Ambient electrochemical N2 reduction is emerging as a highly promising alternative to the Haber–Bosch process but is typically hampered by a high reaction barrier and competing hydrogen evolution, leading to an extremely low Faradaic efficiency. Here, we demonstrate that under ambient conditions, a single-atom catalyst, iron on nitrogen-doped carbon, could positively shift the ammonia synthesis process to an onset potential of 0.193 V, enabling a dramatically enhanced Faradaic efficiency of 56.55%. The only doublet coupling representing 15NH4+ in an isotopic labeling experiment confirms reliable NH3 production data. Molecular dynamics simulations suggest efficient N2 access to the single-atom iron with only a small energy barrier, which benefits preferential N2 adsorption instead of H adsorption via a strong exothermic process, as further confirmed by first-principle calculations. The released energy helps promote the following process and the reaction bottleneck, which is widely considered to be the first hydrogenation step, is successfully overcome.
By substituting Fe with the 5d-transition metal Pt in BaFe2As2, we have successfully synthesized the superconductors BaFe2−xPtxAs2. The systematic evolution of the lattice constants indicates that the Fe ions were successfully replaced by Pt ions. By increasing the doping content of Pt, the antiferromagnetic order and structural transition of the parent phase is suppressed and superconduc-tivity emerges at a doping level of about x = 0.02. At a doping level of x = 0.1, we get a maximum transition temperature Tc of about 25 K. While even for this optimally doped sample, the residual resistivity ratio (RRR) is only about 1.35, indicating a strong impurity scattering effect. We thus argue that the doping to the Fe-sites naturally leads to a high level impurity scattering, although the superconductivity can still survive at about 25 K. The synchrotron powder x-ray diffraction shows that the resistivity anomaly is in good agreement with the structural transition. The super-conducting transitions at different magnetic fields were also measured at the doping level of about x = 0.1, yielding a slope of-dHc2/dT = 5.4 T/K near Tc. Finally a phase diagram was established for the Pt doped 122 system. Our results suggest that superconductivity can also be easily induced in the FeAs family by substituting the Fe with Pt, with almost the similar maximum transition temperatures as doping Ni, Co, Rh and Ir.
We present a study of angle-resolved quantum oscillations of electric and thermoelectric transport coefficients in semi-metallic WTe2, which has the particularity of displaying a large B 2 magnetoresistance. The Fermi surface consists of two pairs of electron-like and hole-like pockets of equal volumes in a "Russian doll" structure. Carrier density, Fermi energy, mobility and the mean-freepath of the system are quantified. An additional frequency is observed above a threshold field and attributed to magnetic breakdown across two orbits. In contrast to all other dilute metals, the Nernst signal remains linear in magnetic field even in the high-field (ωcτ ≫ 1) regime. Surprisingly, none of the pockets extend across the c-axis of the first Brillouin zone, making the system a three-dimensional metal with moderate anisotropy in Fermi velocity yet a large anisotropy in mean-free-path. 2 ) was reported with no sign of saturation up to 60 T[6]. This is the expected behavior of a perfectly-compensated semi-metal [7], but has not been seen in bismuth [8] or graphite [9], two compensated semi-metals whose Fermi surface is accurately known. A first step towards uncovering the ultimate reason behind the quadratic magnetoresistance of WTe 2 is a quantitative determination of the structure of the Fermi surface and the components of the mobility tensor.In this letter, we report on a study of quantum oscillations of resistivity, Seebeck and Nernst coefficients in high-quality single crystals of WTe 2 and find that the Fermi surface consists of two pairs of electron-like and hole-like pockets. Each pair is concentric with identical structure like a set of Russian dolls. The anisotropy is much smaller than one would naively expect in a layered system. The longer axis of the pockets is much shorter than the height of the Brillouin zone, in contrast to the theoretical expectations. Moreover, we find another distinctive feature of this semi-metal in addition to quadratic magnetoresistance, which is a Nernst response linear in magnetic field deep inside the high-field limit. Our results quantify carrier concentration of the system and set plausible quantitative windows for mobilities and Fermi energies leading to the huge quadratic magnetoresistance and large field-linear Nernst signal.
We have studied EuFe2(As0.7P0.3)2 by the measurements of x-ray diffraction, electrical resistivity, thermopower, magnetic susceptibility, magnetoresistance and specific heat. Partial substitution of As with P results in the shrinkage of lattice, which generates chemical pressure to the system. It is found that EuFe2(As0.7P0.3)2 undergoes a superconducting transition at 26 K, followed by ferromagnetic ordering of Eu 2+ moments at 20 K. This finding is the first observation of superconductivity stabilized by internal chemical pressure, and supplies a rare example showing coexistence of superconductivity and ferromagnetism in the ferro-arsenide family.
A new type of amino polar binder with 3D network flexibility structure for high energy Li-S batteries is synthesized and successfully used with commercial sulfur powder cathodes. The binder shows significant performance improvement in capacity retention and high potential for practical application, which arouse the battery community's interest in the commercial application of high energy Li-S battery.
