Membrane technology has become the mainstream process for the production of electronic grade hydrogen peroxide (H₂O₂). But due to the oxidation degradation of the organic membranes (e.g. polyamide) by the strong oxidative radicals (e.g.·OH) generated via the activation of H₂O₂ by iron ions (Fe³⁺), the short effective lifetime of membranes remains a challenge. Inorganic nano tin oxide (SnO₂) has great potential for the removal of Fe³⁺ in strongly oxidative H₂O₂ because of its ability to stabilize H₂O₂ and preferentially adsorb Fe³⁺. Herein, we have designed for the first time a flower-like robust SnO₂ membrane on the ceramic support by in situ template-free one-step hydrothermal method. The three-dimensional loose pore structure in the membrane built by interlacing SnO₂ nanosheets endows the SnO₂ membrane with a high specific surface area and abundant adsorption sites (—OH). Based on the coordination complexation and electrostatic attraction between the SnO₂ surface and Fe³⁺, the membrane shows a high Fe³⁺ removal efficiency (83%) and permeability (24 L·m^-2·h^-1·MPa^-1) in H₂O₂. This study provides an innovative and simple approach to designing robust SnO₂ membranes for highly efficient removal of Fe³⁺ in harsh environments, such as strong oxidation conditions.

Coal gasification fly ash (CGFA) is an industrial solid waste from the coal circulating fluidized bed (CFB) gasification process, and it needs to be effectively disposed to achieve sustainable development of the environment. To realize the application of CGFA as a precursor of porous carbon materials, the physicochemical properties of three kinds of CGFA from industrial CFB gasifiers are analyzed. Then, the activation potential of CGFA is acquired via steam activation experiments in a tube furnace reactor. Finally, the fluidization activation technology of CGFA is practiced in a bench-scale CFB test rig, and its advantages are highlighted. The results show that CGFA is characterized by a high carbon content in the range of 54.06%-74.09%, an ultrafine particle size (d₅₀:16.3-26.1 lm), and a relatively developed pore structure (specific surface area S_SA:139.29-551.97 m²·g^-1). The proportion of micropores in CGFA increases gradually with the coal rank. Steam activation experiments show that the pore development of CGFA mainly includes three stages:initial pore development, dynamic equilibrium between micropores and mesopores and pore collapse. The S_SA of lignite fly ash (LFA), subbituminous fly ash (SBFA) and anthracite fly ash (AFA) is maximally increased by 105%, 13% and 72% after steam activation; the order of the largest carbon reaction rate and decomposition ratio of steam among the three kinds of CGFA is SBFA > LFA > AFA. As the ratio of oxygen to carbon during the fluidization activation of LFA is from 0.09 to 0.19, the carbon conversion ratio increases from 14.4% to 26.8% and the cold gas efficiency increases from 6.8% to 10.2%. The S_SA of LFA increases by up to 53.9% during the fluidization activation process, which is mainly due to the mesoporous development. Relative to steam activation in a tube furnace reactor, fluidization activation takes an extremely short time (seconds) to achieve the same activation effect. It is expected to further improve the activation effect of LFA by regulating the carbon conversion ratio range of 27%-35% to create pores in the initial development stage.

Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry. Herein, a heterogeneous Pd catalyst (Pd/NCF) was prepared by supporting Pd ultrafine metal nanoparticles (NPs) on nitrogen-doped carbon;synthesized by using F127 as a stabilizer, as well as chitosan as a carbon and nitrogen source. The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate, exhibiting higher stability than Pd/NC prepared without F127 addition. The hydrogen bond between chitosan (CTS) and F127 was enhanced by F127, which anchored the N in the free amino group, increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs. This process helped to improve metal dispersion. The increased metal-support interaction, which limits the leaching and coarsening of Pd NPs, improves the stability of the Pd/NCF catalyst. Furthermore, density functional theory calculations indicated that pyridine N stabilized the Pd²⁺ species, significantly inhibiting the loss of Pd²⁺ in Pd/NCF during the reaction process. This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

As a common precursor for supercritical CO₂ (scCO₂) deposition techniques, solubility data of organometallic complexes in scCO₂ is crucial for the preparation of nanocomposites. Recently, metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials. In this study, the solubilities of iron(III) acetylacetonate (Fe(acac)₃) and nickel(II) acetylacetonate (Ni(acac)₂) were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5-25.2 MPa to accumulate new solubility data. Solubility was measured using a static weight loss method. The semi-empirical models proposed by Chrastil and Sung et al. were used to correlate the solubility data of Fe(acac)₃ and Ni(acac)₂. The equations obtained can be used to predict the solubility of the same system in the experimental range.

