A simple condensation afforded some new 3-thioxo-1,2,4-triazin-5-one derivatives (4, 6 and 8). Utilizing a facile condensation of (E)-4-(4’-bromo styryl)-2-oxo-3-buteneoic acid with thiosemicarbazide, dithioic formic...A simple condensation afforded some new 3-thioxo-1,2,4-triazin-5-one derivatives (4, 6 and 8). Utilizing a facile condensation of (E)-4-(4’-bromo styryl)-2-oxo-3-buteneoic acid with thiosemicarbazide, dithioic formic acid hydrazide, and thiocarbahydrazide in different conditions. Structures of these compounds were confirmed by elemental and spectral analysis. The preliminary biocidal activity of these products were evaluated against some microbial and compared to Mycostatine and piperacillin as antibiotics were most of derivatives exhibited good activity.展开更多
Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthfield,and environmentalfield,and recen...Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthfield,and environmentalfield,and recently applied in energy storage.Seed-assisted synthesis is a very effective approach in promoting the crystallization of zeolites.In some cases,the target zeolite cannot be formed in the absence of seed zeolite.In homologous seed-assisted synthesis,the structure of the seed zeolite is the same to that of the target zeolite,while the structure of the seed zeolite is different to that of the target zeolite in the heterologous seed-assisted synthesis.In this review,we briefly summarized the heterologous seed-assisted syntheses of zeolites and analyzed the structure-directing effect of heterologous seeds and surveyed the“common composite building units(CBUs)hypothesis”and the“common secondary building units(SBUs)hypothesis”.However,both hypotheses cannot explain all observations on the heterologous seed-assisted syntheses.Finally,we proposed that the formation of the target zeolite does need nuclei with the structure of target zeolite and the formation of the nuclei of the target zeolite can be promoted by either the undissolved seed crystals with the same CBUs or SBUs to the target zeolite or by the facilitated appropriate distribution of the specific building units due to the presence of the heterologous seed that does not have any common CBUs and SBUs with the target zeolite.展开更多
Transition metal phosphides(TMPs)have been regarded as alternative hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts owing to their comparable activity to those of noble metal-based catalysts...Transition metal phosphides(TMPs)have been regarded as alternative hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts owing to their comparable activity to those of noble metal-based catalysts.TMPs have been produced in various morphologies,including hollow and porous nanostructures,which are features deemed desirable for electrocatalytic materials.Templated synthesis routes are often responsible for such morphologies.This paper reviews the latest advances and existing challenges in the synthesis of TMP-based OER and HER catalysts through templated methods.A comprehensive review of the structure-property-performance of TMP-based HER and OER catalysts prepared using different templates is presented.The discussion proceeds according to application,first by HER and further divided among the types of templates used-from hard templates,sacrificial templates,and soft templates to the emerging dynamic hydrogen bubble template.OER catalysts are then reviewed and grouped according to their morphology.Finally,prospective research directions for the synthesis of hollow and porous TMP-based catalysts,such as improvements on both activity and stability of TMPs,design of environmentally benign templates and processes,and analysis of the reaction mechanism through advanced material characterization techniques and theoretical calculations,are suggested.展开更多
Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sit...Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst.展开更多
Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption...Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption and waste gas emissions.To address this,electrocatalytic nitric oxide reduction reaction(NORR)has emerged as a promising strategy to bridge NH3consumption to NH3production,harnessing renewable electricity for a sustainable future.Copper(Cu)stands out as a prominent electrocatalyst for NO reduction,given its exceptional NH3yield and selectivity.However,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR performance.In this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cathodes through an in situ growth method.Remarkably,CuO-NF exhibited an impressive NH3yield of 0.50±0.02 mg cm^(-2)h^(-1)at-0.6 V vs.reversible hydrogen electrode(RHE)with faradaic efficiency of29,68%±1,35%,surpassing that of Cu-NF(0.17±0.01 mg cm^(-2)h^(-1),16.18%±1.40%).Throughout the electroreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ensued.Conversely,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same timeframe.The distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation mechanisms.Further Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44×10^(-6)A cm^(-2)and 3.77×10^(-6)cm^(-2)s^(-1)when NORR was driven by overpotentials.These findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance.展开更多
