Synchronously Producing H2 and Purifying Methyl Orange-Polluted Water through the Reaction of an Al-GaInSn Alloy Plate and H2O.

Hydrogen gas (H2) as a fuel has the advantages of high energy density (122 kJ g-1) and zero carbon emissions. To meet the growing demand for H2 in the future, green, efficient, and convenient production technologies must be developed. The Al-H2O reaction, which produces H2 by reacting aluminum (Al) with water (H2O), is considered a rapid method for producing H2. However, Al-H2O creates a protective oxide layer on the surface of Al, preventing the production of H2. In this study, we developed a simple method for forming Al-GaInSn alloy by brushing GaInSn-Al2O3 grease onto an Al plate to form an Al/GaInSn-Al2O3/Al sandwich structure. Al2O3 in the sample supports GaInSn, prevents the leakage of GaInSn, and promotes its penetration into the Al lattice to form Al-GaInSn alloy. By forming a liquid phase within the alloy, GaInSn increases the accessibility of Al to the reaction. As a result, the Al-GaInSn alloy can rapidly react with pure H2O to produce H2 at room temperature conditions, with yields as high as ∼93.2%. It was interesting to find that dye-polluted water (methyl orange) could be synchronically purified by the Al-H2O reaction at the same time.

Enhanced Adsorption of Aromatic Volatile Organic Compounds on a Perchloro Covalent Triazine Framework through Multiple Intermolecular Interactions.

Volatile organic compounds (VOCs) may have short- and long-term adverse health effects. Especially, aromatic VOCs including benzene, toluene, ethylbenzene, and xylene (BTEX) are important indoor air pollutants. Developing highly efficient porous adsorbents with broad applicability remains a major challenge. In this study, a perchlorinated covalent-triazine framework (ClCTF-1-400) is prepared for adsorbing BTEX. ClCTF-1-400 is confirmed as a partially oxidized/chlorinated microporous covalent triazine framework through a variety of characterization. It is found that ClCTF-1-400 is reversible VOCs absorbent with very high absorption capacities, which can adsorb benzene (693 mg g-1 ), toluene (621 mg g-1 ), ethylbenzene (603 mg g-1 ), o-xylene (500 mg g-1 ), m-xylene (538 mg g-1 ), and p-xylene (592 mg g-1 ) at 25 °C and their saturated vapor pressure (≈ 1 kPa). ClCTF-1-400 is of higher adsorption capacities for all selected VOCs than activated carbon and other reported adsorbents. The adsorption mechanism is also inferred through theoretical calculation and in-site Fourier Transform Infrared (FTIR) spectroscopy. The observed excellent BTEX adsorption performance is attributed to the multiple weak interactions between the ClCTF-1-400 frameworks and aromatic molecules through multiple weak interactions (CH… π and CCl… π). The breakthrough experiment demonstrates ClCTF-1-400 has the potential for real VOCs pollutant removal in air.

Atomic understanding of the strain-induced electrocatalysis from DFT calculation: progress and perspective.

Catalyst activity affects the reaction rate, and an increasing number of studies have shown that strain can significantly increase the electrocatalytic activity. Catalysts such as alloys and core-shell structures can modulate their properties through strain effects. Reasonable simulation techniques can be used to predict and design the catalytic performance based on understanding the strain action mechanism. Therefore, the methodological flow of theoretical simulations is summarised in this review. The mechanism underlying the strain-adsorption-reaction relationship is discussed using density functional theory (DFT) calculations. An introduction to DFT is given first, followed by a quick rundown of the strain classification and application. Typical electrocatalytic reactions, namely, the hydrogen and oxygen evolution reactions and oxygen reduction reaction, are taken as examples. After briefly explaining these reactions, the relevant studies on simulating the strain to tune the catalyst performance are covered. The simulation methods are summarised and analysed to observe the effects of strain on electrocatalytic properties. Finally, a summary of the issues with simulated strain-assisted design and a discussion on the perspectives and forecasts for the future design of effective catalysts are provided.

Multifunctional Photothermal Phase-Change Superhydrophobic Film with Excellent Light-Thermal Conversion and Thermal-Energy Storage Capability for Anti-icing/De-icing Applications.

