Recent experiments revealed that Mn3Sn and Mn3Ge exhibit a strong anomalous Hall effect at room temperature, provoking us to explore their electronic structures for topological properties. By ab ...initio band structure calculations, we have observed the existence of multiple Weyl points in the bulk and corresponding Fermi arcs on the surface, predicting antiferromagnetic Weyl semimetals in Mn3Ge and Mn3Sn. Here the chiral antiferromagnetism in the Kagome-type lattice structure is essential to determine the positions and numbers of Weyl points. Our work further reveals a new guiding principle to search for magnetic Weyl semimetals among materials that exhibit a strong anomalous Hall effect.
For high-temperature catalytic reaction, it is of significant importance and challenge to construct stable active sites in catalysts. Herein, we report the construction of sufficient and stable ...copper clusters in the copper‒ceria catalyst with high Cu loading (15 wt.%) for the high-temperature reverse water gas shift (RWGS) reaction. Under very harsh working conditions, the ceria nanorods suffered a partial sintering, on which the 2D and 3D copper clusters were formed. This partially sintered catalyst exhibits unmatched activity and excellent durability at high temperature. The interaction between the copper and ceria ensures the copper clusters stably anchored on the surface of ceria. Abundant in situ generated and consumed surface oxygen vacancies form synergistic effect with adjacent copper clusters to promote the reaction process. This work investigates the structure-function relation of the catalyst with sintered and inhomogeneous structure and explores the potential application of the sintered catalyst in C1 chemistry.
Metal-support interaction is of great significance for catalysis as it can induce charge transfer between metal and support, tame electronic structure of supported metals, impact adsorption energy of ...reaction intermediates, and eventually change the catalytic performance. Here, we report the metal size-dependent charge transfer reversal, that is, electrons transfer from platinum single atoms to sulfur-doped carbons and the carbon supports conversely donate electrons to Pt when their size is expanded to ~1.5 nm cluster. The electron-enriched Pt nanoclusters are far more active than electron-deficient Pt single atoms for catalyzing hydrogen evolution reaction, exhibiting only 11 mV overpotential at 10 mA cm
and a high mass activity of 26.1 A mg
at 20 mV, which is 38 times greater than that of commercial Pt/C. Our work manifests that the manipulation of metal size-dependent charge transfer between metal and support opens new avenues for developing high-active catalysts.
Cu‐based metal–organic frameworks have attracted much attention for electrocatalytic CO2 reduction, but they are generally instable and difficult to control the product selectivity. We report ...flexible Cu(I) triazolate frameworks as efficient, stable, and tunable electrocatalysts for CO2 reduction to C2H4/CH4. By changing the size of ligand side groups, the C2H4/CH4 selectivity ratio can be gradually tuned and inversed from 11.8 : 1 to 1 : 2.6, giving C2H4, CH4, and hydrocarbon selectivities up to 51 %, 56 %, and 77 %, respectively. After long‐term electrocatalysis, they can retain the structures/morphologies without formation of Cu‐based inorganic species. Computational simulations showed that the coordination geometry of Cu(I) changed from triangular to tetrahedral to bind the reaction intermediates, and two adjacent Cu(I) cooperated for C−C coupling to form C2H4. Importantly, the ligand side groups controlled the catalyst flexibility by the steric hindrance mechanism, and the C2H4 pathway is more sensitive than the CH4 one.
Flexible Cu(I) triazolate frameworks functionalized with dinuclear copper sites can serve as highly stable and efficient electrocatalysts for CO2 reduction to C2H4/CH4, and the selectivity is tunable by the size of uncoordinated ligand side groups.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
While 5G is being commercialized worldwide, research institutions around the world have started to look beyond 5G and 6G is expected to evolve into green networks, which deliver high Quality of ...Service and energy efficiency. To meet the demands of future applications, significant improvements need to be made in mobile network architecture. We envision 6G undergoing unprecedented breakthrough and integrating traditional terrestrial mobile networks with emerging space, aerial and underwater networks to provide anytime anywhere network access. This paper presents a detailed survey on wireless evolution towards 6G networks. In this survey, the prime focus is on the new architectural changes associated with 6G networks, characterized by ubiquitous 3D coverage, introduction of pervasive AI and enhanced network protocol stack. Along with this, we discuss related potential technologies that are helpful in forming sustainable and socially seamless networks, encompassing terahertz and visible light communication, new communication paradigm, blockchain and symbiotic radio. Our work aims to provide enlightening guidance for subsequent research of green 6G.
Lead (Pb) pollution in natural water bodies is an environmental concern due to toxic effects on aquatic ecosystems and human health, while adsorption is an effective approach to remove Pb from the ...water. Surface interactions between adsorbents and adsorbates play a dominant role in the adsorption process, and properly engineering a material’s surface property is critical to the improvement of adsorption performance. In this study, the magnesium oxide (MgO) nanoparticles stabilized on the N-doped biochar (MgO@N-biochar) were synthesized by one-pot fast pyrolysis of an MgCl2-loaded N-enriched hydrophyte biomass as a way to increase the exchangeable ions and N-containing functional groups and facilitate the adsorption of Pb2+. The as-synthesized MgO@N-biochar has a high performance with Pb in an aqueous solution with a large adsorption capacity (893 mg/g), a very short equilibrium time (<10 min), and a large throughput (∼4450 BV). Results show that this excellent adsorption performance can be maintained with various environmentally relevant interferences including pH, natural organic matter, and other metal ions, suggesting that the material may be suitable for the treatment of wastewater, natural bodies of water, and even drinking water. In addition, MgO@N-biochar quickly and efficiently removed Cd2+ and tetracycline. Multiple characterizations and comparative tests have been performed to demonstrate the surface adsorption and ion exchange contributed to partial Pb adsorption, and it can be inferred from these results that the high performance of MgO@N-biochar is mainly due to the surface coordination of Pb2+ and CO or OC–O, pyridinic, pyridonic, and pyrrolic N. This work suggests that engineering surface functional groups of biochar may be crucial for the development of high performance heavy metal adsorbents.
