Sodium Dodecyl Sulfate-Adjusted Phase Composition of Hydrated Tungsten Oxides as Stable Self-Supporting Electrodes for Supercapacitors with High Volumetric Specific Capacitance.

High pseudocapacitive activity of hydrated tungsten oxides (WO3·xH2O, x = 1 or 2) makes them promising materials for supercapacitors (SCs). During their synthesis, additives such as complexing agents and surfactants generally can only affect the morphology and/or size of the products. Here, we demonstrate that not only morphology and size of WO3·xH2O were affected, its phase composition could also change from WO3·2H2O to WO3·H2O simply by increasing the amount of sodium dodecyl sulfate (SDS) during its anodization synthesis. To the best of our knowledge, such a phenomenon has not been reported before. In addition, SDS introduced a special structure to the products, i.e., WO3·xH2O nanoplatelets constructed from nanoparticle multilayers with abundant nanogaps between the multilayers, which further arranged into nanoflowers with increased amounts of SDS. Benefiting from such a structure, low internal resistance, enhanced stability, and fast redox kinetics, the as-obtained WO3·xH2O/W-3 self-supporting electrode showed a high volumetric specific capacitance of 1402.92 F cm-3 and good cycling stability (a capacity retention of 106% after 10 000 cycles). In addition, an all-solid-state asymmetric SC device based on WO3·xH2O/W-3 delivered high a volumetric energy density of 44.0 mW h cm-3 at 0.5 W cm-3. Our method demonstrates a potential way to fabricate excellent self-supporting electrodes for SCs.

Pickering Emulsion Templated 3D Cylindrical Open Porous Aerogel for Highly Efficient Solar Steam Generation.

Porous-structured evaporators have been fabricated for achieving a high clean water throughput due to their maximized surface area. However, most of the evaporation surfaces in the porous structure are not active because of the trapped vapor in pores. Herein, a three-dimensional (3D) cylindrical aerogel-based photothermal evaporator with a disordered interconnected hierarchical porous structure is developed via a Pickering emulsion-involved polymerization method. The obtained cotton cellulose/aramid nanofibers/polypyrrole (CAP) aerogel-based evaporator achieved all-cold evaporation under 1.0 sun irradiation, which not only completely eliminated energy loss via radiation, convection, and conduction, but also harvested massive extra energy from the surrounding environment and bulk water, thus significantly increasing the total energy input for vapor generation to deliver an extremely high evaporation rate of 5.368 kg m-2 h-1 . In addition, with the external convective flow, solar steam generation over the evaporator can be dramatically enhanced due to fast vapor diffusion out of its unique opened porous structure, realizing an ultrahigh evaporation rate of 18.539 kg m-2 h-1 under 1.0 sun and 4.0 m s-1 . Moreover, this evaporator can continuously operate with concentrated salt solution (20 wt.% NaCl). This work advances rational design and construction of solar evaporator to promote the application of solar evaporation technology in freshwater production.

Evolution of Morphology and Distribution of Salt Crystals on a Photothermal Layer during Solar Interfacial Evaporation.

Solar interfacial evaporation (SIE) by leveraging photothermal conversion could be a clean and sustainable solution to the scarcity of fresh water, decontamination of wastewater, and steam sterilization. However, the process of salt crystallization on photothermal materials used in SIE, especially from saltwater evaporation, has not been completely understood. We report the temporal and spatial evolution of salt crystals on the photothermal layer during SIE. By using a typical oil lamp evaporator, we found that salt crystallization always initiates from the edge of the evaporation surface of the photothermal layer due to the local fast flux of the vapor to the surroundings. Interestingly, the salt crystals exhibit either compact or loose morphology, depending on the location and evaporation duration. By employing a suite of complementary analytical techniques of Raman and infrared spectroscopy and temperature mapping, we followed the evolution and spatial distribution of salt crystals, interfacial water, and surface temperature during evaporation. Our results suggested that the compact crystal structure may emerge from the recrystallization of salt in an initially porous structure, driven by continuous water evaporation from the porous and loose crystals. The holistic view provided in this study may lay the foundation for effective strategies for mitigation of the negative impact of salt crystallization in solar evaporation.

