Latest ArticlesLeveraging the interplay between the metal component and the supporting material represents a cornerstone strategy for augmenting electrocatalytic efficiency, e.g., electrocatalytic CO2 reduction reaction (CO2RR). Herein, we employ freestanding porous carbon fibers (PCNF) as an efficacious and stable support for the uniformly distributed SnO2 nanoparticles (SnO2PCNF), thereby capitalizing on the synergistic support effect that arises from their strong interaction. On one hand, the interaction between the SnO2 nanoparticles and the carbon support optimizes the electronic configuration of the active centers. This interaction leads to a noteworthy shift of the d-band center toward stronger intermediate adsorption energy, consequently lowering the energy barrier associated with CO2 reduction. As a result, the SnO2PCNF realizes a remarkable CO2RR performance with excellent selectivity towards formate (98.1%). On the other hand, the porous carbon fibers enable the uniform and stable dispersion of SnO2 nanoparticles, and this superior porous structure of carbon supports can also facilitate the exposure of the SnO2 nanoparticles on the reaction interface to a great extent. Consequently, adequate contact between active sites, reactants, and electrolytes can significantly increase the metal utilization, eventually bringing forth a remarkable 7.09 A/mg mass activity. This work might provide a useful idea for improving the utilization rate of metals in numerous electrocatalytic reactions.
Weakly solvating electrolyte (WSE) demonstrates superior compatibility with lithium (Li) metal batteries (LMBs). However, its application in fast-charging high-voltage LMBs is challenging. Here, we propose a diluent modified WSE for fast-charging high-voltage LMBs, which is formed by adding diluent of 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) into the tetrahydropyran (THP) based WSE. A relatively loose solvation structure is formed due to the formation of weak hydrogen bond between TTE and THP, which accelerates the de-solvation kinetics of Li+. Besides, more anions are involved in solvation structure in the presence of TTE, yielding inorganic-rich interphases with improved stability. Li (30 µm)LiNi0.5 Co0.2Mn0.3O2 (4.1 mAh/cm2) batteries with the TTE modified WSE retain over 64% capacity retention after 175 cycles under high rate of 3 C and high-voltage of 4.5 V, much better than that with pure THP based WSE. This work points out that the combination of diluent with weakly solvating solvent is a promising approach to develop high performance electrolytes for fast-charging high-voltage LMBs.
Available online Alkaline water electrolysis (AWE) is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure. Noble metal-based electrocatalysts, owing to their exceptional hydrogen binding energy, exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction (HER). However, the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts. This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst, while considering the principles of sustainable development. The initial discussion covers the fundamental principle of HER, followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals, along with a thorough examination of recent advancements. The subsequent discussion focuses on the strategies employed to improve noble metal-based catalysts, including enhancing the intrinsic activity at active sites and increasing the quantity of active sites. Ultimately, this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.
Customized design of well-defined cathode structures with abundant adsorption sites and rapid diffusion dynamics, holds great promise in filling capacity gap of carbonaceous cathodes towards high-performance Zn-ion hybrid supercapacitors (ZHC). Herein, we fabricate a series of dynamics-oriented hierarchical porous carbons derived from the unique organic-inorganic interpenetrating polymer networks. The interpenetrating polymer networks are obtained through physically knitting polyferric chloride (PFC) network into the highly crosslinked resorcinol-formaldehyde (RF) network. Instead of covalent bonding, physical interpenetrating force in such RF-PFC networks efficiently relieves the RF skeleton shrinkage upon pyrolysis. Meanwhile, the in-situ PFC network sacrifices as a structure-directing agent to suppress the macrophase separation, and correspondingly 3D hierarchical porous structure with plentiful ion-diffusion channels (pore volume of 1.35 cm3/g) is generated in the representative HPC4 via nanospace occupation and swelling effect. Further removal of Fe fillers leaves behind a large accessible specific surface area of 1550 m2/g for enhanced Zn-ion adsorption. When used as the cathode for ZHC, HPC4 demonstrates a remarkable electrochemical performance with a specific capacity of 215.1 mAh/g at 0.5 A/g and a high Zn2+ ion diffusion coefficient of 11.1 × 10−18 cm2/s. The ZHC device yields 117.0 Wh/kg energy output at a power density of 272.1 W/kg, coupled with good cycle lifespan (100,000 cycles@10 A/g). This work inspires innovative insights to accelerate Zn diffusion dynamics by structure elaboration towards high-capacity cathode materials.
Hydrogen, as a cheap, clean, and cost-effective secondary energy source, performs an essential role in optimizing today’s energy structure. Magnesium hydride (MgH2) represents an attractive hydrogen carrier for storage and transportation, however, the kinetic behavior and operating temperature remain undesirable. In this work, a dual-phase multi-site alloy (MsA) anchored on carbon substrates was designed, and its superior catalytic effects on the hydrogen storage properties of MgH2 were reported. Mechanism analysis identified that multi-site FeNi3/NiCu nanoalloys synergistically served as intrinsic drivers for the striking de/hydrogenation performance of the MgH2−MsA systems. Concretely, the unique multi-metallic site structure attached to the surface of MgH2 provided substantial reversible channels and accessible active sites conducive to the adsorption, activation, and nucleation of H atoms. In addition, the coupling system formed by FeNi3 and NiCu dual-phase alloys further enhanced the reactivity between Mg/MgH2 and H atoms. Hence, the onset dehydrogenation temperature of MgH2 + 5 wt% MsA was reduced to 195 ℃ and the hydrogen desorption apparent activation energy was reduced to 83.6 kJ/mol. 5.08 wt% H2 could be released at 250 ℃ in 20 min, reaching a high dehydrogenation rate of 0.254 wt% H2/min, yet that for MgH2 at a higher temperature of 335 ℃ was only 0.145 wt% H2/min. Then, the dehydrogenated MgH2−MsA sample could absorb hydrogen from room temperature (30 ℃) and charge 3.93 wt% H2 at 100 ℃ within 20 min under 3.0 MPa H2 pressure. Benefiting from carbon substrates, the 5 wt% MsA doped-MgH2 could still maintain 6.36 wt% hydrogen capacity after 20 cycles. In conclusion, this work provides experimental rationale and new insights for the design of efficient catalysts for magnesium-based solid-state hydrogen storage materials.
