Ammonia (NH) is regarded as an essential hydrogen storage material in the new energy field, and plasma-electrocatalytic synthesis of NH (PESA) is an alternative to the traditional Haber-Bosch process. Here, a bifunctional catalyst CoOOH/CF is proposed to enhance the PESA process. Benefiting from the efficient activation of O by CoOOH/CF, NO yield rate can reach the highest value of 171.
View Article and Find Full Text PDFLithium-air batteries (LABs) have aroused worldwide interest due to their high energy density as a promising next-generation battery technology. From a practical standpoint, one of the most pressing issues currently in LABs is their poor rate performance. Accelerating the mass transfer rate within LABs is a crucial aspect for enhancing their rate capability.
View Article and Find Full Text PDFLi-O batteries (LOBs) possess the highest theoretical gravimetric energy density among all types of secondary batteries, but they are still far from practical applications. The poor rate performance resulting from the slow mass transfer is one of the primary obstacles in LOBs. To solve this issue, a rotating cathode with periodic changes in the electrolyte layer thickness is designed, decoupling the maximum transfer rate of Li and O.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2024
Ambient electrochemical ammonia (NH ) synthesis is one promising alternative to the energy-intensive Haber-Bosch route. However, the industrial requirement for the electrochemical NH production with amperes current densities or gram-level NH yield remains a grand challenge. Herein, we report the high-rate NH production via NO reduction using the Cu activated Co electrode in a bipolar membrane (BPM) assemble electrolyser, wherein BPM maintains the ion balance and the liquid level of electrolyte.
View Article and Find Full Text PDFAmmonia (NH ) is essential for modern agriculture and industry, and, due to its high hydrogen density and no carbon emission, it is also expected to be the next-generation of "clean" energy carrier. Herein, directly from air and water, a plasma-electrocatalytic reaction system for NH production, which combines two steps of plasma-air-to-NO and electrochemical NO reduction reaction (eNO RR) with a bifunctional catalyst, is successfully established. Especially, the bifunctional catalyst of CuCo O /Ni can simultaneously promote plasma-air-to-NO and eNO RR processes.
View Article and Find Full Text PDFConstructing solid-state lithium-oxygen batteries (SSLOBs) holds a great promise to solve the safety and stability bottlenecks faced by lithium-oxygen batteries (LOBs) with volatile and flammable organic liquid electrolytes. However, the realization of high-performance SSLOBs is full of challenges due to the poor ionic conductivity of solid electrolytes, large interfacial resistance, and limited reaction sites of cathodes. Here, a flexible integrated cathode-electrolyte structure (ICES) is designed to enable the tight connection between the cathode and electrolyte through supporting them on a 3D SiO nanofibers (NFs) framework.
View Article and Find Full Text PDFThe lithium-oxygen battery (LOB) with a high theoretical energy density (∼3500 Wh kg) has been regarded as a strong competitor for next-generation energy storage systems. However, its performance is still far from satisfactory due to the lack of stable electrolyte that can simultaneously withstand the strong oxidizing environment during battery operation, evaporation by the semiopen feature, and high reactivity of lithium metal anode. Here, we have developed a deep eutectic electrolyte (DEE) that can fulfill all the requirements to enable the long-term operation of LOBs by just simply mixing solid -methylacetamide (NMA) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) at a certain ratio.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2022
The severe performance degradation of high-capacity Li-O batteries induced by Li dendrite growth and concentration polarization from the low Li transfer number of conventional electrolytes hinder their practical applications. Herein, lithiated Nafion (LN) with the sulfonic group immobilized on the perfluorinated backbone has been designed as a soluble lithium salt for preparing a less flammable polyelectrolyte solution, which not only simultaneously achieves a high Li transfer number (0.84) and conductivity (2.