The accumulation of ice may cause serious safety problems in numerous fields. A photothermal superhydrophobic surface is considered to be useful for preventing ice formation because of its environmentally friendly, energy-saving, and excellent anti-icing/de-icing properties. However, it easily fails to work in the absence of sunlight. To improve its anti-icing property without sunlight irradiation, a multifunctional photothermal phase-change superhydrophobic film (MPPSF) consisting of phase-change microcapsules (PCMs) and carbon nanotubes (CNTs) was fabricated using a facile spraying method. Benefitting from the excellent light-thermal conversion effect of CNTs, the surface temperature could increase from -20 to 130.1 °C within 180 s under 808 nm near-infrared laser irradiation of 1 W/cm2, thus realizing high-efficiency de-icing. Meanwhile, a portion of the light-thermal energy was stored in the MPPSF because of the phase change of the PCMs. Without sunlight irradiation, the latent heat of the PCMs was released when the external temperature approached the phase-transition temperature. The synergistic effects of the phase-transition latent heat release and superhydrophobicity allowed the MPPSF to effectively hinder the formation of ice for 10.1 min at -20 °C. Therefore, this MPPSF with outstanding anti-icing and de-icing performances is expected to achieve ice prevention and removal in all-days.

The Features and Progress of Electrolyte for Potassium Ion Batteries.

Nowadays, Li-ion batteries have achieved great success and are widely used in various fields. However, the scarcity and uneven distribution of lithium resources together with the increasing cost may hamper the sustainable development of Li-ion batteries in the future. Hence, many researchers have turned to potassium ion batteries due to their abundant raw materials, low price, and high energy density. Although great progress has been made in recent years, there are still existing many challenges, especially the severe side reaction between electrolyte and K metal, which leads to an unstable solid-liquid interface and low coulombic efficiency. Hence, an excellent electrolyte may be the key to development of K-ion batteries in the future. Unfortunately, no systematic research has been conducted to study the electrolyte and its role on the performance yet. In order to compensate for this limitation, in this paper, the status and progress of electrolytes for K-ion batteries are reviewed, the issues and challenges existing in the development of electrolyte are clarified, and the future development is prospected.

Multifunctional Polypropylene Separator via Cooperative Modification and Its Application in the Lithium-Sulfur Battery.

The continuous shuttling of dissolved polysulfides between the electrodes is the primary cause for the rapid decay of lithium-sulfur batteries. Modulation of the separator-electrolyte interface through separator modification is a promising strategy to inhibit polysulfide shuttling. In this work, we develop a graphene oxide and ferrocene comodified polypropylene separator with multifunctionality at the separator-electrolyte interface. The graphene oxide on the functionalized separator could physically adsorb the polysulfide while the ferrocene component could effectively facilitate the conversion of the adsorbed polysulfide. Due to the combination of these beneficial functionalities, the separator exhibits an excellent battery performance, with a high reversible capacity of 409 mAh g-1 after 500 cycles at 0.2 C. We anticipate that the combinatorial separator functionalization proposed herein is an effective approach for improving the performance of lithium-sulfur batteries.

A Simple Mechanical Method to Modulate the Electrochemical Electrosorption Processes at Metal Surfaces.

The coupling of electrochemical processes and surface strain has been widely investigated in the past. The present work briefly introduces a simple method to modulate the electrochemical process at metal surfaces by mechanical bending. In this way, the static strain at the metal layer can reach the order of 1%. The cyclic voltammogram was used to study the electrosorption process of oxygen species at sputtered metal surfaces under different strain states. The experimental results show that the desorption peak potential of oxygen at the Au surface shifted positively by tensile strain, whereas the desorption peak potential at the Pt surface shifted negatively. This phenomenon indicates that tensile strain has an opposite effect on the electrosorption process for Au and Pt surfaces. Our results agree with the previous reports on the potential variation induced by dynamic strain. This work thus offers a simple method to modulate the electrosorption process at metal surfaces and then to enhance the reactivity of metal electrodes.

Improvement of Hydrogen Desorption Characteristics of MgH2 With Core-shell Ni@C Composites.

Magnesium hydride (MgH2) has become popular to study in hydrogen storage materials research due to its high theoretical capacity and low cost. However, the high hydrogen desorption temperature and enthalpy as well as the depressed kinetics, have severely blocked its actual utilizations. Hence, our work introduced Ni@C materials with a core-shell structure to synthesize MgH2-x wt.% Ni@C composites for improving the hydrogen desorption characteristics. The influences of the Ni@C addition on the hydrogen desorption performances and micro-structure of MgH2 have been well investigated. The addition of Ni@C can effectively improve the dehydrogenation kinetics. It is interesting found that: i) the hydrogen desorption kinetics of MgH2 were enhanced with the increased Ni@C additive amount; and ii) the dehydrogenation amount decreased with a rather larger Ni@C additive amount. The additive amount of 4 wt.% Ni@C has been chosen in this study for a balance of kinetics and amount. The MgH2-4 wt.% Ni@C composites release 5.9 wt.% of hydrogen in 5 min and 6.6 wt.% of hydrogen in 20 min. It reflects that the enhanced hydrogen desorption is much faster than the pure MgH2 materials (0.3 wt.% hydrogen in 20 min). More significantly, the activation energy (EA) of the MgH2-4 wt.% Ni@C composites is 112 kJ mol-1, implying excellent dehydrogenation kinetics.