Dust removal from pyrolytic vapors at high temperatures is an obstacle to the industrialization of the coal pyrolysis process. In this work, a granular bed with expanded perlites as filtration media was designed and integrated into a 10 t·d^-1 coal pyrolysis facility. The testing results showed that around 97.56% dust collection efficiency was achieved. As a result, dust content in tar was significantly lowered. The pressure drop of the granular bed maintained in the range of 356 Pa to 489 Pa. The dust size in the effluent after filtration exhibited a bimodal distribution, which was attributed to the heterogeneity of the dust components. The effects of filtration bed on pyrolytic product yields were also discussed. A modified filtration model based on the macroscopic phenomenological theory was proposed to describe the performance of the granular bed. The computation results were well agreed with the experimental data.

The reduction of phosphogypsum (PG) to lime slag and SO₂ using coke can effectively alleviate the environmental problems caused by PG. However, the PG decomposition temperature remains high and the product yield remains poor. By adding additives, the decomposition temperature can be further reduced and PG decomposition rate and product yield can be improved. However, the use of current additives such as Fe₂O₃ and SiO₂ brings the problem of increasing economic cost. Therefore, it is proposed to use solid waste copper slag (CS) as a new additive to reduce PG to prepare SO₂, which can reduce the cost and meet the environmental benefits at the same time. The effects of proportion, temperature and thermostatic time on PG decomposition are investigated by experimental and kinetic analysis combined with FactSage thermodynamic calculations to optimize the roasting conditions. Finally, the reaction mechanism is proposed. It is found that adding CS to the coke and PG system can increase the rate of PG decomposition and SO₂ yield while lowering the PG decomposition temperature. For example, when the CS/PG mass ratio increases from 0 to 1, PG decomposition rate increases from 83.38% to 99.35%, SO₂ yield increases from 78.62% to 96.81%, and PG decomposition temperature decreases from 992.4 ℃ to 949.6 ℃. The optimal reaction parameters are CS/PG mass ratio of 1, Coke/PG mass ratio of 0.06 at 1100 ℃ for 20 min with 99.35% PG decomposition rate and 96.81% SO₂ yield. The process proceeds according to the following reactions:2CaSO₄+0.7C+0.8Fe₂SiO₄→0.8Ca₂SiO₄+0.2Ca₂Fe₂O₅+0.4Fe₃O₄+2SO₂+0.7CO₂ Finally, a process for decomposing PG with coke and CS is proposed.

NF₃ is commonly used as an etching and cleaning gas in semiconductor industry, however it is a strongly greenhouse gas. Therefore, the destruction of disposal NF₃ is an urgent task to migrate the greenhouse effect. Among the technologies for NF₃ abatement, the destructive sorption of NF₃ over metal oxides sor bents is an effective way. Thus, the search for a highly reactive and utilized sorbent for NF₃ destruction is in great demand. In this work, AlOOH supported on carbon-sphere (AlOOH/CS) as precursors were syn thesized hydrothermally and heat-treated to prepare the Al₂O₃ sorbents. The influence of AlOOH/CS hydrothermal temperatures on the reactivity of derived Al₂O₃ sorbents for NF₃ destruction was investi gated, and it is shown that the Al₂O₃ from AlOOH/CS hydro-thermalized at 120℃ is superior to others. Subsequently, the optimized Al₂O₃ was covered by Mn(OH)_x to prepare Mn/Al₂O₃ sorbents via changing hydrothermal temperatures and Mn loadings. The results show that the Mn/Al₂O₃ sorbents are more uti lized than bare Al₂O₃ in NF₃ destructive sorption due to the promotional effect of Mn₂O₃ as surface layer on the fluorination of Al₂O₃ as substrate, especially the optimal 5%Mn/Al₂O₃(160 ℃) exhibits a utilization percentage as high as 90.4%, and remarkably exceeds all the sorbents reported so far. These findings are beneficial to develop more efficient sorbents for the destruction of NF₃.