Molybdenum disulfide(MoS_(2))has garnered significant attention in the field of catalysis due to the high density of active sites in its unique two-dimensional(2D)structure,which could be developed into numerous high-...Molybdenum disulfide(MoS_(2))has garnered significant attention in the field of catalysis due to the high density of active sites in its unique two-dimensional(2D)structure,which could be developed into numerous high-performance catalysts.The synthesis of ultra-small MoS2 particles(<10 nm)is highly desired in various experimental studies.The ultra-small structure could often lead to a distinct S-Mo coordination state and nonstoichiometric composition in MoSx,minimizing in-plane active sites of the 2D structure and making it probable to regulate the atomic and electronic structure of its intrinsic active sites on a large extent,especially in MoSx clusters.This article summarizes the recent progress of catalysis over ultra-small undoped MoS_(2) particles for renewable fuel production.Through a systematic review of their synthesis,structural,and spectral characteristics,as well as the relationship between their catalytic performance and inherent defects,we aim to provide insights into catalysis over this matrix that may potentially enable advancement in the development of high-performance MoS_(2)-based catalysts for sustainable energy generation in the future.展开更多
In order to improve the energy output consistency of 3, 3’-diamino-4, 4’-azoxyfurazan(DAAF) in the new insensitive booster and the safety and efficiency in the preparation process, a continuous preparation system of...In order to improve the energy output consistency of 3, 3’-diamino-4, 4’-azoxyfurazan(DAAF) in the new insensitive booster and the safety and efficiency in the preparation process, a continuous preparation system of DAAF from synthesis to spherical coating was designed and established in this paper, which combined ultrasonic micromixing reaction with microdroplet globular template. In the rapid micromixing stage, the microfluidic mixing technology with ultrasonic was used to synergistically strengthen the uniform and rapid mass transfer mixing reaction between raw materials to ensure the uniformity of DAAF particle nucleation-growth, and to prepare high-quality DAAF crystals with uniform structure and morphology and concentrated particle size distribution. In the microdroplet globular template stage, the microfluidic droplet technology was used to form a droplet globular template with uniform size under the shear action of the continuous phase of the dispersed phase solution containing DAAF particles and binder. The size of the droplet template was controlled by adjusting the flow rate ratio between the continuous phase and the dispersed phase. In the droplet globular template, with the diffusion of the solvent in the dispersed phase droplets, the binder precipitates to coat the DAAF into a ball, forming a DAAF microsphere with high sphericity, narrow particle size distribution and good monodispersity. The problem of discontinuity and DAAF particle suspension in the process was solved, and the coating theory under this process was studied. DAAF was coated with different binder formulations of fluororubber(F2604), nitrocellulose(NC) and NC/glycidyl azide polymer(GAP), and the process verification and evaluation of the system were carried out. The balling effects of large, medium and small droplet templates under different binder formulations were studied. The scanning electron microscope(SEM) results show that the three droplet templates under the three binder formulations exhibit good balling effect and narrow particle size distribution. The DAAF microspheres were characterized by powder X-ray diffraction(XRD), differential scanning calorimetry(DSC), thermo-gravimetric(TG) and sensitivity analyzer. The results showed that the crystal structure of DAAF did not change during the process, and the prepared DAAF microspheres had lower decomposition temperature and lower mechanical sensitivity than raw DAAF. The results of detonation parameters show that the coating of DAAF by using the above three binder formulations will not greatly reduce the energy output of DAAF, and has comparable detonation performance to raw DAAF. This study proves an efficient and safe continuous system from synthesis to spherical coating modification of explosives, which provides a new way for the continuous, safe and efficient preparation of spherical explosives.展开更多
The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia syn...The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.展开更多
The Cs_(2)NaInCl_(6)double perovskite is one of the most promising lead-free perovskites due to its exceptional stability and straightforward synthesis.However,it faces challenges related to inefficient photoluminesce...The Cs_(2)NaInCl_(6)double perovskite is one of the most promising lead-free perovskites due to its exceptional stability and straightforward synthesis.However,it faces challenges related to inefficient photoluminescence.Doping and high pressure are employed to tailor the optical properties of Cs_(2)NaInCl_(6).Herein,Sb^(3+)doped Cs_(2)NaInCl_(6)(Sb^(3+):Cs_(2)NaInCl_(6))was synthesized and it exhibits blue emission with a photoluminescence quantum yield of up to 37.3%.Further,by employing pressure tuning,a blue stable emission under a very wide range from 2.7 GPa to 9.8 GPa is realized in Sb^(3+):Cs_(2)NaInCl_(6).Subsequently,the emission intensity of Sb^(3+):Cs_(2)NaInCl_(6)experiences a significant increase(3.3 times)at 19.0 GPa.It is revealed that the pressure-induced distinct emissions can be attributed to the carrier self-trapping and detrapping between Cs_(2)NaInCl_(6)and Sb^(3+).Notably,the lattice compression in the cubic phase inevitably modifies the band gap of Sb^(3+):Cs_(2)NaInCl_(6).Our findings provide valuable insights into effects of the high pressure in further boosting unique emission characteristics but also offer promising opportunities for development of doped double perovskites with enhanced optical functionalities.展开更多
MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical str...MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical strength,etc.This review begins by presenting MXenes,providing insights into their structural characteristics,synthesis methods,and surface functional groups.The review covers a thorough analysis of MXene surface properties,including surface chemistry and termination group impacts.The properties of MXenes are influenced by their synthesis,which can be fluorine-based or fluorinedependent.Fluorine-based synthesis techniques involve etching with fluorine-based reagents,mainly including HF or LiF/HCl,while fluorine-free methods include electrochemical etching,chemical vapor deposition(CVD),alkaline etching,Lewis acid-based etching,etc.These techniques result in the emergence of functional groups such as-F,-O,-OH,-Cl,etc.on the MXenes surface,depending on the synthesis method used.Properties of MXenes,such as electrical conductivity,electronic properties,catalytic activity,magnetic properties,mechanical strength,and chemical and thermal stability,are examined,and the role of functional groups in determining these properties is explored.The review delves into the diverse applications of MXenes,encompassing supercapacitors,battery materials,hydrogen storage,fuel cells,electromagnetic interference(EMI) shielding,pollutant removal,water purification,flexible electronics,sensors,additive manufacturing,catalysis,biomedical and healthcare fields,etc.Finally,this article outlines the challenges and opportunities in the current and future development of MXenes research,addressing various aspects such as synthesis scalability,etching challenges,and multifunctionality,and exploring novel applications.The review concludes with future prospects and conclusions envisioning the impact of MXenes on future technologies and innovation.展开更多
MXene has been the limelight for studies on electrode active materials,aiming at developing supercapacitors with boosted energy density to meet the emerging influx of wearable and portable electronic devices.Despite i...MXene has been the limelight for studies on electrode active materials,aiming at developing supercapacitors with boosted energy density to meet the emerging influx of wearable and portable electronic devices.Despite its various desirable properties including intrinsic flexibility,high specific surface area,excellent metallic conductivity and unique abundance of surface functionalities,its full potential for electrochemical performance is hindered by the notorious restacking phenomenon of MXene nanosheets.Ascribed to its two-dimensional(2D)nature and surface functional groups,inevitable Van der Waals interactions drive the agglomeration of nanosheets,ultimately reducing the exposure of electrochemically active sites to the electrolyte,as well as severely lengthening electrolyte ion transport pathways.As a result,energy and power density deteriorate,limiting the application versatility of MXene-based supercapacitors.Constructing 3D architectures using 2D nanosheets presents as a straightforward yet ingenious approach to mitigate the fatal flaws of MXene.However,the sheer number of distinct methodologies reported,thus far,calls for a systematic review that unravels the rationale behind such 3D MXene structural designs.Herein,this review aims to serve this purpose while also scrutinizing the structure–property relationship to correlate such structural modifications to their ensuing electrochemical performance enhancements.Besides,the physicochemical properties of MXene play fundamental roles in determining the effective charge storage capabilities of 3D MXene-based electrodes.This largely depends on different MXene synthesis techniques and synthesis condition variations,hence,elucidated in this review as well.Lastly,the challenges and perspectives for achieving viable commercialization of MXene-based supercapacitor electrodes are highlighted.展开更多
The use of hybrid wheat is one way to improve the yield in the future.However,greater plant heights increase lodging risk to some extent.In this study,two hybrid combinations with differences in lodging resistance wer...The use of hybrid wheat is one way to improve the yield in the future.However,greater plant heights increase lodging risk to some extent.In this study,two hybrid combinations with differences in lodging resistance were used to analyze the stem-related traits during the filling stage,and to investigate the mechanism of the difference in lodging resistance by analyzing lignin synthesis of the basal second internode(BSI).The stem-related traits such as the breaking strength,stem pole substantial degree(SPSD),and rind penetration strength(RPS),as well as the lignin content of the lodging-resistant combination(LRC),were significantly higher than those of the lodgingsensitive combination(LSC).The phenylpropanoid biosynthesis pathway was significantly and simultaneously enriched according