Temperature can govern morphologies, structures and properties of products from synthesis in solution. A reaction in solution at low temperature may result in different materials than at higher ...temperature due to thermodynamics and kinetics of nuclei formation. Here, we report a low-temperature solution synthesis of atomically dispersed cobalt in a catalyst with superior performance. By using a water/alcohol mixed solvent with low freezing point, liquid-phase reduction of a cobalt precursor with hydrazine hydrate is realized at -60 °C. A higher energy barrier and a sluggish nucleation rate are achieved to suppress nuclei formation; thus atomically dispersed cobalt is successfully obtained in a catalyst for oxygen reduction with electrochemical performance superior to that of a Pt/C catalyst. Furthermore, the atomically dispersed cobalt catalyst is applied in a microbial fuel cell to obtain a high maximum power density (2550 ± 60 mW m
) and no current drop upon operation for 820 h.
High-efficiency thermoelectric materials require a high conductivity. It is known that a large number of degenerate band valleys offers many conducting channels for improving the conductivity without ...detrimental effects on the other properties explicitly, and therefore, increases thermoelectric performance. In addition to the strategy of converging different bands, many semiconductors provide an inherent band nestification, equally enabling a large number of effective band valley degeneracy. Here we show as an example that a simple elemental semiconductor, tellurium, exhibits a high thermoelectric figure of merit of unity, not only demonstrating the concept but also filling up the high performance gap from 300 to 700 K for elemental thermoelectrics. The concept used here should be applicable in general for thermoelectrics with similar band features.
Writing, erasing and computing are three fundamental operations required by any working electronic device. Magnetic skyrmions could be essential bits in promising in emerging topological spintronic ...devices. In particular, skyrmions in chiral magnets have outstanding properties like compact texture, uniform size, and high mobility. However, creating, deleting, and driving isolated skyrmions, as prototypes of aforementioned basic operations, have been a grand challenge in chiral magnets ever since the discovery of skyrmions, and achieving all these three operations in a single device is even more challenging. Here, by engineering chiral magnet Co
Zn
Mn
into the customized micro-devices for in-situ Lorentz transmission electron microscopy observations, we implement these three operations of skyrmions using nanosecond current pulses with a low current density of about 10
A·m
at room temperature. A notched structure can create or delete magnetic skyrmions depending on the direction and magnitude of current pulses. We further show that the magnetic skyrmions can be deterministically shifted step-by-step by current pulses, allowing the establishment of the universal current-velocity relationship. These experimental results have immediate significance towards the skyrmion-based memory or logic devices.
Compared to commercially available p‐type PbTe thermoelectrics, SnTe has a much bigger band offset between its two valence bands and a much higher lattice thermal conductivity, both of which limit ...its peak thermoelectric figure of merit, zT of only 0.4. Converging its valence bands or introducing resonant states is found to enhance the electronic properties, while nanostructuring or more recently introducing interstitial defects is found to reduce the lattice thermal conductivity. Even with an integration of some of the strategies above, existing efforts do not enable a peak zT exceeding 1.4 and usually involve Cd or Hg. In this work, a combination of band convergence and interstitial defects, each of which enables a ≈150% increase in the peak zT, successfully accumulates the zT enhancements to be ≈300% (zT up to 1.6) without involving any toxic elements. This opens new possibilities for further improvements and promotes SnTe as an environment‐friendly solution for conventional p‐PbTe thermoelectrics.
A combination of band convergence by alloying with MnTe and interstitial defect scattering by alloying with Cu2Te, each of which enables an ≈150% increase in the peak thermoelectric figure of merit, zT of SnTe, successfully accumulates the zT enhancements to be ≈300% without involving any toxic elements. This promotes SnTe as an eco‐friendly solution for p‐PbTe thermoelectrics.
To minimize the lattice thermal conductivity in thermoelectrics, strategies typically focus on the scattering of low-frequency phonons by interfaces and high-frequency phonons by point defects. In ...addition, scattering of mid-frequency phonons by dense dislocations, localized at the grain boundaries, has been shown to reduce the lattice thermal conductivity and improve the thermoelectric performance. Here we propose a vacancy engineering strategy to create dense dislocations in the grains. In Pb
Sb
Se solid solutions, cation vacancies are intentionally introduced, where after thermal annealing the vacancies can annihilate through a number of mechanisms creating the desired dislocations homogeneously distributed within the grains. This leads to a lattice thermal conductivity as low as 0.4 Wm
K
and a high thermoelectric figure of merit, which can be explained by a dislocation scattering model. The vacancy engineering strategy used here should be equally applicable for solid solution thermoelectrics and provides a strategy for improving zT.
