The carbon-free electrocatalytic nitrogen reduction reaction (NRR) is an alternative technology to the current Haber-Bosch method, that can be conducted under ambient conditions, and directly converting water and nitrogen (N₂) into ammonia (NH₃). However, the limited activity and selectivity of NH₃ electrosynthesis hinder the practical applications of NRR. In this study, we present a novel type of electrocatalyst called boridene nanosheets enriched with metal vacancies that are specifically designed for efficient electrocatalytic NRR under ambient conditions.
View Article and Find Full Text PDFThe adhesion of H bubbles on the electrode surface is one of the main factors limiting the performance of H evolution of electrolytic water, especially at high current density. To overcome this problem, here a "quasi-gas phase" electrolytic water reaction system based on capillary effect is proposed for the first time to improve the mass transfer efficiency of H. The typical feature of this reaction system is that the main site of H evolution reaction is transferred from the bulk aqueous solution to the gas phase environment above the bulk aqueous solution, thus effectively inhibiting the aggregation of H bubbles and reducing the resistance of their diffusion away.
View Article and Find Full Text PDFAn ultra-thin quasi-solid electrolyte (QSE) with dendrite-inhibiting properties is a requirement for achieving high energy density quasi-solid lithium metal batteries (LMBs). Here, a 5.1 µm rigid QSE layer is directly designed on the cathode, in which Kevlar (poly(p-phenylene terephthalate)) nanofibers (KANFs) with negatively charged groups bridging metal-organic framework (MOF) particles are served as a rigid skeleton, and non-flammable deep eutectic solvent is selected to be encapsulated into the MOF channels, combined with in situ polymerization to complete safe electrolyte system with high rigidness and stability.
View Article and Find Full Text PDFRenewable photo-/electrocatalytic coreduction of CO and nitrate to urea is a promising method for high-value utilization of CO . However, because of the low yields of the urea synthesis by photo-/electrocatalysis process, the accurate quantification of low concentration urea is challenging. The traditional diacetylmonoxime-thiosemicarbazide (DAMO-TSC) method for urea detection has a high limit of quantification and accuracy, but it is easily affected by NO in the solution, which limits its application scope.
View Article and Find Full Text PDFRedox flow batteries have been discussed as scalable and simple stationary energy storage devices. However, currently developed systems encounter less competitive energy density and high costs, restricting their wider application. There is a lack of appropriate redox chemistry, preferably based on active materials that are abundant in nature and show high solubility in aqueous electrolytes.
View Article and Find Full Text PDFElectrocatalytic N reduction reaction (NRR) is recognized as a zero-carbon emission method for NH synthesis. However, to date, this technology still suffers from low yield and low selectivity associated with the catalyst. Herein, inspired by the activation of N by lithium metal, a highly reactive defective black phosphorene (D-BP ) is proposed as a lithium-like catalyst for boosting electrochemical N activation.
View Article and Find Full Text PDFThe aqueous electrocatalytic reduction of NO into NH (NitrRR) presents a sustainable route applicable to NH production and potentially energy storage. However, the NitrRR involves a directly eight-electron transfer process generally required a large overpotential (<-0.2 V versus reversible hydrogen electrode (vs.
View Article and Find Full Text PDFCorrection for 'Super-large dendrites composed of trigonal PbO2 nanoplates with enhanced performances for electrochemical devices' by Liang-Xin Ding et al., Chem. Commun.
View Article and Find Full Text PDFCorrection for 'Cu2O template synthesis of high-performance PtCu alloy yolk-shell cube catalysts for direct methanol fuel cells' by Sheng-Hua Ye et al., Chem. Commun.
View Article and Find Full Text PDFWe demonstrate a simple and effective chemical equilibrium regulation strategy to improve the efficiency of electrochemical ammonia synthesis by constructing electrochemical reaction system that works at significantly lower pressure than the Haber-Bosch process. Transferring the nitrogen reduction reaction from ambient conditions to a lightly pressurized environment not only accelerates the activation of the N≡N triple bond but also inhibits the competing reaction of hydrogen evolution while promoting the dissolution and diffusion of nitrogen. The verification experiment of using well-designed Fe Mo C/C composite nanosheets as the nitrogen reduction catalyst shows that the lower pressure reaction system can improve the Faradaic current efficiency by one order of magnitude.
View Article and Find Full Text PDFThe electrochemical reduction of nitrogen into ammonia under ambient conditions is a potential strategy for sustainable ammonia production. At present, one of the main research directions in the field of electrochemical nitrogen fixation is to improve the current efficiency and ammonia yield by developing efficient nitrogen reduction catalysts. To optimise the selectivity and catalytic activity of nitrogen reduction catalysts more efficiently, herein, we systematically summarise the progress of research on nitrogen reduction catalysts in recent years and present some general catalyst design strategies.
View Article and Find Full Text PDFConstructing efficient catalysts for the N reduction reaction (NRR) is a major challenge for artificial nitrogen fixation under ambient conditions. Herein, inspired by the principle of "like dissolves like", it is demonstrated that a member of the nitrogen family, well-exfoliated few-layer black phosphorus nanosheets (FL-BP NSs), can be used as an efficient nonmetallic catalyst for electrochemical nitrogen reduction. The catalyst can achieve a high ammonia yield of 31.