to the transcriptomics and metabolomics analysis at the later filling stage.A total of 35 critical regulatory genes involved in the phenylpropanoid pathway were identified.Moreover,42%of the identified genes were significantly and differentially expressed at the later grain-filling stage between the two combinations,among which more than 80%were strongly up-regulated at that stage in the LRC compared with LSC.On the contrary,the LRC displayed lower contents of lignin intermediate metabolites than the LSC.These results suggested that the key to the lodging resistance formation of LRC is largely the higher lignin synthesis at the later grain-filling stage.Finally,breeding strategies for synergistically improving plant height and lodging resistance of hybrid wheat were put forward by comparing the LRC with the conventional wheat applied in large areas.展开更多
The Gibberellic Acid-stimulated Arabidopsis(GASA)gene family is involved in the regulation of gene expression and plant growth,development,and stress responses.To investigate the function of loquat GASA genes in the g...The Gibberellic Acid-stimulated Arabidopsis(GASA)gene family is involved in the regulation of gene expression and plant growth,development,and stress responses.To investigate the function of loquat GASA genes in the growth and developmental regulation of plants,a loquat EjGASA6 gene homologous to Arabidopsis AtGASA6 was cloned.EjGASA6 expression was induced by gibberellin,and ectopic transgenic plants containing this gene exhibited earlier bloom and longer primary roots since these phenotypic characteristics are related to higher gibberellin content.Transcriptome analysis and qRT-PCR results showed that the expression levels of GA3ox1 and GA20ox1,which encode key enzymes in gibberellin biosynthesis,were significantly increased.Furthermore,we confirmed that EjGASA6 could promote the expression of GA20ox1 via the luciferase reporter system.Overall,our results suggest that EjGASA6 promotes blooming and main-root elongation by positively regulating gibberellin biosynthesis.These findings broaden our understanding of the role of GASAs in plant development and growth,and lay the groundwork for future research into the functions of EjGASA6 in regulating loquat growth and development.展开更多
Two-dimensional(2D)magnetic materials have been demonstrated to have excellent chemical,optical,electrical,and magnetic properties,particularly in the development of multifunctional electronic and spin electronic devi...Two-dimensional(2D)magnetic materials have been demonstrated to have excellent chemical,optical,electrical,and magnetic properties,particularly in the development of multifunctional electronic and spin electronic devices,showcasing tremendous potential.Therefore,corresponding synthesis techniques for 2D magnetic materials that offer high quality,high yield,low cost,time-saving,and simplicity are highly desired.This review provides a comprehensive overview of recent research advances in preparation of magnetic 2D materials,with a particular focus on the preparation methods employed.Moreover,the characteristics and applications of these magnetic materials are also discussed.Finally,the challenges and prospects of synthesis methods for magnetic 2D materials are briefly addressed.This review serves as a guiding reference for the controlled synthesis of 2D magnetic materials.展开更多
In the realm of the synthesis of heat-integrated distillation configurations,the conventional approach for exploring more heat integration possibilities typically entails the splitting of a single column into a twocol...In the realm of the synthesis of heat-integrated distillation configurations,the conventional approach for exploring more heat integration possibilities typically entails the splitting of a single column into a twocolumn configuration.However,this approach frequently necessitates tedious enumeration procedures,resulting in a considerable computational burden.To surmount this formidable challenge,the present study introduces an innovative remedy:The proposition of a superstructure that encompasses both single-column and multiple two-column configurations.Additionally,a simultaneous optimization algorithm is applied to optimize both the process parameters and heat integration structures of the twocolumn configurations.The effectiveness of this approach is demonstrated through a case study focusing on industrial organosilicon separation.The results underscore that the superstructure methodology not only substantially mitigates computational time compared to exhaustive enumeration but also furnishes solutions that exhibit comparable performance.展开更多
The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challen...The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.展开更多