The effect of an external magnetic field on the dealloying process of the Ni-Al alloy in alkaline solution.

Our work investigates the effect of an external magnetic field on different dealloying stages of the formation of a nanoporous magnetic material. The magnetic field first prolongs the Ni rearrangement process at a low magnetic flux density, whereas the trend is reversed and the Ni rearrangement process is shortened at a higher magnetic flux density. The much finer morphology of nanoporous Ni can be prepared by adjusting the external magnetic flux density.

Electrocapillary coupling at rough surfaces.

We investigate the impact of the surface roughness on the experimental value of the electrocapillary coupling coefficient, ς. This quantity relates the response of electrode potential, E, to tangential elastic strain, e, and also measures the variation of the surface stress, f, with the superficial charge density, q. We combine experiments measuring the apparent coupling coefficient ςeff for gold thin film electrodes in weakly adsorbing electrolyte with data for the surface roughness determined by atomic force microscopy and by the capacitance ratio method. We find that even moderate roughness has a strong impact on the value of ςeff. Analyzing the mechanics of corrugated surfaces affords a correction scheme yielding values of ς that are invariant with roughness and that agree with expectations for the true coupling coefficient on ideal, planar surfaces. The correction is simple and readily applied to experiments measuring ςeff from surface stress changes in cantilever bending studies or from the potential variation in dynamic electro-chemo-mechanical analysis.

Less Noble or More Noble: How Strain Affects the Binding of Oxygen on Gold.

Many heterogeneous catalysts exploit strained active layers to modulate reactivity and/or selectivity. It is therefore significant that density functional theory, as well as experimental approaches, find that tensile strain makes the gold surface more binding for oxygen, in other words, less noble. We show that this behavior does not apply when re-structuring of the gold surface is allowed to occur simultaneously with the adsorption of oxygen. In situ cantilever-bending studies show the surface stress to increase when oxygen species adsorb on a (111)-textured gold surface in aqueous H2 SO4 . This implies a positive sign of the electrocapillary coupling parameter and, hence, a trend for weaker oxygen binding in response to tensile strain. These conflicting findings indicate that different electrosorption processes, and specifically oxygen species adsorption on the bulk-terminated surface, exhibit fundamentally different coupling between the chemistry and the mechanics of the surface.

Electrocapillary coupling during electrosorption.

The electrocapillary coupling coefficient, ς, measures the response of the electrode potential, E, to tangential elastic strain at the surface of an electrode. Using dynamic electro-chemo-mechanical analysis, we study ς(E) simultaneously with cyclic voltammetry. The study covers extended potential intervals on Au, Pt, and Pd, including the electrosorption of oxygen species and of hydrogen. The magnitude and sign of ς vary during the scans, and quite generally the graphs of ς(E) emphasize details which are less obvious or missing in the cyclic voltammograms (CVs). Capacitive processes on the clean electrode surfaces exhibit ς < 0, whereas capacitive processes on oxygen-covered surfaces are characterized by ς < 0 on Au but ς > 0 on Pt and Pd. The findings of ς < 0 during the initial stages of oxygen species adsorption and ς > 0 for hydrogen electrosorption agree with the trend that tensile strain makes surfaces more binding for adsorbates. However, the large hysteresis of oxygen electrosorption on all electrodes raises the question: is the exchange current associated with that process sufficient for its measurement by potential response during small cyclic strain?

Ultrasound-Assisted Preparation and Performance Regulation of Electrocatalytic Materials.

