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1.
Angew Chem Int Ed Engl ; : e202413297, 2024 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-39269331

RESUMO

Current industrial propane dehydrogenation (PDH) processes predominantly use either toxic Cr-based or expensive Pt-based catalysts, necessitating urgent exploration for alternatives. Herein, we present Zn2SiO4, an easily prepared, cost-effective material, as a highly efficient and stable catalyst for PDH. Uniquely, Zn2SiO4 nanocrystals do not require dispersion on support materials, commonly needed for catalytic active oxide clusters, but function as a self-supporting catalyst instead. During the reaction's induction period, surface Zn species on the Zn2SiO4 crystal reduce to coordinately unsaturated ZnOx single sites, serving as highly active catalytic centers. The Zn2SiO4 catalyst demonstrates a stable performance over 200 hours of PDH operation at 550 °C. We further find that introducing a minuscule amount of CO2 into the propane feed significantly extends the catalyst lifespan to over 2000 hours. This enhancement arises from the special role of CO2 in facilitating the removal of strongly adsorbed H*, preventing the complete reduction of ZnOx. After prolonged reaction, the activity of Zn2SiO4 can be fully restored by etching the surface layer to expose fresh Zn species, available throughout the crystals. The combination of CO2 introduction and catalytic site regeneration strategies is expected to enable a year-long PDH operation using a single batch of Zn2SiO4 catalyst.

2.
Molecules ; 28(12)2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-37375344

RESUMO

Aqueous zinc ion batteries (AZIBs) are promising electrochemical energy storage devices due to their high theoretical specific capacity, low cost, and environmental friendliness. However, uncontrolled dendrite growth poses a serious threat to the reversibility of Zn plating/stripping, which impacts the stability of batteries. Therefore, controlling the disordered dendrite growth remains a considerable challenge in the development of AZIBs. Herein, a ZIF-8-derived ZnO/C/N composite (ZOCC) interface layer was constructed on the surface of the Zn anode. The homogeneous distribution of zincophilic ZnO and the N element in the ZOCC facilitates directional Zn deposition on the (002) crystal plane. Moreover, the conductive skeleton with a microporous structure accelerates Zn2+ transport kinetics, resulting in a reduction in polarization. As a result, the stability and electrochemical properties of AZIBs are improved. Specifically, the ZOCC@Zn symmetric cell sustains over 1150 h at 0.5 mA cm-2 with 0.25 mA h cm-2, while the ZOCC@Zn half-cell achieves an outstanding Coulombic efficiency of 99.79% over 2000 cycles. This work provides a simple and effective strategy for improving the lifespan of AZIBs.

3.
Molecules ; 27(15)2022 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-35897949

RESUMO

Reasonable structural design and composition control are the dominant factors for tuning the electromagnetic absorbing properties of materials. In this paper, microspheres composed of NiO, Ni, and Co3O4 nanoparticles (NCMO) were successfully synthesized using a mild oxidation method. Benefiting from the multi-component composition and a unique microstructure, the RLmin of CNMO can reach -46.8 dB at 17 GHz, with an effective absorption bandwidth of 4.1 GHz (13.9-18 GHz). The absorbing properties and the absorbing mechanism analysis showed that the microsphere-structured NCMO composed of multi-component nanoparticles enhanced the interface polarization, thereby improving the absorption performance. This research provides a new avenue for MOF-derived oxide materials with excellent electromagnetic wave absorbing properties.

4.
Molecules ; 28(1)2022 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-36615427

RESUMO

Recently, the development of composite materials composed of magnetic materials and MXene has attracted significant attention. However, the thickness and microwave absorption performance of the composite is still barely satisfactory. In this work, the C-N@NiFe2O4@MXene/Ni nanocomposites were successfully synthesized in situ by hydrothermal and calcination methods. Benefiting from the introduction of the carbon-nitrogen(C-N) network structure, the overall dielectric properties are improved effectively, consequently reducing the thickness of the composite while maintaining excellent absorption performance. As a result, the minimum reflection loss of C-N@NiFe2O4@MXene/Ni can reach -50.51 dB at 17.3 GHz at an ultralow thickness of 1.5 mm, with an effective absorption bandwidth of 4.95 GHz (13.02-18 GHz). This research provides a novel strategy for materials to maintain good absorption performance at an ultralow thickness level.

5.
Nanoscale ; 16(7): 3701-3713, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-38291954

RESUMO

The designability of the porous structure of carbon material makes it a popular material for zinc-ion hybrid capacitors (ZIHCs). However, the micropore confinement effect leads to sluggish kinetics and is not well resolved yet. In this work, a pore-size controllable carbon material was designed to enhance ion accessibility. The experimental and calculated results revealed that suitable pore sizes and defects were beneficial to ion transfer/adsorption. Meanwhile, oxygen-containing functional groups could introduce a pseudocapacitance reaction. Its large specific surface area and interconnecting network structure could shorten the ion/electron transfer length to reach high ion adsorption capacity and fast kinetic behavior. When used as a zinc-ion hybrid capacitor cathode material, it showed 9.9 kW kg-1 power density and 100 W h kg-1 energy density. Even at 5 A g-1, after 50 000 cycles, there was still 93% capacity retention. Systemic ex situ characterization and first-principles calculations indicated that the excellent electrochemical performance is attributed to the electric double layer capacitance (EDLC) - pseudocapacitance coupled mechanism via the introduction of an appropriate amount of oxygen-containing functional groups. This work provides a robust design for pore engineering and mechanistic insights into rapid zinc-ion storage in carbon materials.