Titanium matrix composites reinforced with ceramic particles are considered a promising engineering material due to their combination of high specific strength,low density,and high modulus.In this study,the TA15-based...Titanium matrix composites reinforced with ceramic particles are considered a promising engineering material due to their combination of high specific strength,low density,and high modulus.In this study,the TA15-based composites reinforced with a volume fraction of 10% to 25%(TiB+TiC)were prepared using powder metallurgy and casting technique.Microstructural characterization and phase constitution were examined using optical microscopy(OM),scanning electron microscopy(SEM),and X-ray diffraction(XRD).In addition,the microhardness,room temperature(RT)and high temperature(HT)tensile properties of the composites were evaluated.Results revealed that the reinforcements are distributed uniformly even in the composites with a high volume of TiB and TiC.However,as the volume fraction exceeds 15%,TiB and TiC particles become coarsening and exhibit rod-like and dendritic-like morphology.Microhardness increases gradually from 321.2 HV for the base alloy to a maximum of 473.3 HV as the reinforcement increases to 25vol.%.Tensile test results indicate that a reinforcement volume fraction above 20% is beneficial for enhancing tensile strength and yield strength at high temperatures,but it has an adverse effect on room temperature elongation.Conversely,if the reinforcement volume fraction is below 20%,it can improve high-temperature elongation when the temperature exceeds 600℃.展开更多
Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the...Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.展开更多
Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-...Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.展开更多
A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal cry...A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composition and synthesis conditions.Characterizations show that Fe ZSM-22 zeolite synthesized with OSDA-free owns high crystallinity,obvious thin needle-shaped morphology and high Bronsted/Lewis acid ratio.Significantly,when used for n-octane hydroisomerization reaction,its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C_(8)isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals,respectively.This work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance.展开更多
文摘A simple condensation afforded some new 3-thioxo-1,2,4-triazin-5-one derivatives (4, 6 and 8). Utilizing a facile condensation of (E)-4-(4’-bromo styryl)-2-oxo-3-buteneoic acid with thiosemicarbazide, dithioic formic acid hydrazide, and thiocarbahydrazide in different conditions. Structures of these compounds were confirmed by elemental and spectral analysis. The preliminary biocidal activity of these products were evaluated against some microbial and compared to Mycostatine and piperacillin as antibiotics were most of derivatives exhibited good activity.
基金support from the National Key Research and Development Program of China(2021YFA1500401,2021YFA1501202)the National Natural Science Foundation of China(22288101)the 111 Project(B17020)for supporting this work.
文摘Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthfield,and environmentalfield,and recently applied in energy storage.Seed-assisted synthesis is a very effective approach in promoting the crystallization of zeolites.In some cases,the target zeolite cannot be formed in the absence of seed zeolite.In homologous seed-assisted synthesis,the structure of the seed zeolite is the same to that of the target zeolite,while the structure of the seed zeolite is different to that of the target zeolite in the heterologous seed-assisted synthesis.In this review,we briefly summarized the heterologous seed-assisted syntheses of zeolites and analyzed the structure-directing effect of heterologous seeds and surveyed the“common composite building units(CBUs)hypothesis”and the“common secondary building units(SBUs)hypothesis”.However,both hypotheses cannot explain all observations on the heterologous seed-assisted syntheses.Finally,we proposed that the formation of the target zeolite does need nuclei with the structure of target zeolite and the formation of the nuclei of the target zeolite can be promoted by either the undissolved seed crystals with the same CBUs or SBUs to the target zeolite or by the facilitated appropriate distribution of the specific building units due to the presence of the heterologous seed that does not have any common CBUs and SBUs with the target zeolite.
基金the support from the CIPHER Project(IIID 2018-008)funded by the Commission on Higher Education-Philippine California Advanced Research Institutes(CHED-PCARI)。
文摘Transition metal phosphides(TMPs)have been regarded as alternative hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts owing to their comparable activity to those of noble metal-based catalysts.TMPs have been produced in various morphologies,including hollow and porous nanostructures,which are features deemed desirable for electrocatalytic materials.Templated synthesis routes are often responsible for such morphologies.This paper reviews the latest advances and existing challenges in the synthesis of TMP-based OER and HER catalysts through templated methods.A comprehensive review of the structure-property-performance of TMP-based HER and OER catalysts prepared using different templates is presented.The discussion proceeds according to application,first by HER and further divided among the types of templates used-from hard templates,sacrificial templates,and soft templates to the emerging dynamic hydrogen bubble template.OER catalysts are then reviewed and grouped according to their morphology.Finally,prospective research directions for the synthesis of hollow and porous TMP-based catalysts,such as improvements on both activity and stability of TMPs,design of environmentally benign templates and processes,and analysis of the reaction mechanism through advanced material characterization techniques and theoretical calculations,are suggested.