With the advancement of scientific research, the introduction of external physical methods not only adds extra freedom to the design of electro-catalytical processes for green technologies but also effectively improves the reactivity of materials. Physical methods can adjust the intrinsic activity of materials and modulate the local environment at the solid-liquid interface. In particular, this approach holds great promise in the field of electrocatalysis. Among them, the ultrasonic waves have shown reasonable control over the preparation of materials and the electrocatalytic process. However, the research on coupling ultrasonic waves and electrocatalysis is still early. The understanding of their mechanisms needs to be more comprehensive and deep enough. Firstly, this article extensively discusses the adhibition of the ultrasonic-assisted preparation of metal-based catalysts and their catalytic performance as electrocatalysts. The obtained metal-based catalysts exhibit improved electrocatalytic performances due to their high surface area and more exposed active sites. Additionally, this article also points out some urgent unresolved issues in the synthesis of materials using ultrasonic waves and the regulation of electrocatalytic performance. Lastly, the challenges and opportunities in this field are discussed, providing new insights for improving the catalytic performance of transition metal-based electrocatalysts.

Controllable synthesis of a hybrid mesoporous sheets-like Fe0.5NiS2@ P, N-doped carbon electrocatalyst for alkaline oxygen evolution reaction.

Owing to the high cost of precious metal catalysts for the oxygen evolution reaction (OER), the production of highly efficient and affordable electrocatalysts is important for generating pollution-free and renewable energy via electrochemical processes. A facile hydrothermal approach was employed to synthesize hybrid mesoporous iron-nickel bimetallic sulfides @ P, N-doped carbon for the OER. The prepared Fe0.5NiS2@C exhibited an overpotential (η) of 250 mV at 10 mA/cm2. This exceeded the overpotentials recently reported for surface-modified P, N-doped carbon-based catalysts for the OER in a 1 M KOH medium. Moreover, the Fe0.5NiS2@C catalyst showed a notable Tafel slope of 90.5 mV/dec with long-dated stability even after 24 h at 10 mA/cm2. The superior OER performance of the Fe0.5NiS2@C catalysts may be due to their large surface area, sheet-like morphology with abundant active sites, fast transfer of mass and electrons, control of the electronic structure by co-treatment with heteroatoms (e.g., P and N), and the synergistic effect of bimetallic sulfides, making them favorable catalysts for the oxygen evolution reaction. Density functional theory (DFT) calculations showed that the Fe0.5NiS2@C catalyst exhibited strong H2O-adsorption energy. The enhanced OER activity of Fe0.5NiS2@C was attributed to its higher surface area, favorable H2O adsorption energy, improved electron transfer efficiency, and lower Gibbs free energy compared to those of the other proposed catalysts.

Core-shell NiS2@C encased by thin carbon layer as high-rate and durable electrode for aqueous rechargeable battery.

Nickel sulfides, as promising candidate for aqueous rechargeable battery, have aroused broad attention on account of abundant natural resources, rich phases, moderate price and high theoretical capacity. Nevertheless, tremendous volume expansion during repeated charging-discharging procedure leads to the poor rate capability and cycling stability of nickel sulfide electrodes. Therefore, in this work, core-shell NiS2@C encapsulated by thin hydrothermal carbon (HC) layer (NiS2@C/HC) has been designed and prepared without any surfactants or templates assistance, which avoid tedious process and shorten preparation cycle greatly. When matched with the treated iron powder (TIP) electrode to form NiS2@C/HC//TIP aqueous rechargeable battery, the NiS2@C/HC//TIP battery exhibits a high discharge capacity of 205.1 mAh g-1 at 1 A g-1, remarkable rate ability (176.4 mAh g-1 at 5 A g-1, about 86% capacity conversation) and superiorly durable stability (80.8 % capacity retention after 10,000 cycles at ultra-high current density of 15 A g-1). The outstanding high-rate capability and cycling stability for aqueous rechargeable battery can be ascribed to the distinct cowpea-like architecture and intrinsic properties of NiS2@C/HC. Specifically, the interior porous carbon provides a space to tolerate the volume expansion of the NiS2 nanoparticles and prevent NiS2 nanoparticles from aggregation, guaranteeing its high-rate capability. Meanwhile, the exterior HC layer is conducive to improve the electric conductivity to facilitate the electrons transfer and promote the mechanical strength of the whole active materials, ensuring its robust cycling stability.

Progress and Perspective of Glass-Ceramic Solid-State Electrolytes for Lithium Batteries.

The all-solid-state lithium battery (ASSLIB) is one of the key points of future lithium battery technology development. Because solid-state electrolytes (SSEs) have higher safety performance than liquid electrolytes, and they can promote the application of Li-metal anodes to endow batteries with higher energy density. Glass-ceramic SSEs with excellent ionic conductivity and mechanical strength are one of the main focuses of SSE research. In this review paper, we discuss recent advances in the synthesis and characterization of glass-ceramic SSEs. Additionally, some discussions on the interface problems commonly found in glass-ceramic SSEs and their solutions are provided. At the end of this review, some drawbacks of glass-ceramic SSEs are summarized, and future development directions are prospected. We hope that this review paper can help the development of glass-ceramic solid-state electrolytes.