View Article and Find Full Text PDFFormic acid (HCOOH) is one of the most promising chemical fuels that can be produced through CO electroreduction. However, most of the catalysts for CO electroreduction to HCOOH in aqueous solution often suffer from low current density and limited production rate. Herein, we provide a bismuth/cerium oxide (Bi/CeO ) catalyst, which exhibits not only high current density (149 mA cm ), but also unprecedented production rate (2600 μmol h cm ) with high Faradaic efficiency (FE, 92 %) for HCOOH generation in aqueous media.
View Article and Find Full Text PDFThe dendrite growth of Li anodes severely degrades the performance of lithium-oxygen (Li-O) batteries. Recently, hybrid solid electrolyte (HSE) has been regarded as one of the most promising routes to tackle this problem. However, before this is realized, the HSE needs to simultaneously satisfy contradictory requirements of high modulus and even, flexible contact with Li anode, while ensuring uniform Li distribution.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2019
The flexible Li-O battery is suitable to satisfy the requirements of a self-powered energy system, thanks to environmental friendliness, low cost, and high theoretical energy density. Herein, a flexible porous bifunctional electrode with both electrocatalytic and photocatalytic activity was synthesized and introduced as a cathode to assemble a high-performance Li-O battery that achieved an overpotential of 0.19 V by charging with the aid of solar energy.
View Article and Find Full Text PDFThe electrochemical N fixation, which is far from practical application in aqueous solution under ambient conditions, is extremely challenging and requires a rational design of electrocatalytic centers. We observed that bismuth (Bi) might be a promising candidate for this task because of its weak binding with H adatoms, which increases the selectivity and production rate. Furthermore, we successfully synthesized defect-rich Bi nanoplates as an efficient noble-metal-free N reduction electrocatalyst via a low-temperature plasma bombardment approach.
View Article and Find Full Text PDFEfficient and selective dehydrogenation of formic acid is a key challenge for a fuel-cell-based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear.
View Article and Find Full Text PDFRechargeable aprotic alkali metal (Li or Na)-O batteries are the subject of great interest because of their high theoretical specific energy. However, the growth of dendrites and cracks at the Li or Na anode, as well as their corrosive oxidation lead to poor cycling stability and safety issues. Understanding the mechanism and improving Li/Na-ion plating and stripping electrochemistry are therefore essential to realizing their technological potential.
View Article and Find Full Text PDFTo promote the development of high energy Li-O batteries, it is important to design and construct a suitable and effective oxygen-breathing cathode. Herein, activated cobalt-nitrogen-doped carbon nanotube/carbon nanofiber composites (Co-N-CNT/CNF) as the effective cathodes for Li-O batteries are prepared by in situ chemical vapor deposition (CVD). The unique architecture of these electrodes facilitates the rapid oxygen diffusion and electrolyte penetration.
View Article and Find Full Text PDFLarge-scale application of renewable energy and rapid development of electric vehicles have brought unprecedented demand for advanced energy-storage/conversion technologies and equipment. Rechargeable zinc (Zn)-air batteries represent one of the most promising candidates because of their high energy density, safety, environmental friendliness, and low cost. The air electrode plays a key role in managing the many complex physical and chemical processes occurring on it to achieve high performance of Zn-air batteries.
View Article and Find Full Text PDFConversion of carbon dioxide (CO ) into valuable chemicals, especially liquid fuels, through electrochemical reduction driven by sustainable energy sources, is a promising way to get rid of dependence on fossil fuels, wherein developing of highly efficient catalyst is still of paramount importance. In this study, as a proof-of-concept experiment, first a facile while very effective protocol is proposed to synthesize amorphous Cu NPs. Unexpectedly, superior electrochemical performances, including high catalytic activity and selectivity of CO reduction to liquid fuels are achieved, that is, a total Faradaic efficiency of liquid fuels can sum up to the maximum value of 59% at -1.