基金supported by China National Natural Science Foundation(22008260,21908123)。
文摘Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst.
基金supported by the Fundamental Research Funds for the Central Universities(FRF-EYIT-23-07)。
文摘Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption and waste gas emissions.To address this,electrocatalytic nitric oxide reduction reaction(NORR)has emerged as a promising strategy to bridge NH3consumption to NH3production,harnessing renewable electricity for a sustainable future.Copper(Cu)stands out as a prominent electrocatalyst for NO reduction,given its exceptional NH3yield and selectivity.However,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR performance.In this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cathodes through an in situ growth method.Remarkably,CuO-NF exhibited an impressive NH3yield of 0.50±0.02 mg cm^(-2)h^(-1)at-0.6 V vs.reversible hydrogen electrode(RHE)with faradaic efficiency of29,68%±1,35%,surpassing that of Cu-NF(0.17±0.01 mg cm^(-2)h^(-1),16.18%±1.40%).Throughout the electroreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ensued.Conversely,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same timeframe.The distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation mechanisms.Further Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44×10^(-6)A cm^(-2)and 3.77×10^(-6)cm^(-2)s^(-1)when NORR was driven by overpotentials.These findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance.
基金support from the Tangshan Talent Funding Project(A202202007)the National Natural Science Foundation of China(21703065)+1 种基金the Natural Science Foundation of Hebei Province(B2018209267,E2022209039)the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(51888103).
文摘Molybdenum disulfide(MoS_(2))has garnered significant attention in the field of catalysis due to the high density of active sites in its unique two-dimensional(2D)structure,which could be developed into numerous high-performance catalysts.The synthesis of ultra-small MoS2 particles(<10 nm)is highly desired in various experimental studies.The ultra-small structure could often lead to a distinct S-Mo coordination state and nonstoichiometric composition in MoSx,minimizing in-plane active sites of the 2D structure and making it probable to regulate the atomic and electronic structure of its intrinsic active sites on a large extent,especially in MoSx clusters.This article summarizes the recent progress of catalysis over ultra-small undoped MoS_(2) particles for renewable fuel production.Through a systematic review of their synthesis,structural,and spectral characteristics,as well as the relationship between their catalytic performance and inherent defects,we aim to provide insights into catalysis over this matrix that may potentially enable advancement in the development of high-performance MoS_(2)-based catalysts for sustainable energy generation in the future.
基金National Natural Science Foundation of China(Grant No.22005275)to provide fund for conducting experiments.
文摘In order to improve the energy output consistency of 3, 3’-diamino-4, 4’-azoxyfurazan(DAAF) in the new insensitive booster and the safety and efficiency in the preparation process, a continuous preparation system of DAAF from synthesis to spherical coating was designed and established in this paper, which combined ultrasonic micromixing reaction with microdroplet globular template. In the rapid micromixing stage, the microfluidic mixing technology with ultrasonic was used to synergistically strengthen the uniform and rapid mass transfer mixing reaction between raw materials to ensure the uniformity of DAAF particle nucleation-growth, and to prepare high-quality DAAF crystals with uniform structure and morphology and concentrated particle size distribution. In the microdroplet globular template stage, the microfluidic droplet technology was used to form a droplet globular template with uniform size under the shear action of the continuous phase of the dispersed phase solution containing DAAF particles and binder. The size of the droplet template was controlled by adjusting the flow rate ratio between the continuous phase and the dispersed phase. In the droplet globular template, with the diffusion of the solvent in the dispersed phase droplets, the binder precipitates to coat the DAAF into a ball, forming a DAAF microsphere with high sphericity, narrow particle size distribution and good monodispersity. The problem of discontinuity and DAAF particle suspension in the process was solved, and the coating theory under this process was studied. DAAF was coated with different binder formulations of fluororubber(F2604), nitrocellulose(NC) and NC/glycidyl azide polymer(GAP), and the process verification and evaluation of the system were carried out. The balling effects of large, medium and small droplet templates under different binder formulations were studied. The scanning electron microscope(SEM) results show that the three droplet templates under the three binder formulations exhibit good balling effect and narrow particle size distribution. The DAAF microspheres were characterized by powder X-ray diffraction(XRD), differential scanning calorimetry(DSC), thermo-gravimetric(TG) and sensitivity analyzer. The results showed that the crystal structure of DAAF did not change during the process, and the prepared DAAF microspheres had lower decomposition temperature and lower mechanical sensitivity than raw DAAF. The results of detonation parameters show that the coating of DAAF by using the above three binder formulations will not greatly reduce the energy output of DAAF, and has comparable detonation performance to raw DAAF. This study proves an efficient and safe continuous system from synthesis to spherical coating modification of explosives, which provides a new way for the continuous, safe and efficient preparation of spherical explosives.