Recent Development of Moisture-Enabled-Electric Nanogenerators.

Power generation by converting energy from the ambient environment has been considered a promising strategy for developing decentralized electrification systems to complement the electricity supply for daily use. Wet gases, such as water evaporation or moisture in the atmosphere, can be utilized as a tremendous source of electricity by emerging power generation devices, that is, moisture-enabled-electric nanogenerators (MEENGs). As a promising technology, MEENGs provided a novel manner to generate electricity by harvesting energy from moisture, originating from the interactions between water molecules and hydrophilic functional groups. Though the remarkable progress of MEENGs has been achieved, a systematic review in this specific area is urgently needed to summarize previous works and provide sharp points to further develop low-cost and high-performing MEENGs through overcoming current limitations. Herein, the working mechanisms of MEENGs reported so far are comprehensively compared. Subsequently, a systematic summary of the materials selection and fabrication methods for currently reported MEENG construction is presented. Then, the improvement strategies and development directions of MEENG are provided. At last, the demonstrations of the applications assembled with MEENGs are extracted. This work aims to pave the way for the further MEENGs to break through the performance limitations and promote the popularization of future micron electronic self-powered equipment.

Facet-specific Active Surface Regulation of Bix MOy (M=Mo, V, W) Nanosheets for Boosted Photocatalytic CO2 reduction.

Photocatalytic performance can be optimized via introduction of reactive sites. However, it is practically difficult to engineer these on specific photocatalyst surfaces, because of limited understanding of atomic-level structure-activity. Here we report a facile sonication-assisted chemical reduction for specific facets regulation via oxygen deprivation on Bi-based photocatalysts. The modified Bi2 MoO6 nanosheets exhibit 61.5 and 12.4 µmol g-1 for CO and CH4 production respectively, ≈3 times greater than for pristine catalyst, together with excellent stability/reproducibility of ≈20 h. By combining advanced characterizations and simulation, we confirm the reaction mechanism on surface-regulated photocatalysts, namely, induced defects on highly-active surface accelerate charge separation/transfer and lower the energy barrier for surface CO2 adsorption/activation/reduction. Promisingly, this method appears generalizable to a wider range of materials.

Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres.

Product selectivity in multielectron electrocatalytic reactions is crucial to energy conversion efficiency and chemical production. However, a present practical drawback is the limited understanding of actual catalytic active sites. Here, using as a prototype single-atom catalysts (SACs) in acidic oxygen reduction reaction (ORR), we report the structure-property relationship of catalysts and show for the first time that molecular-level local structure, including first and second coordination spheres (CSs), rather than individual active atoms, synergistically determines the electrocatalytic response. ORR selectivity on Co-SACs can be tailored from a four-electron to a two-electron pathway by modifying first (N or/and O coordination) and second (C-O-C groups) CSs. Using combined theoretical predictions and experiments, including X-ray absorption fine structure analyses and in situ infrared spectroscopy, we confirm that the unique selectivity change originates from the structure-dependent shift of active sites from the center Co atom to the O-adjacent C atom. We show this optimizes the electronic structure and *OOH adsorption behavior on active sites to give the present "best" activity and selectivity of >95% for acidic H2O2 electrosynthesis.

Efficient Nitrogen Fixation to Ammonia through Integration of Plasma Oxidation with Electrocatalytic Reduction.

Present one-step N2 fixation is impeded by tough activation of the N≡N bond and low selectivity to NH3 . Here we report fixation of N2 -to-NH3 can be decoupled to a two-step process with one problem effectively solved in each step, including: 1) facile activation of N2 to NOx - by a non-thermal plasma technique, and 2) highly selective conversion of NOx - to NH3 by electrocatalytic reduction. Importantly, this process uses air and water as low-cost raw materials for scalable ammonia production under ambient conditions. For NOx - reduction to NH3 , we present a surface boron-rich core-shell nickel boride electrocatalyst. The surface boron-rich feature is the key to boosting activity, selectivity, and stability via enhanced NOx - adsorption, and suppression of hydrogen evolution and surface Ni oxidation. A significant ammonia production of 198.3 µmol cm-2 h-1 was achieved, together with nearly 100 % Faradaic efficiency.