View Article and Find Full Text PDFHydrogen is widely considered to be a sustainable and clean energy alternative to the use of fossil fuels in the future. Its high hydrogen content, nontoxicity, and liquid state at room temperature make formic acid a promising hydrogen carrier. Designing highly efficient and low-cost heterogeneous catalysts is a major challenge for realizing the practical application of formic acid in the fuel-cell-based hydrogen economy.
View Article and Find Full Text PDFTo meet the increasing demands for portable and flexible devices in a rapidly developing society, it is urgently required to develop highly safe and flexible electrochemical energy-storage systems. Flexible lithium-oxygen batteries with high theoretical specific energy density are promising candidates; however, the conventional half-open structure design prevents it from working properly under water or fire conditions. Herein, as a proof-of-concept experiment, a highly safe flexible lithium-oxygen battery achieved by the synergy of a vital multifunctional structure design and a unique composite separator is proposed and fabricated.
View Article and Find Full Text PDFAmmonia synthesis is one of the most kinetically complex and energetically challenging chemical processes in industry and has used the Harber-Bosch catalyst for over a century, which is processed under both harsh pressure (150-350 atm) and hightemperature (623-823 K), wherein the energy and capital intensive Harber-Bosch process has a huge energy cost accounting for about 1%-3% of human's energy consumption. Therefore, there has been a rough and vigorous exploration to find an environmentally benign alternative process. As the amorphous material is in a metastable state and has many "dangling bonds", it is more active than the crystallized one.
View Article and Find Full Text PDFWith the development of renewable energy and electrified transportation, electrochemical energy storage will be more urgent in the future. Supercapacitors have received extensive attention due to their high power density, fast charge and discharge rates, and long-term cycling stability. During past five years, supercapacitors have been boomed benefited from the development of nanostructured materials synthesis and the promoted innovation of devices construction.
View Article and Find Full Text PDFTo recycle rusty stainless-steel meshes (RSSM) and meet the urgent requirement of developing high-performance cathodes for potassium-ion batteries (KIB), we demonstrate a new strategy to fabricate flexible binder-free KIB electrodes via transformation of the corrosion layer of RSSM into compact stack-layers of Prussian blue (PB) nanocubes (PB@SSM). When further coated with reduced graphite oxide (RGO) to enhance electric conductivity and structural stability, the low-cost, stable, and binder-free RGO@PB@SSM cathode exhibits excellent electrochemical performances for KIB, including high capacity (96.8 mAh g ), high discharge voltage (3.
View Article and Find Full Text PDFTo achieve a high reversibility and long cycle life for Li-O battery system, the stable tissue-directed/reinforced bifunctional separator/protection film (TBF) is in situ fabricated on the surface of metallic lithium anode. It is shown that a Li-O cell composed of the TBF-modified lithium anodes exhibits an excellent anodic reversibility (300 cycles) and effectively improved cathodic long lifetime (106 cycles). The improvement is attributed to the ability of the TBF, which has chemical, electrochemical, and mechanical stability, to effectively prevent direct contact between the surface of the lithium anode and the highly reactive reduced oxygen species (Li O or its intermediate LiO ) in cell.
View Article and Find Full Text PDFAs the NN bond in N is one of the strongest bonds in chemistry, the fixation of N to ammonia is a kinetically complex and energetically challenging reaction and, up to now, its synthesis is still heavily relying on energy and capital intensive Haber-Bosch process (150-350 atm, 350-550 °C), wherein the input of H and energy are largely derived from fossil fuels and thus result in large amount of CO emission. In this paper, it is demonstrated that by using Au sub-nanoclusters (≈0.5 nm ) embedded on TiO (Au loading is 1.
View Article and Find Full Text PDFTo turn waste into treasure, a facile and cost-effective strategy is developed to revive electroless nickel plating wastewater and cotton-textile waste toward a novel electrode substrate. Based on the substrate, a binder-free PB@GO@NTC electrode is obtained, which exhibits superior electrochemical performance. Moreover, for the first time, a novel tube-type flexible and wearable sodium-ion battery is successfully fabricated.
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