Unlocking Enhanced Capacitive Deionization of NaTi2(PO4)3/Carbon Materials by the Yolk-Shell Design.

The low salt adsorption capacities (SACs) of benchmark carbon materials (usually below 20 mg g-1) are one of the most challenging issues limiting further commercial development of capacitive deionization (CDI), an energetically favorable method for sustainable water desalination. Sodium superionic conductor (NASICON)-structured NaTi2(PO4)3 (NTP) materials, especially used in combination with carbon to prepare NTP/C materials, provide emerging options for higher CDI performance but face the problems of poor cycling stability and dissolution of active materials. In this study, we report the development of the yolk-shell nanoarchitecture of NASICON-structured NTP/C materials (denoted as ys-NTP@C) using a metal-organic framework@covalent organic polymer (MOF@COP) as a sacrificial template and space-confined nanoreactor. As expected, ys-NTP@C exhibits good CDI performance, including exemplary SACs with a maximum SAC of 124.72 mg g-1 at 1.8 V in the constant-voltage mode and 202.76 mg g-1 at 100 mA g-1 in the constant-current mode, and good cycling stability without obvious performance degradation or energy consumption increase over 100 cycles. Furthermore, X-ray diffraction used to study CDI cycling clearly exhibits the good structural stability of ys-NTP@C during repeated ion intercalation/deintercalation processes, and the finite element simulation shows why yolk-shell nanostructures exhibit better performance than other materials. This study provides a new synthetic paradigm for preparing yolk-shell structured materials from MOF@COP and highlights the potential use of yolk-shell nanoarchitectures for electrochemical desalination.

Numerical simulation of cavitation-vortex interaction mechanism in an advanced rotational hydrodynamic cavitation reactor.

Hydrodynamic cavitation (HC), a promising technology for enhancing processes, has shown distinct effectiveness and versatility in various chemical and environmental applications. The recently developed advanced rotational hydrodynamic cavitation reactors (ARHCRs), employing cavitation generation units (CGUs) to induce cavitation, have demonstrated greater suitability for industrial-scale applications than conventional devices. However, the intricate interplay between vortex and cavitation, along with its spatial-temporal evolution in the complex flow field of ARHCRs, remains inadequately elucidated. This study investigated the interaction mechanism between cavitation and vortex in a representative interaction-type ARHCR for the first time using the "simplified flow field strategy" and the Q-criterion. The findings reveal that the flow instability caused by CGUs leads to intricate helical and vortex flows, subsequently giving rise to both sheet and vortex cavitation. Subsequently, utilizing the Q-criterion, the vortex structures are identified to be concentrated inside and at CGU edges with evolution process of mergence and separation. These vortex structures directly influence the shape and dimensions of cavities, establishing a complex interaction with cavitation. Lastly, the vorticity transport equation analysis uncovered that the stretching and dilatation terms dominate the vorticity transport process. Simultaneously, the baroclinic term focuses on the vapor-liquid interface, characterized by significant alterations in density and pressure gradients. These findings contribute to a better comprehension of the cavitation-vortex interaction in ARHCRs.

Hydrodynamic cavitation-assisted preparation of porous carbon from garlic peels for supercapacitors.

Hydrodynamic cavitation (HC), which can effectively induce sonochemical effects, is widely considered a promising process intensification technology. In the present study, HC was successfully utilized to intensify the alkali activation of GPs for SCs, for the first time. Five BDCMs were synthesized following the method reported in the literature. For comparison, four more BDCMs with HC-treated, among which a sample was further doped with nitrogen during the HC treatment, were prepared. Then all the samples were compared from microscopical characteristics to electrochemical performance as SCs materials. The morphology study demonstrated that the HC treatment had created many defects and amorphous carbon structures on the GP-based BDCMs, with the highest SSA reaching 3272 m2/g (1:6-HCGP), which 32 folded that of the Raw carbon sample's. The HC treatment also intensified the N-doping process. XRD and XPS results manifested that the N content had been increased and consequently changed the electronic structure of the carbon atoms, leading to the increase of specific capacitance (1:6-HCGP+N-based SC, 227 F/g at 10 A/g). The cycle performance proved that the GP-based BDCMs have long-term stability, indicating that the HC-treated BDCMs were good choices for energy storage technologies. Compared with the ultrasound-assisted method, which may have a high energy density, the HC-assisted method enables high production and energy efficiency. This work is a first time attempt towards the industrial application of HC method in energy-related materials synthesis and encourages more in-depth studies in the future.