Complex structures with versatile chemistry provide considerable chemical tunability of the transport properties. Good thermoelectric materials are generally extrinsically doped semiconductors with ...optimal carrier concentrations, while charged intrinsic defects (e.g., vacancies, interstitials) can also adjust the carriers, even in the compounds with no apparent deviation from a stoichiometric nominal composition. Here we report that in Zintl compounds Mg3+x Sb1.5Bi0.5, the carrier concentration can be tuned from p-type to n-type by simply altering the initial Mg concentration. The spherical-aberration-corrected (C S-corrected) high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDX) mapping analysis show that the excess Mg would form a separate Mg-rich phase after Mg vacancies have been essentially compensated. Additionally, a slight Te doping at Bi site on Mg3.025Sb1.5Bi0.5 has enabled good n-type thermoelectric properties, which is comparable to the Te-doped Mg-rich sample. The actual final composition of Mg3.025Sb1.5Bi0.5 analyzed by EPMA is also close to the stoichiometry Mg3Sb1.5Bi0.5, answering the open question whether excess Mg is prerequisite to realize exceptionally high n-type thermoelectric performance by different sample preparation methods. The motivation for this work is first to understand the important role of vacancy and then to guide for discovering more promising n-type Zintl thermoelectric materials.
Preparation of single atom catalysts (SACs) is of broad interest to materials scientists and chemists but remains a formidable challenge. Herein, we develop an efficient approach to synthesize SACs ...via a precursor-dilution strategy, in which metalloporphyrin (MTPP) with target metals are co-polymerized with diluents (tetraphenylporphyrin, TPP), followed by pyrolysis to N-doped porous carbon supported SACs (M
/N-C). Twenty-four different SACs, including noble metals and non-noble metals, are successfully prepared. In addition, the synthesis of a series of catalysts with different surface atom densities, bi-metallic sites, and metal aggregation states are achieved. This approach shows remarkable adjustability and generality, providing sufficient freedom to design catalysts at atomic-scale and explore the unique catalytic properties of SACs. As an example, we show that the prepared Pt
/N-C exhibits superior chemoselectivity and regioselectivity in hydrogenation. It only converts terminal alkynes to alkenes while keeping other reducible functional groups such as alkenyl, nitro group, and even internal alkyne intact.
Phonon scattering by nanostructures and point defects has become the primary strategy for minimizing the lattice thermal conductivity (κL) in thermoelectric materials. However, these scatterers are ...only effective at the extremes of the phonon spectrum. Recently, it has been demonstrated that dislocations are effective at scattering the remaining mid‐frequency phonons as well. In this work, by varying the concentration of Na in Pb0.97Eu0.03Te, it has been determined that the dominant microstructural features are point defects, lattice dislocations, and nanostructure interfaces. This study reveals that dense lattice dislocations (≈4 × 1012 cm−2) are particularly effective at reducing κL. When the dislocation concentration is maximized, one of the lowest κL values reported for PbTe is achieved. Furthermore, due to the band convergence of the alloyed 3% mol. EuTe the electronic performance is enhanced, and a high thermoelectric figure of merit, zT, of ≈2.2 is achieved. This work not only demonstrates the effectiveness of dense lattice dislocations as a means of lowering κL, but also the importance of engineering both thermal and electronic transport simultaneously when designing high‐performance thermoelectrics.
Eu‐doping effectively converges the valence bands of PbTe, while Na‐doping enables dense lattice dislocations, leading to an extremely low lattice thermal conductivity (κL) of <0.4 W m−1 K−1. This contributes to a high zT of ≈2.2, opening new possibilities for advancing thermoelectrics through dislocation and band‐engineering approaches.
Photochemical solution-phase reactions have been widely applied for the syntheses of nanocrystals. In particular, tuning of the nucleation and growth of solids has been a major area of focus. Here we ...demonstrate a facile approach to generate atomically dispersed platinum via photochemical reduction of frozen chloroplatinic acid solution using ultraviolet light. Using this iced-photochemical reduction, the aggregation of atoms is prevented, and single atoms are successfully stabilized. The platinum atoms are deposited on various substrates, including mesoporous carbon, graphene, carbon nanotubes, titanium dioxide nanoparticles, and zinc oxide nanowires. The atomically dispersed platinum on mesoporous carbon exhibits efficient catalytic activity for the electrochemical hydrogen evolution reaction, with an overpotential of only 65 mV at a current density of 100 mA cm
and long-time durability (>10 h), superior to state-of-the-art platinum/carbon. This iced-photochemical reduction may be extended to other single atoms, for example gold and silver, as demonstrated in this study.
Defects can greatly influence the properties of oxide materials; however, facile defect engineering of oxides at room temperature remains challenging. The generation of defects in oxides is difficult ...to control by conventional chemical reduction methods that usually require high temperatures and are time consuming. Here, we develop a facile room-temperature lithium reduction strategy to implant defects into a series of oxide nanoparticles including titanium dioxide (TiO
), zinc oxide (ZnO), tin dioxide (SnO
), and cerium dioxide (CeO
). Our lithium reduction strategy shows advantages including all-room-temperature processing, controllability, time efficiency, versatility and scalability. As a potential application, the photocatalytic hydrogen evolution performance of defective TiO
is examined. The hydrogen evolution rate increases up to 41.8 mmol g
h
under one solar light irradiation, which is ~3 times higher than that of the pristine nanoparticles. The strategy of tuning defect oxides used in this work may be beneficial for many other related applications.
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