View Article and Find Full Text PDFMetal-organic framework (MOF) membranes show great promise for propene/propane separation, yet a sharp molecular sieving has not been achieved due to their inherent linker mobility. Here, zeolitic imidazolate framework ZIF-8-type membranes with suppressed linker mobility are prepared by a fast current-driven synthesis (FCDS) strategy within 20 min, showing sharpened molecular sieving for propene/propane separation with a separation factor above 300. During membrane synthesis, the direct current promotes the metal ions and ligands to assemble into inborn-distorted and stiffer frameworks with ZIF-8_Cm (a newly discovered polymorph of ZIF-8) accounting for 60 to 70% of the membrane composition.
View Article and Find Full Text PDFElectrocatalytic nitrogen fixation is considered a promising approach to achieve NH production. However, due to the chemical inertness of nitrogen, it is necessary to develop efficient catalysts to facilitate the process of nitrogen reduction. Here, molybdenum carbide nanodots embedded in ultrathin carbon nanosheets (Mo C/C) are developed to serve as a catalyst candidate for highly efficient and robust N fixation through an electrocatalytic nitrogen reduction reaction (NRR).
View Article and Find Full Text PDFSeparator modification has been proved to be an effective approach for overcoming lithium polysulfide (LiPS) shuttling in lithium-sulfur (Li-S) cells. However, the weight and stability of the modified layer also affect the cycling properties and the energy density of Li-S cells. Here, we initially construct an ultrathin and lightweight MnO layer (380 nm, 0.
View Article and Find Full Text PDFMolecular sieving membranes with sufficient and uniform nanochannels that break the permeability-selectivity trade-off are desirable for energy-efficient gas separation, and the arising two-dimensional (2D) materials provide new routes for membrane development. However, for 2D lamellar membranes, disordered interlayer nanochannels for mass transport are usually formed between randomly stacked neighboring nanosheets, which is obstructive for highly efficient separation. Therefore, manufacturing lamellar membranes with highly ordered nanochannel structures for fast and precise molecular sieving is still challenging.
View Article and Find Full Text PDFWe report the discovery of a dramatically enhanced N electroreduction reaction (NRR) selectivity under ambient conditions via the Li incorporation into poly(N-ethyl-benzene-1,2,4,5-tetracarboxylic diimide) (PEBCD) as a catalyst. The detailed electrochemical evaluation and density functional theory calculations showed that Li association with the O atoms in the PEBCD matrix can retard the HER process and can facilitate the adsorption of N to afford a high potential scope for the NRR process to proceed in the "[O-Li]·N-H" alternating hydrogenation mode. This atomic-scale incorporation strategy provides new insight into the rational design of NRR catalysts with higher selectivity.
View Article and Find Full Text PDFFreestanding three-dimensional nitrogen-doped carbon foam with large pores is proposed as a promising electrode configuration for elastic electronics. Although it exhibits excellent mechanical performance, the capacitive performances (especially its rate capability) are still unsatisfactory. By using KMnO, we demonstrate a smart etching and catalytic process to form highly graphitized and etched nitrogen-doped carbon foam (ENCF) with an exfoliated carbon-shell architecture.
View Article and Find Full Text PDFInhibiting CO formation can more directly address the problem of CO poisoning during methanol electro-oxidation. In this study, 1D self-supported porous PtAuP alloy nanotube arrays (ANTAs) are synthesized via a facile electro-codeposition approach and present enhanced activity and improved resistance to CO poisoning through inhibiting CO formation (non-CO pathway) during the methanol oxidation reaction in acidic medium. This well-controlled Pt-/transition metal-/nonmetal ternary nanostructure exhibits a specific electroactivity twice as great as that of PtAu alloy nanotube arrays and Pt/C.
View Article and Find Full Text PDFFreestanding and highly compressible nitrogen-doped carbon foam (NCF) with excellent hydrophilicity and good electrochemical properties is prepared. Based on NCF electrodes, a high-performance all solid-state symmetric supercapacitor device is fabricated with native, full compressibility, and excellent mechanical stability, addressing two major problems in the current technology.
View Article and Find Full Text PDFThe catalytic activity and durability are crucial for the development of high-performance electrocatalysts. To design electrocatalysts with excellent electroactivity and durability, the structure and composition are two important guiding principles. In this work, novel Pt/Ni(OH)-NiOOH/Pd multi-walled hollow nanorod arrays (MHNRAs) are successfully synthesized.
View Article and Find Full Text PDFHybrid electrocatalysts with excellent electrocatalytic activity for hydrogen reduction are fabricated using an efficient and facile electrochemical route. The electronic and synergistic effects between Co(OH)2 and polyaniline (PANI) in the composite structure are the key factors that generate the high electrocatalytic activity and excellent stability. A highly efficient, non-precious metal-based flexible electrocatalyst for high-performance electrocatalysts is shown, which reveals a novel route for the design and synthesis of electrocatalysts.
View Article and Find Full Text PDFPerovskites show excellent specific catalytic activity toward both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in alkaline solutions; however, small surface areas of the perovskites synthesized by traditional sol-gel methods lead to low utilization of catalytic sites, which gives rise to poor Li-O2 batteries performance and restricts their application. Herein, a hierarchical mesporous/macroporous perovskite La0.5Sr0.
View Article and Find Full Text PDFNitrogen-doped bamboo-like carbon nanotubes (N-BCNTs) were synthesised using a facile one-step pyrolysis process. Due to their unique one-dimensional hollow structure and intrinsic high nitrogen content, N-BCNTs exhibit high capacity, superior rate capability, and excellent cycle stability and are, thus, promising anode materials for sodium-ion batteries.
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