Effect of the arrangement of cavitation generation unit on the performance of an advanced rotational hydrodynamic cavitation reactor.

Hydrodynamic cavitation (HC) is widely considered a promising process intensification technology. The novel advanced rotational hydrodynamic cavitation reactors (ARHCRs), with considerably higher performance compared with traditional devices, have gained increasing attention of academic and industrial communities. The cavitation generation unit (CGU), located on the rotor and/or stator of an ARHCR, is utilized to generate cavitation and consequently, its geometrical structure is vital for the performance. The present work studied, for the first time, the effect of the arrangement of CGU on the performance of a representative ARHCR by employing computational fluid dynamics based on the "simplified flow field" strategy. The effect of CGU arrangement, which was neglected in the past, was evaluated: radial offset distance (c), intersection angle (ω), number of rows (N), circumferential offset angle (γ), and radial spacing (r). The results indicate that the CGU, with an arrangement of a low ω and moderate c, N, γ, and r, performed the highest cavitation efficiency. The corresponding reasons were analyzed by combining the flow field and cavitation pattern. Moreover, the results also exposed a weakness of the "simplified flow field" strategy which may induce the unfavorable "sidewall effect" and cause false high-pressure region. The findings of this work may provide a reference value to the design of ARHCRs.

Particle size optimization of metal-organic frameworks for superior capacitive deionization in oxygenated saline water.

Pyrolysis-free metal-organic frameworks (MOFs) with optimized particle sizes were used as capacitive deionization (CDI) materials in oxygenated saline water. Upon decreasing the particle size of the MOFs, excellent cycling stability and higher CDI performance were achieved. This was possibly due to the improvement in charge transfer and electrolyte permeation, uncovering the significance of particle size control in improving CDI performance.

Photolysis for the Removal and Transformation of Pesticide Residues During Food Processing: A State-of-the-Art Minireview.

Pesticide residues are of great significant issue that exerted adverse effects on humans. There is a need for effective and non-toxic decontamination of pesticide residues during food processing. In this minireview, the recent advances in the degradation of pesticide residues by photolysis have been firstly described during food processing. The mechanisms of pesticide residues destruction by photolysis were discussed accordingly. Finally, applications of photolysis in the degradation of pesticide residues from beverages, fresh produce, and food rinse waste were also summarized.

Carbon Aerogels as Electrocatalysts for Sustainable Energy Applications: Recent Developments and Prospects.

Carbon aerogel (CA) based materials have multiple advantages, including high porosity, tunable molecular structures, and environmental compatibility. Increasing interest, which has focused on CAs as electrocatalysts for sustainable applications including oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and CO2 reduction reaction (CO2RR) has recently been raised. However, a systematic review covering the most recent progress to boost CA-based electrocatalysts for ORR/OER/HER/CO2RR is now absent. To eliminate the gap, this critical review provides a timely and comprehensive summarization of the applications, synthesis methods, and principles. Furthermore, prospects for emerging synthesis, screening, and construction methods are outlined.

Metal-Organic Frameworks-Based Sensors for the Detection of Toxins in Food: A Critical Mini-Review on the Applications and Mechanisms.

Using scientific technologies to detect toxins in food is significant to prevent food safety problems and protect people's health. Recently, the rise of sensors has made rapid, efficient, and safe detection of food toxins possible. One of the key factors impacting the sensor's performance is the nanomaterials employed. Metal-organic frameworks (MOFs), with high specific surface area, tunable composition, porous structure, and flexible properties, have aroused the interest of researchers. The applications of MOFs in detecting food toxins have seen remarkable success in the past few years. In this critical mini-review, the impact of various synthesis methods on MOFs' properties is first presented. Then, the applications and mechanisms of MOFs-based sensors in detecting various toxins are summarized and analyzed. Finally, future perspectives, potential opportunities, and challenges in this field are discussed.

Recent advances in hydrodynamic cavitation-based pretreatments of lignocellulosic biomass for valorization.

