above 263 GPa relative to MgH2 and solid hydrogen (H2). Moreover, the absence of imaginary frequency in phonon calculations implies that this MgH6 structure is dynamically stable. Furthermore, our electron-phonon coupling calculation based on BCS theory indicates that this MgH6 phase is a conventional superconductor with a high superconducting critical temperature of ~260 K under high pressure, which is even higher than that of the recently reported compressed H2S. The present results offer insights in understanding and designing new high-temperature superconductors.
Polymeric nitrogen, stabilized by compressing pure molecular nitrogen, has yet to be recovered to ambient conditions, precluding its application as a high-energy density material. Here we suggest a route for synthesis of a tetragonal polymeric nitrogen, denoted t-N, via He-N compounds at high pressures. Using first-principles calculations with structure searching, we predict a class of nitrides with stoichiometry HeN4 that are energetically stable (relative to a mixture of solid He and N2) above 8.5 GPa. At high pressure, HeN4 comprises a polymeric channel-like nitrogen framework filled with linearly arranged helium atoms. The nitrogen framework persists to ambient pressure on decompression after removal of helium, forming pure polymeric nitrogen, t-N. t-N is dynamically and mechanically stable at ambient pressure with an estimated energy density of ~11.31 kJ/g, marking it out as a remarkable high-energy density material. This expands the known polymeric forms of nitrogen and indicates a route to its synthesis.
The recent discovery of H 3 S and LaH 10 superconductors with record high superconducting transition temperatures T c at high pressure has fueled the search for room-temperature superconductivity in the compressed superhydrides. Here we introduce a new class of high T c hydrides with a novel structure and unusual properties. We predict the existence of an unprecedented hexagonal HfH 10 , with remarkably high value of T c (around 213-234 K) at 250 GPa. As concerns the novel structure, the H ions in HfH 10 are arranged in clusters to form a planar "pentagraphenelike" sublattice. The layered arrangement of these planar units is entirely different from the covalent sixfold cubic structure in H 3 S and clathratelike structure in LaH 10 . The Hf atom acts as a precompressor and electron donor to the hydrogen sublattice. This pentagraphenelike H 10 structure is also found in ZrH 10 , ScH 10 , and LuH 10 at high pressure, each material showing a high T c ranging from 134 to 220 K. Our study of dense superhydrides with pentagraphenelike layered structures opens the door to the exploration of a new class of high T c superconductors.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.