Electrochemical CO
2
reduction reaction (CO
2
RR) is an attractive pathway for closing the anthropogenic carbon cycle and storing intermittent renewable energy by converting CO
2
to valuable ...chemicals and fuels. The production of highly reduced carbon compounds beyond CO and formate, such as hydrocarbon and oxygenate products with higher energy density, is particularly desirable for practical applications. However, the productivity towards highly reduced chemicals is typically limited by high overpotential and poor selectivity due to the multiple electron-proton transfer steps. Tandem catalysis, which is extensively utilized by nature for producing biological macromolecules with multiple enzymes via coupled reaction steps, represents a promising strategy for enhancing the CO
2
RR performance. Improving the efficiency of CO
2
RR via tandem catalysis has recently emerged as an exciting research frontier and achieved significant advances. Here we describe the general principles and also considerations for designing tandem catalysis for CO
2
RR. Recent advances in constructing tandem catalysts, mainly including bimetallic alloy nanostructures, bimetallic heterostructures, bimetallic core-shell nanostructures, bimetallic mixture catalysts, metal-metal organic framework (MOF) and metal-metallic complexes, metal-nonmetal hybrid nanomaterials and copper-free hybrid nanomaterials for boosting the CO
2
RR performance are systematically summarized. The study of tandem catalysis for CO
2
RR is still at the early stage, and future research challenges and opportunities are also discussed.
The exploration of new porous hybrid materials is of great importance because of their unique properties and promising applications in separation of materials, catalysis, etc. Herein, for the first ...time, by integration of metal–organic frameworks (MOFs) and covalent organic frameworks (COFs), a new type of MOF@COF core–shell hybrid material, i.e., NH2‐MIL‐68@TPA‐COF, with high crystallinity and hierarchical pore structure, is synthesized. As a proof‐of‐concept application, the obtained NH2‐MIL‐68@TPA‐COF hybrid material is used as an effective visible‐light‐driven photocatalyst for the degradation of rhodamine B. The synthetic strategy in this study opens up a new avenue for the construction of other MOF–COF hybrid materials, which could have various promising applications.
By integration of metal–organic frameworks (MOFs) and covalent organic frameworks (COFs), a new type of MOF@COF core–shell hybrid material, i.e., NH2‐MIL‐68@TPA‐COF, with high crystallinity and hierarchical pore structure, is synthesized. The obtained hybrid material can be used as an effective visible‐light‐driven photocatalyst for the degradation of rhodamine B.
Functional nanomaterials are playing a crucial role in the emerging field of energy‐related devices. Recently, as a novel synthesis method, high‐temperature shock (HTS), which is rapid, low cost, ...eco‐friendly, universal, scalable, and controllable, has provided a promising option for the rational design and synthesis of various high‐quality nanomaterials. In this report, the HTS technique, including the equipment setup and operating principle, is systematically introduced, and recent progress in the synthesis of nanomaterials for energy storage and conversion applications using this HTS method is summarized. The growth mechanisms of nanoparticles and carbonaceous nanomaterials are thoroughly discussed, followed by the summary of the characteristic advantages of the HTS strategy. A series of nanomaterials prepared by the HTS method, including carbon‐based films, metal nanoparticles and compound nanoparticles, show high performance in the diverse applications of storage energy batteries, highly active catalysts, and smart energy devices. Finally, the future perspectives and directions of HTS in nanomanufacturing for broader applications are presented.
This progress report systematically introduces the high‐temperature shock (HTS) technique, a nanomanufacturing technique that enables rapid reaction, high‐efficiency and low‐cost. The recent progress in the synthesis of nanomaterial employing HTS method for energy storage and conversion applications is summarized. Finally, the future perspectives and challenges of HTS are outlined.