Understanding the surface properties and rheology of a silica suspension mediated by a comb-type poly(acrylic acid)/poly(ethylene oxide) (PAA/PEO) copolymer: effect of salinity.

Understanding the surface properties and rheology of colloidal suspensions in the presence of polymer additives with high salinity are of great importance in formulating construction materials and optimizing process conditions in the mining and petroleum industry. In this work, the surface properties and rheology of a model spherical silica aqueous suspension mediated by a comb-type poly(acrylic acid)/poly(ethylene oxide) (PAA/PEO) copolymer at various salt concentrations have been investigated. Adsorption measurements using a Quartz Crystal Microbalance with Dissipation monitoring (QCM-D) align well with zeta potential tests and show that polymer adsorption on silica surfaces is enhanced at high salinity (i.e., 3 M NaCl) than at low salinity (i.e., 1 mM NaCl) due to the suppression of the electrical double layer. Surface Forces Apparatus (SFA) measurements reveal that for interactions between two mica surfaces (the basal plane of which has a similar structure as silica) at a high polymer concentration (e.g., 2 wt%), steric repulsion dominates in 1 mM NaCl while bridging attraction is observed in 3 M NaCl. Surface force measurements agree with rheological results on silica suspensions with 0.5 to 2 wt% of PAA/PEO addition, which shows a significant decrease in yield stress in 1 mM NaCl due to steric repulsion but an insignificant variation in yield stress in 3 M NaCl due to attractive bridging interactions. This work provides useful information regarding the surface properties and rheological properties of comb-type polymer-mediated silica suspensions under different salinity conditions, with implications on designing and processing complex colloidal suspensions with polymer additives for various applications.

Formation of Aluminum Hydroxide-Doped Surface Passivating Layers on Pyrite for Acid Rock Drainage Control.

The aim of this study was to test the performance of a novel method for acid rock drainage (ARD) control through the formation of Al(OH)3-doped passivating surface layers on pyrite. At pH 2.0 and 4.0, there was no obvious inhibition of the pyrite oxidation rate on addition of 20 mg L-1 Al3+ (added as AlCl3·6H2O). In comparison, the pyrite oxidation rate at circumneutral pH (7.4 ± 0.4) decreased with increasing added Al3+ with ≈98% reduction in long-term (282 days) dissolution rates in the presence of 20 mg L-1 Al3+. Al3+ was added to the solution and allowed to equilibrate prior to pyrite addition (2 g L-1). Consequently almost all Al3+ (>99.9%) was initially present as aluminum hydroxide precipitates at pH 7.4. X-ray photoelectron spectroscopy analysis showed a significant concentration of Al3+ (20.3 at. %) on the pyrite surface reacted at pH 7.4 with 20 mg L-1 added Al3+, but no Al3+ on pyrite surfaces reacted at pH 2.0 and 4.0 with added Al3+. Transmission electron microscopy and synchrotron X-ray absorption near edge spectroscopy analyses indicated that compact surface layers containing both goethite and amorphous or nanocrystalline Al(OH)3 formed in the presence of 20 mg L-1 Al3+ at circumneutral pH, in contrast to the porous goethite surface layers formed on pyrite dissolved in the absence of Al3+ under otherwise identical conditions. This work demonstrates the potential for novel Al-based pyrite passivation of relevance to the mining industry where suitable Al-rich waste materials are available for ARD control interventions.

Solvent Effects on the Formation of Surface Nanodroplets by Solvent Exchange.

Solvent exchange is a simple process to form oil nanodroplets at solid-liquid interfaces with well-defined location and morphology. In this process, a good solvent of the oil is displaced by a poor solvent, leading to the nucleation and growth of oil droplets from a transient oversaturation at the mixing front. Our recent work has shown that the final volume of the droplets is related to the flow conditions. In this work, we investigate the effects of the type and the composition of solvents on the droplet formation under the same flow conditions. Water nanodroplets were produced by ethanol/cyclohexane (solution A) and cyclohexane (solution B) on a hydrophilic substrate. We found that the droplet size increases first and then decreases with an increase of the initial ethanol concentration in solution A. This is attributed to the phase separation of ethanol-cyclohexane-water; in particular, the composition of solution A on the phase boundary above the Ouzo region. The same reason also contributes to the lower efficiency in droplet formation for a longer alkane. The important implication from this work is that the maximal droplet volume is limited by the phase separation of the solvents used in the solvent exchange.