Recently, the hydrodynamic cavitation (HC)-based pretreatment has shown high effectiveness in laboratories and even in industrial productions for conversion of lignocellulosic biomass (LCB) into value-added products. The pretreatment capability derives from the extraordinary conditions of pressures at âˆ¼500 bar, local hotspots with âˆ¼5000 K, and oxidation (hydroxyl radicals) created by HC at room conditions. To promote this emerging technology, the present review summarizes the recent advances in the HC-based pretreatment of LCB. The principle of HC including the sonochemical effect and hydrodynamic cavitation reactor is introduced. The effectiveness of HC on the delignification of LCB as well as subsequent fermentation, paper production, and other applications is evaluated. Several key operational factors (i.e., reaction environment, duration, and feedstock characteristics) in HC pretreatments are discussed. The enhancement mechanism of HC including physical and chemical effects is analyzed. Finally, the perspectives on future research on the HC-based pretreatment technology are highlighted.

Hydrodynamic Cavitation: A Novel Non-Thermal Liquid Food Processing Technology.

Hydrodynamic cavitation (HC), as a novel non-thermal processing technology, has recently shown unique effects on the properties of various liquid foods. The extreme conditions of pressure at ~500 bar, local hotspots with ~5,000 K, and oxidation created by HC can help obtain characteristic products with high quality and special taste. Moreover, compared with other emerging non-thermal approaches, the feature of the HC phenomenon and its generation mechanism helps determine that HC is more suitable for industrial-scale processing. This mini-review summarizes the current knowledge of the recent advances in HC-based liquid food processing. The principle of HC is briefly introduced. The effectiveness of HC on the various physical (e.g., particle size, viscosity, temperature, and stability), chemical (nutrition loss), and biological characteristics (microorganism inactivation) of various liquid foods are evaluated. Finally, several recommendations for future research on the HC technique are provided.

Disinfection characteristics of an advanced rotational hydrodynamic cavitation reactor in pilot scale.

Hydrodynamic cavitation is a promising technique for water disinfection. In the present paper, the disinfection characteristics of an advanced hydrodynamic cavitation reactor (ARHCR) in pilot scale were studied. The effects of various flow rates (1.4-2.6 m3/h) and rotational speeds (2600-4200 rpm) on the removal of Escherichia coli (E. coli) were revealed and analyzed. The variation regularities of the log reduction and reaction rate constant at various cavitation numbers were established. A disinfection rate of 100% was achieved in only 4 min for 15 L of simulated effluent under 4200 rpm and 1.4 m3/h, with energy efficiency at 0.0499 kWh/L. A comprehensive comparison with previously introduced HCRs demonstrates the superior performance of the presented ARHCR system. The morphological changes in E. coli were studied by scanning electron microscopy. The results indicate that the ARHCR can lead to serious cleavage and surface damages to E. coli, which cannot be obtained by conventional HCRs. Finally, a possible damage mechanism of the ARHCR, including both the hydrodynamical and sonochemical effects, was proposed. The findings of the present study can provide strong support to the fundamental understanding and applications of ARHCRs for water disinfection.

Multi-objective optimization of the cavitation generation unit structure of an advanced rotational hydrodynamic cavitation reactor.

Hydrodynamic cavitation (HC) has been widely considered a promising technique for industrial-scale process intensifications. The effectiveness of HC is determined by the performance of hydrodynamic cavitation reactors (HCRs). The advanced rotational HCRs (ARHCRs) proposed recently have shown superior performance in various applications, while the research on the structural optimization is still absent. The present study, for the first time, identifies optimal structures of the cavitation generation units of a representative ARHCR by combining genetic algorithm (GA) and computational fluid dynamics, with the objectives of maximizing the total vapor volume, Vvapor , and minimizing the total torque of the rotor wall, M→z . Four important geometrical factors, namely, diameter (D), interaction distance (s), height (h), and inclination angle (θ), were specified as the design variables. Two high-performance fitness functions for Vvapor and M→z were established from a central composite design with 25 cases. After performing 10,001 simulations of GA, a Pareto front with 1630 non-dominated points was obtained. The results reveal that the values of s and θ of the Pareto front concentrated on their lower (i.e., 1.5 mm) and upper limits (i.e., 18.75°), respectively, while the values of D and h were scattered in their variation regions. In comparison to the original model, a representative global optimal point increased the Vvapor by 156% and decreased the M→z by 14%. The corresponding improved mechanism was revealed by analyzing the flow field. The findings of this work can strongly support the fundamental understanding, design, and application of ARHCRs for process intensifications.