All-solid-state Li batteries (ASSLBs) using solid electrolytes (SEs) have gained significant attention in recent years considering the safety issue and their high energy density. Despite these advantages, the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites. Elemental doping is an effective and direct method to enhance the performance of SEs. Here, we report an Al-F co-doping strategy to improve the overall properties including ion conductivity, high voltage stability, and cathode and anode compatibility. Particularly, the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases, thereby constructing a relatively stable interface and promoting uniform Li deposition. The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series. ASSLBs assembled with these optimized electrolytes gain good electrochemical performance, demonstrating the universality of Al-F co-doping towards advanced SEs.
The oxygen reduction reaction (ORR) is a crucial process in Zn-air systems, and the catalyst plays a significant role in this reaction. However, reported catalysts often suffer from poor durability and stability during the ORR process. Herein, we synthesized La-Fe bimetallic nanoparticles encapsulated in a N-doped porous carbon dodecahedron (La-Fe/NC) originated from ZIF-8 by a simple direct carbonization. The La-Fe/NC catalyst had a numerous mesopores and dendritic outer layer generated by carbon nanotubes (CNTs), forming a high conductivity network that helped to optimize electron transfer and mass transport in the ORR process. The effect of different doping transition metals and metal ratios on the ORR activity of Zn-air batteries was investigated. In alkaline media, the La-Fe/NC showed the highest ORR catalytic activity, with a half-wave potential (E1/2) of 0.879 V (vs. RHE, Pt/C 0.845 V). After 5000 cycles, the E1/2 of the La-Fe/NC catalyst only decreased by 7 mV, and its performance in stability tests and methanol tolerance tests was superior to Pt/C. When used as the air electrode in a Zn-air battery, the La-Fe/NC catalyst demonstrated an excellent specific capacity of 755 mAh/g and a peak power density of 179.8 mW/cm2. The results provide important insights for the development of high-performance Zn-air batteries and new directions for the design of ORR catalysts.
Designing highly active electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution and reduction reactions (OER and ORR) is pivotal to renewable energy technology. Herein, based on density functional theory (DFT) calculations, we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks (COF) monolayers with axially coordinated ligands (denotes as FeN4-X@COF, X refers to axial ligand, X = -SCN, -I, -H, -SH, -NO2, -Br, -ClO, -Cl, -HCO3, -NO, -ClO2, -OH, -CN and -F). The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities. The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center, which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity. Importantly, FeN4-SH@COF and FeN4OH@COF are efficient bifunctional catalysts for HER and OER, FeN4OH@COF and FeN4-I@COF are promising bifunctional catalysts for OER and ORR. These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum iron-nitrogen-carbon based catalysts.
The metal ion batteries have gained widespread attention for wearable electronics due to their competitive energy density and long cycling life. Exploring the advanced anode materials is significant for next generation energy storage systems. However, severe electrode volume changes and sluggish redox kinetics are the critical problems for lithium/potassium ion batteries (LIBs/PIBs) towards large-scale applications. Herein, we prepare a novel anode material, which consists of reduced graphene oxide wrapping one-dimensional (1D) N-doped porous carbon nanotube with cobalt phosphoselenide (CoPSe) nanoparticles embedded inside them (rGO@CoPSe/NC). Benefited from the dual carbon decorations and ultrafine nanoparticles structure, it achieves a reversible capacity of 245 mAh/g at 5 A/g after 2000 cycles for LIBs and 215 mAh/g at 1 A/g after 500 cycles for PIBs. The pseudocapacitance and GITT measurements are used to investigate the electrochemical kinetics of rGO@CoPSe/NC for LIBs. In addition, the lithium ion full cell also shows good electrochemical performance when paired with high capacity LiNi0.8Co0.1Mn0.1O2 cathode. This work provides a feasible electrode design strategy for high-efficiency metal ion batteries based on multidimensional nanoarchitecture engineering and composition tailoring.
Pure near-infrared (NIR) phosphorescent materials with emission peak larger than 700 nm are of great significance for the development of optoelectronics and biomedicine. We have designed and synthesized two new B-embedded pure near-infrared (NIR)-emitting iridium complexes (Ir(Bpiq)2acac and Ir(Bpiq)2dpm) with peaks greater than 720 nm. More importantly, they exhibit very narrow phosphorescent emission with full width at half maximum (FWHM) of only about 50 nm (0.12 eV), resulting in a high NIR content (> 90%) in their spectrum. In view of better optical property and solubility, the complex Ir(Bpiq)2dpm was used as the emitting layer of a solution-processed OLED device, and achieved good maximum external quantum efficiency (EQE) (2.8%) peaking at 728 nm. This research provides an important strategy for the design of narrowband NIR-emitting phosphorescent iridium complexes and their optoelectronic applications.
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