Interfacial Solar Evaporation: From Fundamental Research to Applications.

In the last decade, interfacial solar steam generation (ISSG), powered by natural sunlight garnered significant attention due to its great potential for low-cost and environmentally friendly clean water production in alignment with the global decarbonization efforts. This review aims to share the knowledge and engage with a broader readership about the current progress of ISSG technology and the facing challenges to promote further advancements toward practical applications. The first part of this review assesses the current strategies for enhancing the energy efficiency of ISSG systems, including optimizing light absorption, reducing energy losses, harvesting additional energy, and lowering evaporation enthalpy. Subsequently, the current challenges faced by ISSG technologies, notably salt accumulation and bio-fouling issues in practical applications, are elucidated and contemporary methods are discussed to overcome these challenges. In the end, potential applications of ISSG, ranging from initial seawater desalination and industrial wastewater purification to power generation, sterilization, soil remediation, and innovative concept of solar sea farm, are introduced, highlighting the promising potential of ISSG technology in contributing to sustainable and environmentally conscious practices. Based on the review and in-depth understanding of these aspects, the future research focuses are proposed to address potential issues in both fundamental research and practical applications.

Polyelectrolyte Hydrogel-Functionalized Photothermal Sponge Enables Simultaneously Continuous Solar Desalination and Electricity Generation Without Salt Accumulation.

Technologies that can simultaneously generate electricity and desalinate seawater are highly attractive and required to meet the increasing global demand for power and clean water. Here, a bifunctional solar evaporator that features continuous electric generation in seawater without salt accumulation is developed by rational design of polyelectrolyte hydrogel-functionalized photothermal sponge. This evaporator not only exhibits an unprecedentedly high water evaporation rate of 3.53 kg m-2 h-1along with 98.6% solar energy conversion efficiency but can also uninterruptedly deliver a voltage output of 0.972 V and a current density of 172.38 µA cm-2 in high-concentration brine over a prolonged period under one sun irradiation. Many common electronic devices can be driven by simply connecting evaporator units in series or in parallel without any other auxiliaries. Different from the previously proposed power generation mechanism, this study reveals that the water-enabled proton concentration fields in intermediate water region can also induce an additional ion electric field in free water region containing solute, to further enhance electricity output. Given the low-cost materials, simple self-regeneration design, scalable fabrication processes, and stable performance, this work offers a promising strategy for addressing the shortages of clean water and sustainable electricity.

Multi-Interface Engineering of MXenes for Self-Powered Wearable Devices.

Self-powered wearable devices with integrated energy supply module and sensitive sensors have significantly blossomed for continuous monitoring of human activity and the surrounding environment in healthcare sectors. The emerging of MXene-based materials has brought research upsurge in the fields of energy and electronics, owing to their excellent electrochemical performance, large surface area, superior mechanical performance, and tunable interfacial properties, where their performance can be further boosted via multi-interface engineering. Herein, a comprehensive review of recent progress in MXenes for self-powered wearable devices is discussed from the aspects of multi-interface engineering. The fundamental properties of MXenes including electronic, mechanical, optical, and thermal characteristics are discussed in detail. Different from previous review works on MXenes, multi-interface engineering of MXenes from termination regulation to surface modification and their impact on the performance of materials and energy storage/conversion devices are summarized. Based on the interfacial manipulation strategies, potential applications of MXene-based self-powered wearable devices are outlined. Finally, proposals and perspectives are provided on the current challenges and future directions in MXene-based self-powered wearable devices.

Surface hydrophilicity-mediated migration of nano/microparticles under temperature gradient in a confined space.