Ternary iron arsenide EuFe2As2 with ThCr2Si2-type structure has been studied by magnetic susceptibility, resistivity, thermopower, Hall and specific heat measurements. The compound undergoes two magnetic phase transitions at about 200 K and 20 K, respectively. The former was found to be accompanied with a slight drop in magnetic susceptibility (after subtracting the Curie-Weiss paramagnetic contribution), a rapid decrease in resistivity, a large jump in thermopower and a sharp peak in specific heat with decreasing temperature, all of which point to a spin-density-wave-like antiferromagnetic transition. The latter was proposed to be associated with an A-type antiferromagnetic ordering of Eu 2+ moments. Comparing with the physical properties of the iso-structural compounds BaFe2As2 and SrFe2As2, we expect that superconductivity could be induced in EuFe2As2 through appropriate doping. [18,19,20] EuFe 2 As 2 is another member of the ternary iron arsenide family, [21] however, only few work was performed on this material. Mössbauer and magnetic susceptibility studies [22] indicated that EuFe 2 As 2 experienced two magnetic transitions. The first one around 200 K was due to the AFM transition in the iron sublattice. The second one at 19 K arose from the AFM ordering of Eu 2+ magnetic moments. No other physical properties of EuFe 2 As 2 have been reported. In order to assess the potential of inducing superconductivity in this compound, we have carried out a systematic study of the physical properties of EuFe 2 As 2 . We found that the transition at about 200 K was accompanied by a rapid decrease in resistivity, a large jump in thermopower and a sharp peak in specific heat. In addition, a slight drop in magnetic susceptibility was observed after subtracting the Curie-Weiss paramagnetic contribution of Eu 2+ magnetic moments. These properties are quite similar with those of BaFe 2 As 2 and SrFe 2 As 2 , suggesting that EuFe 2 As 2 is another possible parent compound in which superconductivity may be found by proper doping. Polycrystalline samples of EuFe 2 As 2 were synthesized from stoichiometric amounts of the elements as reported previously [21]. Fresh Eu grains, Fe powders and As grains were mixed in a ratio of 1:2:2, sealed in an evacuated quartz tube and sintered at 773 K for 12 hours then 1073 K for another 12 hours. After cooling, the reaction product was thoroughly ground in an agate mortar and pressed into pellets under a pressure of 2000 kg/cm 2 in an argon-filled glove-box. The pellets were annealed in an evacuated quartz tube at 1123 K for 12 hours and furnace-cooled to room temperature. The EuFe 2 As 2 samples were obtained as black powders, which is stable in air.
With over fivefold energy capacity, sulfur demonstrates superior advantages over current commercial intercalation compound (LiCoO 2 and LiFePO 4 ) cathode materials. [3][4][5] Despite its considerable advantages, the practical application of Li-S battery has been hindered by poor cycle life due to the shuttle effect, leading to quick capacity decay due to the loss of active materials and an low Coulombic efficiency. [6,7] Moreover, the insulating nature of S/Li 2 S and as large as 78% volume expansion of sulfur cathode when initial state S (2.03 g cm −3 ) is fully converted to final state Li 2 S (1.66 g cm −3 ) result in rapid capacity fading and short cycle life due to the low utilization of active materials and poor electrical contact between sulfur particles and conductive additives. [8,9] Aiming to address these negative impact of at least some of the detrimental processes described above for realizing commercial application of highenergy Li-S battery, various considerable strategies have been focused on cathode material modification including N-doped materials, [10][11][12] porous materials, [13] hierarchical materials, [14] metal oxides [15,16] transition metal disulfides, [17] and functional separator modification, [18,19] as well as employment of solid or As one of the important ingredients in lithium-sulfur battery, the binders greatly impact the battery performance. However, conventional binders have intrinsic drawbacks such as poor capability of absorbing hydrophilic lithium polysulfides, resulting in severe capacity decay. This study reports a new type of binder by polymerization of hydrophilic poly(ethylene glycol) diglycidyl ether with polyethylenimine, which enables strongly anchoring polysulfides for highperformance lithium sulfur batteries, demonstrating remarkable improvement in both mechanical performance for standing up to 100 g weight and an excellent capacity retention of 72% over 400 cycles at 1.5 C. Importantly, in situ micro-Raman investigation verifies the effectively reduced polysulfides shuttling from sulfur cathode to lithium anode, which shows the greatly suppressed shuttle effect by the polar-functional binder. X-ray photoelectron spectroscopy analysis into the discharge intermediates upon battery cycling reveals that the hydrophilic binder endows the sulfur electrodes with multidimensional Li-O, Li-N, and S-O interactions with sulfur species to effectively mitigate lithium polysulfide dissolution, which is theoretically confirmed by density-functional theory calculations.
Lithium metal, the ideal anode material for rechargeable batteries, suffers from the inherent limitations of sensitivity to the humid atmosphere and dendrite growth. Herein, low-cost fabrication of a metallic-lithium anode that is stable in air and plated dendrite-free from an organic-liquid electrolyte solves four key problems that have plagued the development of large-scale Li-ion batteries for storage of electric power. Replacing the low-capacity carbon anode with a safe, dendrite-free lithium anode provides a fast charge while reducing the cost of fabrication of a lithium battery, and increasing the cycle life of a rechargeable cell by eliminating the liquid-electrolyte ethylene-carbonate additive used to form a solid-electrolyte interphase passivation layer on the anode that is unstable during cycling. This solution is accomplished by formation of a hydrophobic solid-electrolyte interphase on a metallic-lithium anode that allows for handling of the treated lithium anode membrane in a standard dry room during cell fabrication.
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