Elliptical tanks were used as an alternative to circular tanks in order to improve mixing efficiency and reduce mixing time in unbaffled stirred tanks (USTs). Five different aspect ratios of elliptical vessels were designed to compare their mixing time and flow field. Computational fluid dynamics (CFD) simulations were performed using the k-ε model to calculate the mixing time and simulate turbulent flow field features, such as streamline shape, velocity distribution, vortex core region distribution, and turbulent kinetic energy (TKE) transfer. Visualization was also carried out to track the tinctorial evolution of the liquid phase. Results reveal that elliptical stirred tanks can significantly improve mixing performance in USTs. Specifically, the mixing time at an aspect ratio of 2.00 is only 45.3% of the one of a circular stirred tank. Furthermore, the secondary flow is strengthened and the vortex core region increases with the increase of aspect ratio. The axial velocity is more sensitive to the aspect ratio than the circumferential and radial velocity. Additionally, the TKE transfer in elliptical vessels is altered. These findings suggest that elliptical vessels offer a promising alternative to circular vessels for enhancing mixing performance in USTs.

Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals. However, the micropores of zeolites impose diffusion limitations on bulky molecules, greatly reducing the catalytic efficiency. Herein, we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate. The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed. Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores, smaller crystal size, and larger external specific surface area compared to commercial NaX zeolite. Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite, and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite. This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites, which may gain wide applications in fine chemical manufacturing.

The adsorptive separation of C₂H₄ and C₂H₆, as an alternative to distillation units consuming high energy, is a promising yet challenging research. The great similarity in the molecular size of C₂H₄ and C₂H₆ brings challenges to the regulation of adsorbents to realize efficient dynamic separation. Herein, we reported the enhancement of the kinetic separation of C₂H₄/C₂H₆ by controlling the crystal size of ZnAtzPO₄ (Atz=3-amino-1,2,4-triazole) to amplify the diffusion difference of C₂H₄ and C₂H₆. Through adjusting the synthesis temperature, reactant concentration, and ligands/metal ions molar ratio, ZnAtzPO₄ crystals with different sizes were obtained. Both single-component kinetic adsorption tests and binary-component dynamic breakthrough experiments confirmed the enhancement of the dynamic separation of C₂H₄/C₂H₆ with the increase in the crystal size of ZnAtzPO₄. The separation selectivity of C₂H₄/C₂H₆ increased from 1.3 to 98.5 with the increase in the crystal size of ZnAtzPO₄. This work demonstrated the role of morphology and size control of adsorbent crystals in the improvement of the C₂H₄/C₂H₆ kinetic separation performance.

ZSM-5 with hierarchical pore structure was synthesized by a simple two-step hydrothermal crystallization from silica fume without using any organic ammonium templates. The synthesized ZSM-5 were oval shaped particles with a particle size about 2.0 lm and weak acid-dominated with proper Brønsted (B) and Lewis (L) acid sites. The ZSM-5 was used for catalytic co-cracking of n-octane and guaiacol, low-density polyethylene (LDPE) and alkali lignin (AL) to enhance the production of benzene, toluene, ethylbenzene and xylene (BTEX). The most significant synergistic effect occurred at n-octane/guaiacol at 1:1 and LDPE/AL at 1:3, under the condition, the achieved BTEX selectivity were 24% and 33% (mass) higher than the calculated values (weighted average). The highest BTEX selectivity reached 88.5%, which was 3.7% and 54.2% higher than those from individual cracking LDPE and AL. The synthesized ZSM-5 exhibited superior catalytic performance compared to the commercial ZSM-5, indicating potential application prospect.