Experimental and numerical studies on the cavitation in an advanced rotational hydrodynamic cavitation reactor for water treatment.

Hydrodynamic cavitation (HC) has emerged as one of the most potential technologies for industrial-scale water treatment. The advanced rotational hydrodynamic cavitation reactors (ARHCRs) that appeared recently have shown their high effectiveness and economical efficiency compared with conventional devices. For the interaction-type ARHCRs where cavitation is generated from the interaction between the cavitation generation units (CGUs) located on the rotor and the stator, their flow field, cavitation generation mechanism, and interaction process are still not well defined. The present study experimentally and numerically investigated the cavitation flow characteristics in a representative interaction-type ARHCR which has been proposed in the past. The cavitation generation mechanism and development process, which was categorized into "coinciding", "leaving", and "approaching" stages, were analyzed explicitly with experimental flow visualization and computational fluid dynamics (CFD) simulations. The changes in the cavitation pattern, area ratio, and sheet cavitation length showed high periodicity with a period of 0.5 ms/cycle at a rotational speed of 3,600 rpm in the flow visualization. The experimental and CFD results indicated that sheet cavitation can be generated on the downstream sides of both the moving and the static CGUs. The sheet cavitation was induced and continuously enlarged in the "leaving" and "approaching" stages and was crushed after the moving CGUs coincided with the static CGUs. In addition, vortex cavitation was formed in the vortex center of each CGU due to high-speed rotating fluid motion. The shape and size of the vortex cavitation were determined by the compression effect produced by the interaction. The findings of this work are important for the fundamental understanding, design, and application of the ARHCRs in water treatment.

A novel continuous hydrodynamic cavitation technology for the inactivation of pathogens in milk.

Hydrodynamic cavitation is a powerful tool for the enhancement of various processing applications. This study utilizes continuous hydrodynamic cavitation (CHC) for the inactivation of pathogens in milk for the first time. The thermal characteristics, inactivation performance, damage on the nutritional composition, product safety, and cost of the advanced rotational hydrodynamic cavitation reactor at pilot scale were comprehensively investigated. The inactivation results demonstrated that 5.89, 5.53, and 2.99 ± 0.08 log reductions of Escherichia coli, Staphylococcus aureus, and Bacillus cereus were achieved, respectively, at a final treatment temperature of 70 °C for 1-2 s. Moreover, the detrimental effect of CHC on the nutritional composition of milk, including mineral, fat, protein, and vitamin contents, was similar to that of high-temperature short-time method. The change in the concentrations of general bacteria and E. coli, as well as the pH value and acidity of the CHC treated milk stored at 5 °C for 14 days was found to be close to that of low-temperature long-time pasteurized milk. The cost of the present CHC treatment was $0.00268/L with a production rate of 4.2 L/min. CHC appears to be a remarkable method for the continuous processing of milk, as well as other liquid foods with high nutrition and "fresh-picked" flavor, due to its high efficacy, good scalability, high production capacity, and low operating and equipment costs.

Development of an efficient catalyst with controlled sulfur vacancies and high pyridine nitrogen content for the photoelectrochemical reduction of CO2 into methanol.

To efficiently and selectively produce liquid hydrocarbon fuels, e.g., methanol, by CO2 photoelectrochemical reduction, CdS nanoparticles (NPs) anchored on the nitrogen-doped carbon particles (NCP) with core-shell dodecahedral porous structure were used as cathode catalysts. Electron paramagnetic resonance (EPR) spectra indicated that CdS/NCP treated at 500 °C had the maximum S-vacancies. The heterojunction generated between CdS with abundant S-vacancies and NCP with a high content of pyridinic N acted as synergistic catalyst for CO2 reduction. CdS/NCP-500 catalyst exhibited a selectivity of 77.3% towards methanol with a total carbon atom conversion rate of 3052 nmol·h-1·cm-2. Density functional theory (DFT) calculations revealed that the S-vacancies decreased the energy barrier for CO2 conversion into methanol product. NCP, exhibiting a high adsorption capacity for CO2, allowed the conversion of COOH* into CO* (ΔE = -3.6 eV), which was then transferred to the CdS surface displaying abundant S-vacancies for the reduction into the methanol product.