6.
Chem Commun (Camb) ; 60(67): 8928-8931, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-39093012

RESUMO

Here, we report a gold-furnished mesh as the current collector for Zn electrodeposition, which is used as the anode in aqueous zinc-ion batteries. The anode exhibits excellent cycling performance without obvious dendrite growth, and the full cell shows an outstanding specific capacity and long-term durability, surpassing those of bare Zn.

7.
ACS Appl Mater Interfaces ; 16(10): 12781-12792, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38415631

RESUMO

The traditional methods for creating oxygen vacancies in materials present several challenges and limitations, such as high preparation temperatures, limited oxygen vacancy generation, and morphological destruction, which hinder the application of transition metal oxides in the field of zinc-air batteries (ZABs). In order to address these limitations, we have introduced a pioneering lithium reduction strategy for generating oxygen vacancies in δ-MnO2@MXene composite materials. This strategy stands out for its simplicity of implementation, applicability at room temperature, and preservation of the material's structural integrity. This research demonstrates that aqueous Ov-MnO2@MXene-5, with introduced oxygen vacancies, exhibits an outstanding oxygen reduction reaction (ORR) activity with an ORR half-wave potential reaching 0.787 V. DFT calculations have demonstrated that the enhanced activity could be attributed to adjustments in the electronic structure and alterations in adsorption bond lengths. These adjustments result from the introduction of oxygen vacancies, which in turn promote electron transport and catalytic activity. In the context of zinc-air batteries, cells with Ov-MnO2@MXene-5 as the air cathode exhibit outstanding performance, featuring a significantly improved maximum power density (198.3 mW cm-2) and long-term cycling stability. Through the innovative strategy of introducing oxygen vacancies, this study has successfully enhanced the electrochemical catalytic performance of MnO2, overcoming the limitations associated with traditional methods for creating oxygen vacancies. Consequently, this research opens up new avenues and directions for nonprecious metal catalyst application in ZABs.

8.
J Colloid Interface Sci ; 621: 169-179, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35461132

RESUMO

Benefitting from the abundance and inexpensive nature of potassium resources, potassium-ion energy storage technology is considered a potential alternative to current lithium-ion systems. Potassium-ion capacitors (PICs) as a burgeoning K-ion electrochemical energy storage device, are capable of delivering high energy at high power without sacrificing lifespan. However, owing to the sluggish kinetics and significant volume change induced by the large K+-diameter, matched electrode materials with good ion accessibility and fast K+ intercalation/deintercalation capability are urgently desired. In this work, pine needles and graphene oxide (GO) are utilized as precursors to fabricate oxygen-doped activated carbon/graphene (OAC/G) porous nanosheet composites. The introduction of GO not only induces the generation of interconnected nanosheet network, but also increases the oxygen-doping content of the composite, thus expanding the graphite interlayer spacing. Experimental analysis combined with first-principle calculations reveal the transport/storage mechanism of K+ in the OAC/G composite anode, demonstrating that the high surface area, sufficient reactive sites, enlarged interlayer distance and open channels in the porous nanosheet network contribute to rapid and effective K+ diffusion and storage. When incorporated with pine needle-activated carbon as cathode, the assembled dual-carbon PICs can function at a high voltage of 5 V, exhibiting a high energy density of 156.7 Wh kg-1 at a power density of 500 W kg-1 along with a satisfied cycle life, which highlights their potential application in economic and advanced PICs.

9.
Nanoscale ; 12(40): 20710-20718, 2020 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-33029601

RESUMO

A transition metal phosphide is an excellent candidate for supercapacitors due to its superior electrical conductivity and high theoretical capacity. In addition, compared with traditional 3D nano-materials, 2D nanosheets possess a greater specific surface area and shorter electron transport distance. In this study, a reasonable approach is proposed for the synthesis of ZIF-67 nanosheets on nickel foam with subsequent phosphorization by chemical vapor deposition (CVD) to obtain flake-like CoP combined with Ni2P (NCP/NF), in which nickel foam serves as the current collector as well as the resource of Ni to form Ni2P. Benefiting from the nanosheet array of CoP, the NCP/NF can improve the capacity of Ni2P from 0.57 C cm-2 to 1.43 C cm-2 at 1 mA cm-2. Furthermore, the NPC/NF/reduced graphene oxide (RGO) asymmetric supercapacitor (ASC) shows an energy density of 26.9 µW h cm-2 at a power density of 0.896 mW cm-2, and excellent cycling performance with a capacity retention of 93.75% after 5000 cycles at 10 mA cm-2.

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