Co-combustion of methane (CH₄) and acid gas (AG) is required to sustain the temperature in Claus reaction furnace. In this study, oxy-fuel combustion of methane and acid gas has been experimentally studied in a diffusion flame. Three equivalence ratios (ER=1.0, 1.5, 2.0) and CH₄-addition ratios (CH₄/AG=0.3, 0.5, 0.7) were examined and the flame was interpreted by analyzing the distributions of the temperature and species concentration along central axial. CH₄-AG diffusion flame could be classified into three sections namely initial reaction, oxidation and complex reaction sections. Competitive oxidation of CH₄ and H₂S was noted in the first section wherein H₂S was preferred and both were mainly proceeding decomposition and partial oxidation. SO₂ was formed at oxidation section together with obvious presence of H₂ and CO. However, H₂ and CO were inclined to be sustained under fuel rich condition in the complex reaction section. Reducing ER and increasing CH₄/AG contributed to higher temperature, H₂S and CH₄ oxidation and CO₂ reactivity. Hence a growing trend for CH₄ and AG to convert into H₂, CO and SO₂ could be witnessed. And this factor enhanced the generation of CS₂ and COS in the flame inner core by interactions of CH₄ and CO₂ with sulfur species. COS was formed through the interactions of CO and CO₂ with sulfur species. The CS₂ production directly relied on reaction of CH₄ with sulfur species. The concentration of COS was greater than CS₂ since CS₂ was probably inhibited due to the presence of H₂. COS and CS₂ could be consumed by further oxidation or other complex reactions.

To achieve the resource utilization of solid waste phosphogypsum (PG) and tackle the problem of utilizing potassium feldspar (PF), a coupled synergistic process between PG and PF is proposed in this paper. The study investigates the features of P and F in PG, and explores the decomposition of PF using hydrofluoric acid (HF) in the sulfuric acid system for K leaching and leaching of P and F in PG. The impact factors such as sulfuric acid concentration, reaction temperature, reaction time, material ratio (PG/PF), liquid- solid ratio, PF particle size, and PF calcination temperature on the leaching of P and K is systematically investigated in this paper. The results show that under optimal conditions, the leaching rate of K and P reach more than 93% and 96%, respectively. Kinetics study using shrinking core model (SCM) indicates two significant stages with internal diffusion predominantly controlling the leaching of K. The apparent activation energies of these two stages are 11.92 kJ·mol^-1 and 11.55 kJ·mol^-1, respectively.

The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method. During the preparation of the Fe-NC catalyst, the complexation of N elements in urea could anchor Fe, and the formation of C₃N₄ during urea pyrolysis could also prevent migration and aggregation of Fe species, which jointly improve the dispersion and stability of Fe. The FeN₄ sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation, while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process, which together promote catalytic degradation of m-cresol by PMS activation. Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO₄^-· and ·OH, and partially based on ·OH as the active components, and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed. This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.

In this work, the ternary azeotrope of tert-butyl alcohol/ethyl acetate/water is separated by extractive distillation (ED) to recover the available constituents and protect the environment. Based on the conductor like shielding model and relative volatility method, ethylene glycol was selected as the extractant in the separation process. In addition, in view of the characteristic that the relative volatility between components changes with pressure, the multi-objective optimization method based on nondominated sorting genetic algorithm II optimizes the pressure and the amount of solvent cooperatively to avoid falling into the optimal local solution. Based on the optimal process parameters, the proposed heat-integrated process can reduce the gas emissions by 29.30%. The heat-integrated ED, further coupled with the pervaporation process, can reduce gas emission by 42.36% and has the highest exergy efficiency of 47.56%. In addition, based on the heat-integrated process, the proposed two heat pump assisted heat-integrated ED processes show good economic and environmental performance. The double heat pump assisted heat-integrated ED can reduce the total annual cost by 28.78% and the gas emissions by 55.83% compared with the basis process, which has a good application prospect. This work provides a feasible approach for the separation of ternary azeotropes.