基金the Science and Engineering Research Board(SERB),Government of India for funding this work(Sanction No.EEQ/2021/001116)。
文摘The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.
基金supported by the National Key Research and Development Program of China(Grant Nos.2021YFA1400200 and2021YFA0718701)the National Natural Science Foundation of China(Grant Nos.U2032127,11904322,12104411,12174347)+4 种基金the Natural Science Foundation of Henan province of China(Grant No.202300410356)the China Postdoctoral Science Foundation(Grant Nos.2019M652560 and 2020M682326)the CAS Interdisciplinary Innovation Team(Grant No.JCTD-2019-01)the Postdoctoral Research Grant in Henan Province(Grant No.1902013)the Science Foundation for Highlevel Talents of Wuyi University(Grant No.2021AL019)。
文摘The Cs_(2)NaInCl_(6)double perovskite is one of the most promising lead-free perovskites due to its exceptional stability and straightforward synthesis.However,it faces challenges related to inefficient photoluminescence.Doping and high pressure are employed to tailor the optical properties of Cs_(2)NaInCl_(6).Herein,Sb^(3+)doped Cs_(2)NaInCl_(6)(Sb^(3+):Cs_(2)NaInCl_(6))was synthesized and it exhibits blue emission with a photoluminescence quantum yield of up to 37.3%.Further,by employing pressure tuning,a blue stable emission under a very wide range from 2.7 GPa to 9.8 GPa is realized in Sb^(3+):Cs_(2)NaInCl_(6).Subsequently,the emission intensity of Sb^(3+):Cs_(2)NaInCl_(6)experiences a significant increase(3.3 times)at 19.0 GPa.It is revealed that the pressure-induced distinct emissions can be attributed to the carrier self-trapping and detrapping between Cs_(2)NaInCl_(6)and Sb^(3+).Notably,the lattice compression in the cubic phase inevitably modifies the band gap of Sb^(3+):Cs_(2)NaInCl_(6).Our findings provide valuable insights into effects of the high pressure in further boosting unique emission characteristics but also offer promising opportunities for development of doped double perovskites with enhanced optical functionalities.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2020R1A6A1A03043435 and 2020R1A2C1099862)supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(P0012451,The Competency Development Program for Industry Specialist)。
文摘MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical strength,etc.This review begins by presenting MXenes,providing insights into their structural characteristics,synthesis methods,and surface functional groups.The review covers a thorough analysis of MXene surface properties,including surface chemistry and termination group impacts.The properties of MXenes are influenced by their synthesis,which can be fluorine-based or fluorinedependent.Fluorine-based synthesis techniques involve etching with fluorine-based reagents,mainly including HF or LiF/HCl,while fluorine-free methods include electrochemical etching,chemical vapor deposition(CVD),alkaline etching,Lewis acid-based etching,etc.These techniques result in the emergence of functional groups such as-F,-O,-OH,-Cl,etc.on the MXenes surface,depending on the synthesis method used.Properties of MXenes,such as electrical conductivity,electronic properties,catalytic activity,magnetic properties,mechanical strength,and chemical and thermal stability,are examined,and the role of functional groups in determining these properties is explored.The review delves into the diverse applications of MXenes,encompassing supercapacitors,battery materials,hydrogen storage,fuel cells,electromagnetic interference(EMI) shielding,pollutant removal,water purification,flexible electronics,sensors,additive manufacturing,catalysis,biomedical and healthcare fields,etc.Finally,this article outlines the challenges and opportunities in the current and future development of MXenes research,addressing various aspects such as synthesis scalability,etching challenges,and multifunctionality,and exploring novel applications.The review concludes with future prospects and conclusions envisioning the impact of MXenes on future technologies and innovation.