HYPOTHESIS: Particle transport by a temperature gradient is prospective in many biomedical applications. However, the prevalence of boundary confinement in practical use introduces synergistic effects of thermophoresis and thermo-osmosis, causing controversial phenomena and great difficulty in understanding the mechanisms. EXPERIMENTS: We developed a microfluidic chip with a uniform temperature gradient and switchable substrate hydrophilicity to measure the migrations of various particles (d = 200 nm - 2 µm), through which the effects of particle thermophoresis and thermo-osmotic flow from the substrate surface were decoupled. The contribution of substrate hydrophilicity on thermo-osmosis was examined. Thermophoresis was measured to clarify its dependence on particle size and hydrophilicity. FINDINGS: This paper reports the first experimental evidence of a large enthalpy-dependent thermo-osmotic mobility χ âˆ¼ ΔH on a hydrophobic polymer surface, which is 1-2 orders of magnitude larger than that on hydrophilic surfaces. The normalized Soret coefficient for polystyrene particles, ST/d = 18.0 K-1µm-1, is confirmed to be constant, which helps clarify the controversy of the size dependence. Besides, the Soret coefficient of hydrophobic proteins is approximately-four times larger than that of hydrophilic extracellular vesicles. These findings suggest that the intrinsic slip on the hydrophobic surface could enhance both surface thermo-osmosis and particle thermophoresis.

Oxygen Defect and Cl--Doped Modulated TiNb2O7 Compound with High Rate Performance in Lithium-Ion Batteries.

TiNb2O7 has attracted extensive attention from lithium-ion battery researchers due to its superior specific capacity and safety. However, its poor ion conductivity and electron conductivity hinder its further development. To improve the ion/electron transport of TiNb2O7, we report that chlorine doping and oxygen vacancy engineering regulate the energy band and crystal structure simultaneously through a simple solid-phase method. NH4Cl was used to realize Cl- doping and oxygen vacancy production. A Rietveld refinement demonstrates an effective substitution of Cl in the O sites of Nb-O octahedra, with an enlarged crystal plane spacing. The oxygen vacancies provide more active sites for lithium intercalation. The diffusion coefficient of Li+ is inceased from 2.39 × 10-14 to 1.50 × 10-13 cm2 s-1, which reveals the positive influence of Cl- doping and oxygen vacancies on the promoted Li+ transport behavior. Charge compensation is introduced by the doping of Cl- and the generation of oxygen vacancies, leading to the formation of Ti3+ and Nb4+ and the adjustment of the electronic structure. DFT calculations reveal that TiNb2O7 with Cl- doping and an O vacancy shows a metallic property with a finite value at the Fermi level, which is conducive to electron transfer in the electrode material. Benefiting from these advantages, the modified TiNb2O7 presents superior rate performance with a commendable capacity of 172.82 mAh g-1 at 50 C. This work provides guidance to design high-performance anode materials for high-rate lithium-ion batteries.

Rapid seeded growth of monodisperse, quasi-spherical, citrate-stabilized gold nanoparticles via H2O2 reduction.

In this report, we demonstrate a rapid and simple seeded growth method for synthesizing monodisperse, quasi-spherical, citrate-stabilized Au nanoparticles (Au NPs) via H(2)O(2) reduction of HAuCl(4). Au NPs with diameter ranging from 30 to 230 nm can be synthesized by simply adding 12 nm citrate stabilized Au NP seeds to an aqueous solution of H(2)O(2) and HAuCl(4) under ambient conditions. The diameter of the resulting Au NPs can be quantitatively controlled by the molar ratio of HAuCl(4) to the Au seeds. The standard deviation of the Au NP sizes is less than 10%, and the ellipticity (ratio of major to minor axes) of the NPs is less than 1.1. Compared to existing ones, the present seeded growth approach is implemented within 1 min under ambient condition, and no unfavorable additives are involved because H(2)O(2) can readily decompose into H(2)O during storage or via boiling.

Electrostatic repulsion-controlled formation of polydopamine-gold Janus particles.

Polydopamine (PDA)-Au Janus particles were obtained by simply adding HAuCl(4) to a PDA particle suspension, prepared via self-polymerization of dopamine in basic solution at room temperature. The structures of the PDA-Au particles are readily controlled by electrostatic repulsion between the constituent particles, which can be realized simply via adjusting the environmental pH. PDA-Au Janus particles are formed only in a narrow pH range of 2.5-3.0 due to the properly enhanced electrostatic repulsion between the Au particles growing on as-prepared PDA particles and between the Au and PDA particles. The obtained PDA-Au Janus particles can become interfacially active and self-assemble at oil/water interfaces as a result of spatially well-separated hydrophilic (PDA) and hydrophobic (Au) domains on the surfaces, reminiscent of amphiphilic molecules.