In this study, the impact of different reaction times on the preparation of powdered activated carbon (PAC) using a one-step rapid activation method under flue gas atmosphere is investigated, and the underlying reaction mechanism is summarized. Results indicate that the reaction process of this method can be divided into three stages:stage I is the rapid release of volatiles and the rapid consumption of O₂, primarily occurring within a reaction time range of 0-0.5 s; stage II is mainly the continuous release and diffusion of volatiles, which is the carbonization and activation coupling reaction stage, and the carbonization process is the main in this stage. This stage mainly occurs at the reaction time range of 0.5-2.0 s when SL-coal is used as material, and that is 0.5-3.0 s when JJ-coal is used as material; stage III is mainly the activation stage, during which activated components diffuse to both the surface and interior of particles. This stage mainly involves the reaction stage of CO₂ and H₂O (g) activation, and it mainly occurs at the reaction time range of 2.0-4.0 s when SL-coal is used as material, and that is 3.0-4.0 s when JJ-coal is used as material. Besides, the main function of the first two stages is to provide more diffusion channels and contact surfaces/activation sites for the diffusion and activation of the activated components in the third stage. Mastering the reaction mechanism would serve as a crucial reference and foundation for designing the structure, size of the reactor, and optimal positioning of the activator nozzle in PAC preparation.

The homogeneous/particulate fluidization flow regime is particularly suitable for handling the various gas-solid contact processes encountered in the chemical and energy industry. This work aimed to extend such a regime of Geldart-A particles by exerting the axial uniform and steady magnetic field. Under the action of the magnetic field, the overall homogeneous fluidization regime of Geldart-A magnetizable particles became composed of two parts:inherent homogeneous fluidization and newly-created magnetic stabilization. Since the former remained almost unchanged whereas the latter became broader as the magnetic field intensity increased, the overall homogeneous fluidization regime could be extended remarkably. As for Geldart-A nonmagnetizable particles, certain amount of magnetizable particles had to be premixed to transmit the magnetic stabilization. Among others, the mere addition of magnetizable particles could broaden the homogeneous fluidization regime. The added content of magnetizable particles had an optimal value with smaller/lighter ones working better. The added magnetizable particles might raise the ratio between the interparticle force and the particle gravity. After the magnetic field was exerted, the homogeneous fluidization regime was further expanded due to the formation of magnetic stabilization flow regime. The more the added magnetizable particles, the better the magnetic performance and the broader the overall homogeneous fluidization regime. Smaller/lighter magnetizable particles were preferred to maximize the magnetic performance and extend the overall homogeneous fluidization regime. This phenomenon could be ascribed to that the added magnetizable particles themselves became more Geldart-A than -B type as their density or size decreased.

Kathon (CMI-MI), a mixture of 5-chloro-2-methyl-4-isothiazolin-3-one (CMI) and 2-methyl-4-isothiazolin-3-one (MI), was extensively used in industry as a nonoxidizing biocide or disinfectant. However, it would show adverse effects on aquatic life when it is discharged into surface water. In this study, the removal performance, parameter influence, degradation products and enhancement of subsequent biodegradation of CMI-MI in UV/H₂O₂ system were systematically investigated. The degradation rate of CMI-MI could reach 90% under UV irradiation for 20 min when the dosage of H₂O₂ was 0.3 mmol L^-1. The DOC (dissolved organic carbon) mineralization rate of CMI-MI could reach 35% under certain conditions ([H₂O₂]=0.3 mmol L^-1, UV irradiation for 40 min). k_obs was inversely proportional to the concentration of CMI-MI and proportional to the concentration of H₂O₂. The degradation rate of CMI-MI was almost unchanged in the pH range from 4 to 10. Except the presence of CO₃^2- inhibited the removal rate of CMI-MI, SO₄^2-, Cl^-, NO₃^-, and NH₄⁺ did not interfere with the degradation of CMI-MI in the system. It was found that UV/H₂O₂ system had lower energy consumption and more economic advantage compared with UV/PS system by comparing the E_EO (electric energy per order) values under the same conditions. Two main organic products were identified, namely HCOOH and CH₃NH₂. There's also the formation of Cl^- and SO₄^2-. After UV and UV/H₂O₂ photolysis, the biochemical properties of CMI-MI solution were obviously improved, especially the UV/H₂O₂ treatment effect was better, indicating that UV/H₂O₂ technology is expected to combine with biotechnology to remove CMI-MI effectively and environmentally friendly from wastewater.