The rational design and synthesis of anisotropic 3D nanostructures with specific composition, morphology, surface structure, and crystal phase is of significant importance for their diverse ...applications. Here, the synthesis of well‐crystalline lotus‐thalamus‐shaped Pt‐Ni anisotropic superstructures (ASs) via a facile one‐pot solvothermal method is reported. The Pt‐Ni ASs with Pt‐rich surface are composed of one Ni‐rich “core” with face‐centered cubic (fcc) phase, Ni‐rich “arms” with hexagonal close‐packed phase protruding from the core, and facet‐selectively grown Pt‐rich “lotus seeds” with fcc phase on the end surfaces of the “arms.” Impressively, these unique Pt‐Ni ASs exhibit superior electrocatalytic activity and stability toward the hydrogen evolution reaction under alkaline conditions compared to commercial Pt/C and previously reported electrocatalysts. The obtained overpotential is as low as 27.7 mV at current density of 10 mA cm−2, and the turnover frequency reaches 18.63 H2 s−1 at the overpotential of 50 mV. This work provides a new strategy for the synthesis of highly anisotropic superstructures with a spatial heterogeneity to boost their promising application in catalytic reactions.
Well‐crystalline lotus‐thalamus‐shaped Pt‐Ni anisotropic superstructures (ASs) with unique hexagonal‐close‐packed/face‐centered‐cubic crystal phases and Pt‐rich surface are synthesized via a simple one‐pot solvothermal method. The obtained Pt‐Ni ASs exhibit superior electrocatalytic activity and stability toward the hydrogen evolution reaction under alkaline conditions compared to commercial Pt/C and other reported electrocatalysts.
Gastrointestinal involvement is not uncommon in patients with disseminated talaromycosis, but successful management of massive gastrointestinal bleeding and hemorrhagic shock secondary to ...talaromycosis is rarely reported. Clinical management strategies for these patients have not been well documented.
Here, we reported a case of disseminated talaromycosis with recurrent gastrointestinal bleeding and hemorrhagic shock who was successfully alleviated solely with medical treatment.
Early diagnosis and treatment for Talaromyces marneffei, intravenous fluid resuscitation, hemostatic therapy and blood transfusion are all essential for talaromycosis complicated with gastrointestinal bleeding and hemorrhagic shock. It is also necessary to warn about the possibility of bleeding induced or aggravated by endoscopic biopsy trauma.
Fractal metallic dendrites have been drawing more attentions recently, yet they have rarely been explored in electronic printing or packaging applications because of the great challenges in ...large-scale synthesis and limited understanding in such applications. Here we demonstrate a controllable synthesis of fractal Ag micro-dendrites at the hundred-gram scale. When used as the fillers for isotropically electrically conductive composites (ECCs), the unique three-dimensional fractal geometrical configuration and low-temperature sintering characteristic render the Ag micro dendrites with an ultra-low electrical percolation threshold of 0.97 vol% (8 wt%). The ultra-low percolation threshold and self-limited fusing ability may address some critical challenges in current interconnect technology for microelectronics. For example, only half of the laser-scribe energy is needed to pattern fine circuit lines printed using the present ECCs, showing great potential for wiring ultrathin circuits for high performance flexible electronics.
Radiation-induced in situ tumor vaccination alone is very weak and insufficient to elicit robust antitumor immune responses. In this work, we address this issue by developing chiral vidarabine ...monophosphate-gadolinium nanowires (aAGd-NWs) through coordination-driven self-assembly. We elucidate the mechanism of aAGd-NW assembly and characterize their distinct features, which include a negative surface charge, ultrafine topography, and right-handed chirality. Additionally, aAGd-NWs not only enhance X-ray deposition but also inhibit DNA repair, thereby enhancing radiation-induced in situ vaccination. Consequently, the in situ vaccination induced by aAGd-NWs sensitizes radiation enhances CD8
T-cell-dependent antitumor immunity and synergistically potentiates the efficacy immune checkpoint blockade therapies against both primary and metastatic tumors. The well-established aAGd-NWs exhibit exceptional therapeutic capacity and biocompatibility, offering a promising avenue for the development of radioimmunotherapy approaches.