Highly Transparent and Self-Healable Solar Thermal Anti-/Deicing Surfaces: When Ultrathin MXene Multilayers Marry a Solid Slippery Self-Cleaning Coating.

Solar anti-/deicing can solve icing problems by converting sunlight into heat. One of the biggest problems, which has long been plaguing the design of solar anti-/deicing surfaces, is that photothermal materials are always lightproof and appear black, because of the mutual exclusiveness between generating heat and retaining transparency. Herein, a highly transparent and scalable solar anti-/deicing surface is reported, which enables the coated glass to exhibit high transparency (>77% transmittance at 550 nm) and meanwhile causes a >30 °C surface temperature increase relative to the ambient environment under 1.0 sun illumination. Such a transparent anti-/deicing surface can be fabricated onto a large class of substrates (e.g., glass, ceramics, metals, plastics), by applying a solid omniphobic slippery coating onto layer-by-layer-assembled ultrathin MXene multilayers. Hence, the surface possesses a self-cleaning ability to shed waterborne and oil-based liquids thanks to residue-free slipping motion. Passive anti-icing and active deicing capabilities are, respectively, obtained on the solar thermal surface, which effectively prevents water from freezing and simultaneously melts pre-formed ice and thick frost. The self-cleaning effect enables residue-free removal of unfrozen water and interfacially melted ice/frost to boost the anti-/deicing efficiency. Importantly, the surface is capable of self-healing under illumination to repair physical damage and chemical degradation.

Towards sustainable saline agriculture: Interfacial solar evaporation for simultaneous seawater desalination and saline soil remediation.

Interfacial solar steam generation is an efficient way to produce freshwater from saline water. This technology was further harnessed here for simultaneous saline soil remediation and enhanced agricultural sustainability. An interfacial solar evaporation and planting system was designed that uses treated seawater for saline soil washing and agricultural irrigation. In outdoor experiments the evaporator realized high freshwater production (10.95 kg m-2 day-1) with a soil washing efficiency 3 times greater than traditional distillation. Post treatment plant assays showed that initially highly saline soils could be restored to functional agricultural soils with germination rates of 65% after soil washing, where solar evaporation could continuously provide irrigation water for plant growth. This system is fully automated and uses only solar energy and seawater for saline soil remediation and irrigation. The development of this system provides a potentially useful solution to alleviate global problems associated with water scarcity, soil salinization, and desertification.

Electrostatic interaction-controlled dispersion of carbon nanotubes in a ternary composite for high-performance supercapacitors.

Effective dispersion of carbon nanotubes (CNTs) is of great importance to achieve their intrinsic performance. Normally, it is believed that CNT dispersion is decided by interactions between CNTs and their dispersants, while other interactions are often neglected. Herein, three ionic surfactants, sodium dodecyl sulfate (SDS), dodecyl dimethyl betaine (BS-12) and cetyltrimethylammonium bromide (CTAB), are used to disperse CNTs in a ternary composite, i.e., poly(p-phenylenediamine)-phosphomolybdic acid@reduced graphene oxide (DMoG), respectively, leading to three different DMoGC composites. It has been found that the CNT dispersion in DMoGC was mainly controlled by electrostatic interactions between the surfactants and DMoG, which further exerted vital influences on the constitution, content, morphology, porous structure and supercapacitive performance of the DMoGC composites. Among the three surfactants, cationic CTAB showed the best CNT dispersion, while amphoteric BS-12 could hardly disperse CNTs in DMoGC, leading to DMoGC-CTAB with a 2 times larger specific surface area (152.3 m2 g-1) and 1.5 times higher specific capacitance (422 F g-1) than those of DMoGC-(BS-12). Our study can provide valuable guidelines for selecting/designing effective dispersants to prepare multi-component composites containing uniformly dispersed CNTs.