Carbazole is an irreplaceable basic organic chemical raw material and intermediate in industry. The separation of carbazole from anthracene oil by environmental benign solvents is important but still a challenge in chemical engineering. Deep eutectic solvents (DESs) as a sustainable green separation solvent have been proposed for the separation of carbazole from model anthracene oil. In this research, three quaternary ammonium-based DESs were prepared using ethylene glycol (EG) as hydrogen bond donor and tetrabutylammonium chloride (TBAC), tetrabutylammonium bromide or choline chloride as hydrogen bond acceptors. To explore their extraction performance of carbazole, the conductor-like screening model for real solvents (COSMO-RS) model was used to predict the activity coefficient at infinite dilution (γ^∞) of carbazole in DESs, and the result indicated TBAC:EG (1:2) had the stronger extraction ability for carbazole due to the higher capacity at infinite dilution (C^∞) value. Then, the separation performance of these three DESs was evaluated by experiments, and the experimental results were in good agreement with the COSMO-RS prediction results. The TBAC:EG (1:2) was determined as the most promising solvent. Additionally, the extraction conditions of TBAC:EG (1:2) were optimized, and the extraction efficiency, distribution coefficient and selectivity of carbazole could reach up to 85.74%, 30.18 and 66.10%, respectively. Moreover, the TBAC:EG (1:2) could be recycled by using environmentally friendly water as antisolvent. In addition, the separation performance of TBAC:EG (1:2) was also evaluated by real crude anthracene, the carbazole was obtained with purity and yield of 85.32%, 60.27%, respectively. Lastly, the extraction mechanism was elucidated by σ-profiles and interaction energy analysis. Theoretical calculation results showed that the main driving force for the extraction process was the hydrogen bonding ((N-H…Cl) and van der Waals interactions (C-H…O and C-H…π), which corresponding to the blue and green isosurfaces in IGMH analysis. This work presented a novel method for separating carbazole from crude anthracene oil, and will provide an important reference for the separation of other high value-added products from coal tar.

Biochar and bio-oil are produced simultaneously in one pyrolysis process, and they inevitably contact and may interact, influencing the composition of bio-oil and modifying the structure of biochar. In this sense, biochar is an inherent catalyst for pyrolysis. In this study, in order to investigate the influence of functionalities and pore structures of biochar on its capability for catalyzing the conversion of homologous volatiles in bio-oil, three char catalysts (600C, 800C, and 800AC) produced via pyrolysis of poplar wood at 600 or 800 ℃ or activated at 800 ℃, were used for catalyzing pyrolysis of homologous poplar wood at 600 ℃, respectively. The results indicated that the 600C catalyst was more active than 800C and 800AC for catalyzing cracking of volatiles to form more gas (yield increase by 40.2%) and aromatization of volatiles to form more light or heavy phenolics, due to its abundant oxygen-containing functionalities acting as active sites. The developed pores of the 800AC showed no such catalytic effect but could trap some volatiles and allow their further conversion via sufficient aromatization. Nevertheless, the interaction with the volatiles consumed oxygen on 600C (decrease by 50%), enhancing the aromatic degree and increasing thermal stability. The dominance of deposition of carbonaceous material of a very aromatic nature over 800C and 800AC resulted in net weight gain and blocked micropores but formed additional macropores. The in situ diffuse reflectance infrared Fourier transform spectroscopy characterization of the catalytic pyrolysis indicated superior activity of 600C for removal of —OH, while conversion of the intermediates bearing C=O was enhanced over all the char catalysts.

Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide (SO₂) and nitrogen oxide (NO_x) emission control at low temperatures, especially for small and medium-sized coal-fired boilers and furnaces. Herein, phosphorus sludge, an industrial waste from the production process of yellow phosphorus, has been developed to simultaneously eliminate SO₂ and NO_x from coal-fired flue gas. The key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95% can be achieved at a low temperature of 55 ℃. Further, the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption process. The efficient removal of SO₂ is attributed to the abundance of iron (Fe³⁺) and manganese (Mn₂₊) in the absorbent. SO₂ can be rapidly catalyzed and converted to SO₄^2- by them. The key to NO_x removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus, which are then absorbed by water and converted to NO₃^-. Meanwhile, yellow phosphorus is oxidized to phosphoric acid (H₃PO₄). The spent absorption slurry can be reused through wet process phosphoric acid production, as it contains sulfuric acid (H₂SO₄), nitric acid (HNO₃), and H₃PO₄. Accordingly, this is a technology with broad application prospects.