Carbon Nanomaterials From Metal-Organic Frameworks: A New Material Horizon for CO2 Reduction.

The rise of CO2 in the atmosphere, which results in severe climate change and temperature increase, is known as the major reason for the greenhouse effect. Reducing CO2 to value-added products is an attractive solution to this severe problem, along with addressing the energy crisis, to which the catalysts being employed are of vital importance. Due to their high porosity and tunable compositions, metal-organic frameworks (MOFs) show great potential in energy conversion systems. By thermal or chemical treatment methods, the MOFs are easily turned into MOF-derived carbon nanomaterials. The much higher level of conductivity enables MOF-derived carbon nanomaterials to be employed in CO2 conversion processes. The present review, discusses the state of the art of MOF-derived carbon nanomaterials in CO2 electrochemical, photocatalytic, and thermal reduction applications. The corresponding reaction mechanisms and influence of various factors on catalyst performance are elaborated. Finally, the deficiencies and recommendations are provided for future progress.

Single Ni atoms with higher positive charges induced by hydroxyls for electrocatalytic CO2 reduction.

To promote the faradaic efficiency of the electrocatalytic CO2 reduction reaction (CO2RR) with low-cost catalysts, single Ni atoms with higher positive charges induced by hydroxyls were proposed to form an atomically dispersed Ni-N4 structure in a cheap honeycomb-like carbon matrix for electrocatalytic CO2 reduction. Extended X-ray absorption fine structure spectroscopy, aberration-corrected High-angle annular dark-field scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements confirmed that the active-center structure consists of single Ni atoms and the adjacent hydroxyl via hydrothermal treatment (H-Ni/NC). Density functional theory calculations indicated that the isolated Ni atoms with higher positive charges induced by the hydroxyl decreased the free energy of the rate-limiting step to 1.05 eV for the CO2RR. The faradaic efficiency (FE) of CO2 reduction into CO was ≥88.0% over the H-Ni/NC catalyst in the potential range of -0.5 to -0.9 V (vs. RHE). The peak CO FE reached 97% at -0.7 V due to the synergistic effect between the unsaturated Ni-N4 active sites and the hydroxyl species.

Solar driven reduction of CO2 using Pt-Cu/C as a catalyst in a photoelectrochemical cell: experiment and mechanism study.

Carbon supported nano-metal catalysts are expected to improve CO2 reduction selectivity and efficiency due to the addition of more active sites and enhancement of electron transport ability. In this study, HKUST-1 was pyrolyzed and decorated with Pt to prepare Pt-Cu/C catalysts. The catalytic effect of the catalysts with different Pt contents in the CO2 photoeletrochemical reduction reaction (CO2PRR) were compared. The total carbon atom conversion rate in CO2PRR experiments using Pt-Cu/C catalysts first increased to a peak when using 1.6 wt% Pt-Cu/C catalyst and then decreased with the increase of Pt content. The 1.6 wt% Pt-Cu/C catalyst showed good hydrogen evolution reaction (HER) inhibiting ability compared with other Pt-Cu/C catalysts. Density functional theory (DFT) calculations were conducted to give an insight into the CO2PRR mechanism on some possible active sites in Pt-Cu/C catalysts. The result demonstrated that HER was more likely to be inhibited on the Cu/Pt active surface and at the same time CO2PRR was promoted.

Preparation of a Cu(BTC)-rGO catalyst loaded on a Pt deposited Cu foam cathode to reduce CO2 in a photoelectrochemical cell.

To increase the reaction productivity and selectivity of the CO2 photoelectrochemical reduction reaction, a Cu (benzene 1,3,5-tricarboxylic acid [BTC])-reduced graphite oxide (rGO) catalyst was prepared by using a facile hydrothermal method and used in a CO2 photoelectrochemical cell (PEC) as a cathode catalyst. Characterization of the catalyst proved that successfully bonding of rGO to Cu(BTC) not only facilitated faster transfer of electrons on the surface of the catalyst but also created more active sites. CO2 photoelectrochemical reduction experimental results showed that the total carbon atom conversion rate was up to 3256 nmol h-1 cm-2 which was much higher than when pure Cu(BTC) was used as a cathode catalyst. The liquid product's selectivity to alcohols was up to 95% when -2 V voltage was applied to the system with Cu(BTC)-rGO used as the cathode catalyst.