SearcharxivSearch

arXiv subjects

Jiazhen Wu

Publications and source records attributed to Jiazhen Wu.

7 recordsLinked to original sources

Amorphous Nanoconfinement Enables Self-sustaining Sabatier Reaction at Ambient Conditions

The Sabatier reaction, the catalytic hydrogenation of CO2 into CH4, offers a cornerstone for carbon capture and utilization, and in-situ resource utilization during space exploration; however, it faces a fundamental thermodynamic-kinetic paradox: although highly exothermic, conventional catalysts still require continuous external heating to activate CO2 and maintain stable operation. Here we report an amorphous silica-embedded ruthenium catalyst that enables a long-term self-sustaining autothermal Sabatier reaction dispensing with external energy supply. Operating under ambient conditions, this system achieves a record-high CH4 yield of 0.50 mol gcat-1 h-1 with 100% selectivity, stable operation for over 2,000 hours, and a record-low catalyst bed temperature down to 100 oC. This exceptional self-sustaining behavior stems from the synergistic effect of the catalyst's ultralow effective thermal conductivity (0.27 W m-1 K-1), induced by amorphous nanoconfinement, and its superior intrinsic activity. This synergy generates localized hot spots at Ru sites while suppressing macroscopic heat loss. In situ measurements further reveal CH4 formation even at 54 oC and identify a *CO-mediated pathway for CO2 methanation. The reaction ignites readily with a lighter or focused sunlight and persists even under forced convection from an electric fan, demonstrating strong environmental tolerance. By removing the need for constant energy input, this "ignite-and-forget" system paves the way for decentralized Power-to-Gas systems and autonomous fuel production in resource-constrained environments like Mars.

cond-mat.mtrl-sci

Discovery of self-assembled Ru/Si heterostructures with unique periodic nanostripe patterns boosting hydrogen evolution

Two-dimensional (2D) heterostructuring is a versatile methodology for designing nanoarchitecture catalytic systems that allow for reconstruction and modulation of interfaces and electronic structures. However, catalysts with such structures are extremely scarce due to limited synthetic strategies. Here, we report a highly ordered 2D Ru/Si nano-heterostructures (RSHS) by acid etching of the LaRuSi electride. RSHS shows a superior electrocatalytic activity for hydrogen evolution with an overpotential of 14 mV at 10 mA/cm2 in alkaline media. Both experimental analysis and first-principles calculations demonstrate that the electronic states of Ru can be tuned by strong interactions of the interfacial Ru-Si, leading to an optimized hydrogen adsorption energy. Moreover, due to the synergistic effect of Ru and Si, the energy barrier of water dissociation is significantly reduced. The unique nanostripe structure with abundant interfaces in RSHS will provide a paradigm for construction of efficient catalysts with tunable electronic states and dual active sites.

cond-mat.mtrl-sci

Crystal structure built from a GeO$_6$-GeO$_5$ polyhedra network with high thermal stability: $β$-SrGe$_2$O$_5$

By tackling the challenge of extending transparent oxide semiconductors to Ge based oxides, we have found a not-yet-reported crystal structure, named $β$-SrGe$_2$O$_5$, which is composed of edge-sharing GeO$_6$ octahedra interconnected by GeO$_5$ bipyramids. Single crystals were successfully grown by the high-pressure flux method. $β$-SrGe$_2$O$_5$ has a band gap of 5.2 eV and a dispersive conduction band with an effective mass as small as 0.34 times the electron rest mass, which originates from the edge-sharing GeO$_6$ octahedra network. Although known compounds with octahedral GeO$_6$ coordination are commonly unstable at atmospheric pressure and elevated temperatures, $β$-SrGe$_2$O$_5$ exhibits thermal stability up to 700 $^\circ$C.

cond-mat.mtrl-sci

Pressure-induced Topological and Structural Phase Transitions in an Antiferromagnetic Topological Insulator

Recently, natural van der Waals heterostructures of (MnBi2Te4)m(Bi2Te3)n have been theoretically predicted and experimentally shown to host tunable magnetic properties and topologically nontrivial surface states. In this work, we systematically investigate both the structural and electronic responses of MnBi2Te4 and MnBi4Te7 to external pressure. In addition to the suppression of antiferromagnetic order, MnBi2Te4 is found to undergo a metal-semiconductor-metal transition upon compression. The resistivity of MnBi4Te7 changes dramatically under high pressure and a non-monotonic evolution of \r{ho}(T) is observed. The nontrivial topology is proved to persists before the structural phase transition observed in the high-pressure regime. We find that the bulk and surface states respond differently to pressure, which is consistent with the non-monotonic change of the resistivity. Interestingly, a pressure-induced amorphous state is observed in MnBi2Te4, while two high pressure phase transitions are revealed in MnBi4Te7. Our combined theoretical and experimental research establishes MnBi2Te4 and MnBi4Te7 as highly tunable magnetic topological insulators, in which phase transitions and new ground states emerge upon compression.

cond-mat.supr-con

Natural van der Waals heterostructural single crystals with both magnetic and topological properties

Heterostructures having both magnetism and topology are promising materials for the realization of exotic topological quantum states while challenging in synthesis and engineering. Here, we report natural magnetic van der Waals heterostructures of (MnBi2Te4)m(Bi2Te3)n that exhibit controllable magnetic properties while maintaining their topological surface states. The interlayer antiferromagnetic exchange coupling is gradually weakened as the separation of magnetic layers increases, and an anomalous Hall effect that is well coupled with magnetization and shows ferromagnetic hysteresis was observed below 5 K. The obtained homogeneous heterostructure with atomically sharp interface and intrinsic magnetic properties will be an ideal platform for studying the quantum anomalous Hall effect, axion insulator states, and the topological magnetoelectric effect.

cond-mat.mtrl-sci

Universal van der Waals-type interactions in rattler containing cage materials

Rattling motion of fillers in cage materials has been of great interest for their import roles in superconductivity and thermoelectric applications. The standing waves of the rattling oscillations are normally lower in energy than the propagating waves of the acoustic phonons, thus exert large influences on the configuration of phonon dispersions as well as the associated thermal and electrical properties. Although it has been extensively studied, the origin of the low energy soft modes is still not clear. In the present paper, we show that van der Waals-type interactions are predominant between fillers and their surrounding cage frameworks, which explains the origin of the low energy modes in cage materials as a universal rule. Mass, free space and chemical environment of guest atoms are shown to be the most important factors to determine the three dimensional van der Waals-type interactions. The present work is mainly focused on type-I clathrates, skutterudites and pyrochlores.

cond-mat.mtrl-sci

Gap Structure of the Overdoped Iron-Pnictide Superconductor Ba(Fe$_{0.942}$Ni$_{0.058}$)$_{2}$As$_{2}$: A Low-Temperature Specific-Heat Study

Low-temperature specific heat (SH) is measured on the postannealed Ba(Fe_{1-x}Ni_x)_2As_2 single crystal with x = 0.058 under different magnetic fields. The sample locates on the overdoped sides and the critical transition temperature is determined to be 14.8 K by both the magnetization and SH measurements. A simple and reliable analysis shows that, besides the phonon and normal electronic contributions, a clear T2 termemerges in the low temperature SH data.Our observation is similar to that observed in the Co-doped system in our previous work and is consistent with the theoretical prediction for a superconductor with line nodes in the energy gap.

cond-mat.supr-con