The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry. In this study, a series of metal chloride-based ionic liquids were prepared and their performances in the separation of 1,2,3,4-tetrahydronaphthalene (tetralin)/dodecane and tetralin/decalin systems were studied. Among these ionic liquids, 1-ethyl-3-methylimidazolium tetrachloroferrate ([EMIM] [FeCl₄]) with the highest selectivity was used as the extractant. Density functional theory calculations showed that[EMIM] [FeCl₄] interacted more strongly with tetralin than with dodecane and decalin. Energy decomposition analysis of[EMIM] [FeCl₄]-tetralin indicated that electrostatics and dispersion played essential roles, and induction cannot be neglected. The van der Waals forces was a main effect in[EMIM] [FeCl₄] tetralin by independent gradient model analysis. The tetralin distribution coefficient and selectivity were 0.8 and 110, respectively, with 10% (mol) tetralin in the initial tetralin/dodecane system, and 0.67 and 19.5, respectively, with 10% (mol) tetralin in the initial tetralin/decalin system. The selectivity increased with decreasing alkyl chain length of the extractant. The influence of the extraction temperature, extractant dosage, and initial concentrations of the system components on the separation performance were studied. Recycling experiments showed that the regenerated[EMIM] [FeCl₄] could be used repeatedly.

Energetic nanofluid fuel has caught the attention of the field of aerospace liquid propellant for its high energy density (HED), but it suffers from the inevitable solideliquid phase separation problem. To resolve this problem, herein we synthesized the high-Al-/B-containing (up to 30% (mass)) HED gelled fuels, with low-molecular-mass organic gellant Z, which show high net heat of combustion (NHOC), density, storage stability, and thixotropic properties. The characterizations indicate that the application of energetic particles to the gelled fuels obviously destroys their fibrous network structures but can provide the new particleegellant gelation microstructures, resulting in the comparable stability between 1.0% (mass) Z/JP- 10 + 30% (mass) Al or B and pure JP-10 gelled fuel. Moreover, the gelled fuels with high-content Al or B exhibit high shear-thinning property, recovery capability, and mechanical strength, which are favorable for their storage and utilization. Importantly, the prepared 1.0% (mass) Z/JP-10 + 30% (mass) B (or 1.0% (mass) Z/JP-10 + 30% (mass) Al) shows the density and NHOC 1.27 times (1.30) and 1.43 times (1.21) higher than pure JP-10, respectively. This work provides a facile and valid approach to the manufacturing of HED gelled fuels with high content of energetic particles for gel propellants.

Due to a prolonged operation time and low mass transfer efficiency, the primary challenge in the aeration process of non-Newtonian fluids is the high energy consumption, which is closely related to the form and rate of impeller, ventilation, rheological properties and bubble morphology in the reactor. In this perspective, through optimal computational fluid dynamics models and experiments, the relationship between power consumption, volumetric mass transfer rate (k_La) and initial bubble size (d₀) was constructed to establish an efficient operation mode for the aeration process of non-Newtonian fluids. It was found that reducing the d₀ could significantly increase the oxygen mass transfer rate, resulting in an obvious decrease in the ventilation volume and impeller speed. When d₀ was regulated within 2-5 mm, an optimal k_La could be achieved, and 21% of power consumption could be saved, compared to the case of bubbles with a diameter of 10 mm.