The revolutionary improvement of hardware and algorithm in cryogenic electron microscopy (cryo‐EM) has made it a routine method to obtain structures of macromolecules at near‐atomic resolution. ...Nevertheless, this technique still faces many challenges. The structure‐solving efficiency of cryo‐EM can be significantly reduced by the biomolecules' denaturation on the air–water interfaces, the preferred orientation, strong background noise from supporting films and particle motion, and so forth. To overcome these problems, nanomaterials with ultrahigh electronic conductivity and ultrathin thickness are explored as promising cryo‐EM specimen supporting films. Herein, we summarize the structural engineering of graphene, for example, surface and interface modification, as supporting films for grids and the application on high‐resolution cryo‐EM and discuss potential future perspectives.
The functionalized graphene‐based cryogenic electron microscopy (cryo‐EM) grids show superior properties, such as good conductivity, mechanical strength, selectivity on target macromolecules, hydrophilicity, and very low background noise. We believe that the structural engineering of graphene and even other 2D materials will broaden the application for high‐resolution cryo‐EM and significantly improve the development of methodology.
In our work, by constructing an inverse heterogeneous catalyst, e.g., Fe2O3 partially covered on the surface of Pd, we found that this catalyst can effectively transform methanol into formaldehyde ...with high activity and selectivity. Then, we proposed a deep insight into the interfacial effect from the point from atomic, electronic, geometric and electrochemical reaction pathways viewpoint aspect.
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Different from traditional metal-support heterogenous catalysts, inverse heterogeneous catalysts, in which the surface of metal is decorated by metal oxide, have recently attracted increasing interests owing to the unique interfacial effect and electronic structure. However, a deep insight into the effect of metal-oxide interaction on the catalytic performance still remains a great challenge. In our work, an inverse hematite/palladium (Fe2O3/Pd) hybrid nanostructure, i.e., the active Fe2O3 ultrathin oxide layers partially covering on the surface of Pd nanoparticles (NPs), exhibited superior electrocatalytic performance towards methanol oxidation reaction (MOR) as compared to the bare Pd NPs based on density functional theory calculation. The charge could transfer from Pd to Fe2O3 driven by the built-in potential at the interface of Pd and Fe2O3, which favors the downshift of d band center of Pd. With the assistance of interfacial hydroxyl OH*, the cleavage of OH and CH in CH3OH could take place much easily with lower barrier energy on Fe2O3/Pd than that on pure Pd via two electrons transferring reaction pathways. Our results highlight that the synergy of Pd and Fe2O3 at the interface could facilitate the electrochemical transformation of methanol into formaldehyde assisted with interfacial hydroxyl OH*.
The rational design and synthesis of hybrid-type electrode nanomaterials are significant for their diverse applications, including their potential usage as high-efficiency nanoarchitectures for ...supercapacitors (SCs) as a class of promising energy-storage systems for powering next-generation electric vehicles and electronic devices. Here, we reported a facile and controllable synthesis of core-shell NiS/Ni
3
S
2
@ NiWO
4
nanoarrays to fabricate a freestanding electrode for hybrid SCs. Impressively, the as-prepared freestanding NiS/Ni
3
S
2
@NiWO
4
electrode presents an ultrahigh areal capacity of 2032 µA h cm
−2
at 5 mA cm
−2
, and a capacity retention of 63.6% even when the current density increased up to 50 mA cm
−2
. Remarkably, the NiS/Ni
3
S
2
@NiWO
4
nanoarray-based hybrid SC delivers a maximum energy density of 1.283 mW h cm
−2
at 3.128 mW cm
−2
and a maximum power density of 41.105 mW cm
−2
at 0.753 mW h cm
−2
. Furthermore, the hybrid SC exhibits a capacity retention of 89.6% even after continuous 10,000 cycles, proving its superior stability. This study provides a facile pathway to rationally design a variety of core shell metal nanostructures for high performance energy storage devices.
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