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IJS, KILJ, NUK, PNG, UL, UM
Crystal-phase engineering offers opportunities for the rational design and synthesis of noble metal nanomaterials with unusual crystal phases that normally do not exist in bulk materials. However, it ...remains a challenge to use these materials as seeds to construct heterometallic nanostructures with desired crystal phases and morphologies for promising applications such as catalysis. Here, we report a strategy for the synthesis of binary and ternary hybrid noble metal nanostructures. Our synthesized crystal-phase heterostructured 4H/fcc Au nanowires enable the epitaxial growth of Ru nanorods on the 4H phase and fcc-twin boundary in Au nanowires, resulting in hybrid Au-Ru nanowires. Moreover, the method can be extended to the epitaxial growth of Rh, Ru-Rh and Ru-Pt nanorods on the 4H/fcc Au nanowires to form unique hybrid nanowires. Importantly, the Au-Ru hybrid nanowires with tunable compositions exhibit excellent electrocatalytic performance towards the hydrogen evolution reaction in alkaline media.
Cobalt imidazolate frameworks are classical electrocatalysts for the oxygen evolution reaction (OER) but suffer from the relatively low activity. Here, a non‐3d metal modulation strategy is presented ...for enhancing the OER activity of cobalt imidazolate frameworks. Two isomorphous frameworks Co4(MO4)(eim)6 (M=Mo or W, Heim=2‐ethylimidazole) having Co(eim)3(MO4) units and high water stabilities were designed and synthesized. In different neutral media, the Mo‐modulated framework coated on a glassy carbon electrode shows the best OER performances (1 mA cm−2 at an overpotential of 210 mV in CO2‐saturated 0.5 m KHCO3 electrolyte and 2/10/22 mA cm−2 at overpotential of 388/490/570 mV in phosphate buffer solution) among non‐precious metal catalysts and even outperforms RuO2. Spectroscopic measurements and computational simulations revealed that the non‐3d metals modulate the electronic structure of Co for optimum reactant/product adsorption and tailor the energy of rate‐determining step to a more moderate value.
Non‐3D for 3D: Introducing non‐3d metal oxide units into a cobalt imidazolate framework results in the drastic enhancement of electrocatalytic performance of the oxygen evolution reaction in neutral media.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
The development of high‐efficiency bifunctional electrocatalyst for oxygen reduction and evolution reactions (ORR/OER) is critical for rechargeable metal–air batteries, a typical electrochemical ...energy storage and conversion technology. This work reports a general approach for the synthesis of Pd@PdO–Co3O4 nanocubes using the zeolite‐type metal–organic framework (MOF) as a template. The as‐synthesized materials exhibit a high electrocatalytic activity toward OER and ORR, which is comparable to those of commercial RuO2 and Pt/C electrocatalysts, while its cycle performance and stability are much higher than those of commercial RuO2 and Pt/C electrocatalysts. Various physicochemical characterizations and density functional theory calculations indicate that the favorable electrochemical performance of the Pd@PdO–Co3O4 nanocubes is mainly attributed to the synergistic effect between PdO and the robust hollow structure composed of interconnected crystalline Co3O4 nanocubes. This work establishes an efficient approach for the controlled design and synthesis of MOF‐templated hybrid nanomaterials, and provides a great potential for developing high‐performance electrocatalysts in energy storage and conversion.
This work reports a general approach to synthesize Pd@PdO‐Co3O4 nanocubes using the zeolite‐type metal–organic framework (MOF) as a template. The as‐synthesized material exhibits a high electrocatalytic activity toward Oxygen evolution and reduction reactions (OER and ORR). Synergistic effects between PdO and the robust hollow structure crystalline Co3O4 nanocubes are the main contributions to the catalyst's excellent performance.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Nanostructured transition metal dichalcogenides (TMDs) are proven to be efficient and robust earth‐abundant electrocatalysts to potentially replace precious platinum‐based catalysts for the hydrogen ...evolution reaction (HER). However, the catalytic efficiency of reported TMD catalysts is still limited by their low‐density active sites, low conductivity, and/or uncleaned surface. Herein, a general and facile method is reported for high‐yield, large‐scale production of water‐dispersed, ultrasmall‐sized, high‐percentage 1T‐phase, single‐layer TMD nanodots with high‐density active edge sites and clean surface, including MoS2, WS2, MoSe2, Mo0.5W0.5S2, and MoSSe, which exhibit much enhanced electrochemical HER performances as compared to their corresponding nanosheets. Impressively, the obtained MoSSe nanodots achieve a low overpotential of −140 mV at current density of 10 mA cm−2, a Tafel slope of 40 mV dec−1, and excellent long‐term durability. The experimental and theoretical results suggest that the excellent catalytic activity of MoSSe nanodots is attributed to the high‐density active edge sites, high‐percentage metallic 1T phase, alloying effect and basal‐plane Se‐vacancy. This work provides a universal and effective way toward the synthesis of TMD nanostructures with abundant active sites for electrocatalysis, which can also be used for other applications such as batteries, sensors, and bioimaging.
A general and facile method is developed for high‐yield, large‐scale production of water‐dispersed, ultrasmall, high‐percentage 1T‐phase, single‐layer transition metal dichalcogenide nanodots with high‐density active edge sites and clean surface, including MoS2, WS2, MoSe2, Mo0.5W0.5S2, and MoSSe, which exhibit much enhanced electrochemical hydrogen evolution reaction performances as compared to their corresponding nanosheets.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
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