Fouling caused by excess metal ions in hard water can negatively impact the performance of the circulating cooling water system (CCWS) by depositing ions on the heat exchanger's surface. Currently, the operation optimization of CCWS often prioritizes short-term flow velocity optimization for minimizing power consumption, without considering fouling. However, low flow velocity promotes fouling. Therefore, it's crucial to balance fouling and energy/water conservation for optimal CCWS long-term operation. This study proposes a mixed-integer nonlinear programming (MINLP) model to achieve this goal. The model considers fouling in the pipeline, dynamic concentration cycle, and variable frequency drive to optimize the synergy between heat transfer, pressure drop, and fouling. By optimizing the concentration cycle of the CCWS, water conservation and fouling control can be achieved. The model can obtain the optimal operating parameters for different operation intervals, including the number of pumps, frequency, and valve local resistance coefficient. Sensitivity experiments on cycle and environmental temperature reveal that as the cycle increases, the marginal benefits of energy/water conservation decrease. In periods with minimal impact on fouling rate, energy/water conservation can be achieved by increasing the cycle while maintaining a low fouling rate. Overall, the proposed model has significant energy/water saving effects and can comprehensively optimize the CCWS through its incorporation of fouling and cycle optimization.

Nitrogen electro-reduction under mild conditions is one promising alternative approach of the energyconsuming Haber-Bosch process for the artificial ammonia synthesis. One critical aspect to unlocking this technology is to discover the catalysts with high selectivity and efficiency. In this work, the N₂-to-NH₃ conversion on the functional MoS₂ is fully investigated by density functional theory calculations since the layered MoS₂ provides the ideal platform for the elaborating copies of the nitrogenase found in nature, wherein the functionalization is achieved via basal-adsorption, basal-substitution or edge-substitution of transition metal elements. Our results reveal that the edge-functionalization is a feasible strategy for the activity promotion; however, the basal-adsorption and basal-substitution separately suffer from the electrochemical instability and the NRR inefficiency. Specifically, MoS₂ functionalized via edge W-substitution exhibits an exceptional activity. The energetically favored reaction pathway is through the distal pathway and a limiting potential is less than 0.20 V. Overall, this work escalates the rational design of the high-effective catalysts for nitrogen fixation and provides the explanation why the predicated catalyst have a good performance, paving the guidance for the experiments.

Biocatalysis in organic solvents (OSs) has numerous important applications, but native enzymes in OSs often exhibit limited catalytic performance. Herein, we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface. Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue (Arg). Particularly, a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance (five-fold improvement in OS resistance and seven-fold half-life increase in 40% (vol) dimethylsulfoxide). As a result, the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA. Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a) improved the overall structural stability, (b) increased the hydrophobicity of the local microenvironment around the catalytic triad, (c) enriched the hydrophobic substrate around the enzyme molecule, and (d) lowered the contact frequency between OS molecules and the catalytic triad. Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.

In this study, the perovskite nanocomposite PrFe_xCo_1-xO₃(Pr(S)) was successfully synthesized by the sol -gel method; PrFe_xCo_1-xO₃/Al-pillared montmorillonite (Pr(S)/Mt) catalysts were prepared by impregnation (D) method and solid-melting (G) method, respectively, with Pr(S) as the active component and Al-pillared montmorillonite as the carrier. The catalysts were applied to treat the 2-hydroxybenzoic acid (2-HA)-simulated wastewater by catalytic wet peroxide oxidation (CWPO) technique, and the chemical oxygen demand (COD) removal rate and the 2-HA degradation rate were used as indicators to evaluate the catalytic performance. The results of the experiment indicated that the solid-melting method was more conducive to preparing the catalyst when the Co/Fe molar ratio of 7:3 and the optimal structural properties of the catalysts were achieved. The influence of operating parameters, including reaction temperature, catalyst dosage, H₂O₂ dosage, pH, and initial 2-HA concentration, were optimized for the degradation of 2-HA by CWPO. The results showed that 97.64% of 2-HA degradation and 75.23% of COD removal rate were achieved under more suitable experimental conditions. In addition, after the catalyst was used five times, the degradation rate of 2-HA could still reach 76.93%, which implied the high stability and reusability of the catalyst. The high catalytic activity of the catalyst was due to the doping of Co into PrFeO₃, which could promote the generation of HO·, and the high stability could be attributed to the loading of Pr(S) onto Al-Mt, which reduced the leaching of reactive metals. The study of reaction mechanism and kinetics showed that the whole degradation process conformed to the pseudo-firs-torder kinetic equation, and the Langmuir-Hinshelwood method was applied to demonstrate that catalysis was dominant in the degradation process.