MXene-based Materials for Water Splitting: Synthesis and Modification.

With abundant metal site and tunable electronic structure, MXene is considered as a promising electrocatalyst for the conversion of energy molecules. In this review, the latest research progress on inexpensive MXene-based catalysts for water electrolysis is summarized. Typical preparation and modification methods and their advantages and disadvantages are briefly discussed, with a focus on the regulation and design of the surface interface electronic states, which improve the electrocatalytic performance of MXene-based materials. The main strategies for the electronic state modification include end-group modification, heteroatom doping, and heterostructure construction. Some limitations of MXene-based materials, which should be considered in the rational design of advanced MXene-based electrocatalyst, are also discussed. Finally, prospects for the rational design of Mxene-based electrocatalysts is proposed.

Ultrasonic-assisted preparation of two-dimensional materials for electrocatalysts.

Developing green, environmental, sustainable new energy sources is an important problem to be solved in the world. Among the new energy technologies, water splitting system, fuel cell technology and metal-air battery technology are the main energy production and conversion methods, which involve three main electrocatalytic reactions, hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). The efficiency of the electrocatalytic reaction and the power consumption are very dependent on the activity of the electrocatalysts. Among various electrocatalysts, the two-dimensional (2D) materials have received widespread attention due to multiple advantages, such as their easy availability and low price. What' important is that they have adjustable physical and chemical properties. It is possible to develop them as electrocatalysts to replace the noble metals. Therefore, the design of two-dimensional electrocatalysts is a focus in the research area. Some recent advances in ultrasound-assisted preparation of two-dimensional (2D) materials have been overviewed according to the kind of materials in this review. Firstly, the effect of the ultrasonic cavitation and its applications in the synthesis of inorganic materials are introduced. The ultrasonic-assisted synthesis of representative 2D materials for example transition metal dichalcogenides (TMDs), graphene, layered double metal hydroxide (LDH), and MXene, and their catalytic properties as electrocatalysts are discussed in detail. For example, the CoMoS4 electrocatalysts have been synthesized through a facile ultrasound-assisted hydrothermal method. The obatined HER and OER overpotential of CoMoS4 electrode is 141 and 250 mV, respectively. This review points out some problems that need to be solved urgently at present, and provides some ideas for designing and constructing two-dimensional materials with better electrocatalytic performance.

Noble Metal-Based Catalysts with Core-Shell Structure for Oxygen Reduction Reaction: Progress and Prospective.

With the deterioration of the ecological environment and the depletion of fossil energy, fuel cells, representing a new generation of clean energy, have received widespread attention. This review summarized recent progress in noble metal-based core-shell catalysts for oxygen reduction reactions (ORRs) in proton exchange membrane fuel cells (PEMFCs). The novel testing methods, performance evaluation parameters and research methods of ORR were briefly introduced. The effects of the preparation method, temperature, kinds of doping elements and the number of shell layers on the ORR performances of noble metal-based core-shell catalysts were highlighted. The difficulties of mass production and the high cost of noble metal-based core-shell nanostructured ORR catalysts were also summarized. Thus, in order to promote the commercialization of noble metal-based core-shell catalysts, research directions and prospects on the further development of high performance ORR catalysts with simple synthesis and low cost are presented.

Electrocatalyst design for the conversion of energy molecules: electronic state modulation and mass transport regulation.

Electrocatalytic conversions of energy molecules are involved in many energy conversion processes. Improving the activity of electrocatalysts is critical for increasing the efficiency of these energy conversion processes. However, the tailored design of highly active electrocatalysts for practical applications remains challenging. In this regard, we present an overview of the general design principles for efficient electrocatalysts and application of these principles in different electrocatalytic processes. Specifically, enhancing the intrinsic activity of electrocatalysts by electronic state modulation through heteroatom doping, vacancy introduction, interfacial electronic transfer and strain engineering is introduced. In addition, improving the apparent performance of electrocatalysts by mass transport regulation, which is realized by morphological and wettability control, is also discussed. Finally, enlightenment from these studies is summarized and perspectives for the future development of electrocatalysts are provided. The important progress highlighted in this work will provide solid foundations for the tailored design of electrocatalysts toward practical applications.