基金supported by the Fundamental Research Grant Scheme by Ministry of Higher Education Malaysia(FRGS/1/2021/STG04/XMU/02/1 and FRGS/1/2022/TK09/XMU/03/2)the Xiamen University Malaysia Research Fund(XMUMRF/2023-C11/IENG/0056)。
文摘MXene has been the limelight for studies on electrode active materials,aiming at developing supercapacitors with boosted energy density to meet the emerging influx of wearable and portable electronic devices.Despite its various desirable properties including intrinsic flexibility,high specific surface area,excellent metallic conductivity and unique abundance of surface functionalities,its full potential for electrochemical performance is hindered by the notorious restacking phenomenon of MXene nanosheets.Ascribed to its two-dimensional(2D)nature and surface functional groups,inevitable Van der Waals interactions drive the agglomeration of nanosheets,ultimately reducing the exposure of electrochemically active sites to the electrolyte,as well as severely lengthening electrolyte ion transport pathways.As a result,energy and power density deteriorate,limiting the application versatility of MXene-based supercapacitors.Constructing 3D architectures using 2D nanosheets presents as a straightforward yet ingenious approach to mitigate the fatal flaws of MXene.However,the sheer number of distinct methodologies reported,thus far,calls for a systematic review that unravels the rationale behind such 3D MXene structural designs.Herein,this review aims to serve this purpose while also scrutinizing the structure–property relationship to correlate such structural modifications to their ensuing electrochemical performance enhancements.Besides,the physicochemical properties of MXene play fundamental roles in determining the effective charge storage capabilities of 3D MXene-based electrodes.This largely depends on different MXene synthesis techniques and synthesis condition variations,hence,elucidated in this review as well.Lastly,the challenges and perspectives for achieving viable commercialization of MXene-based supercapacitor electrodes are highlighted.
基金supported by the Youth Fund Project from Beijing Academy of Agricultural and Forestry Sciences China(QNJJ202225)the Germplasm Innovation and New Variety Breeding Project of Beijing China(G20220628002)the Training Programme Foundation for the Beijing Municipal Excellent Talents China(2017000020060G130)。
文摘The use of hybrid wheat is one way to improve the yield in the future.However,greater plant heights increase lodging risk to some extent.In this study,two hybrid combinations with differences in lodging resistance were used to analyze the stem-related traits during the filling stage,and to investigate the mechanism of the difference in lodging resistance by analyzing lignin synthesis of the basal second internode(BSI).The stem-related traits such as the breaking strength,stem pole substantial degree(SPSD),and rind penetration strength(RPS),as well as the lignin content of the lodging-resistant combination(LRC),were significantly higher than those of the lodgingsensitive combination(LSC).The phenylpropanoid biosynthesis pathway was significantly and simultaneously enriched according to the transcriptomics and metabolomics analysis at the later filling stage.A total of 35 critical regulatory genes involved in the phenylpropanoid pathway were identified.Moreover,42%of the identified genes were significantly and differentially expressed at the later grain-filling stage between the two combinations,among which more than 80%were strongly up-regulated at that stage in the LRC compared with LSC.On the contrary,the LRC displayed lower contents of lignin intermediate metabolites than the LSC.These results suggested that the key to the lodging resistance formation of LRC is largely the higher lignin synthesis at the later grain-filling stage.Finally,breeding strategies for synergistically improving plant height and lodging resistance of hybrid wheat were put forward by comparing the LRC with the conventional wheat applied in large areas.
基金financially supported by the National Key R&D Program of China (2023YFD1600800)the National Nature Science Foundation of China (32102321)+4 种基金the Chongqing Science and Technology Commission, China (cstc2024ycjh-bgzxm0202, cstc2021jscx-gksbX0010 and cstc2021jcyj-msxmX1156)the Chongqing Forestry Administration, China (YuLinKeYan2022-14)the Innovation Research Group Funds for Chongqing Universities, China (CXQT19005)the Characteristic Fruit Industry and Technology System Innovation Team of Chongqing Agriculture and Rural Affairs Commission, China [(2022)164 and 2020(3)01]the Chongqing Postgraduate Research and Innovation Programme, China (CYB23128)
文摘The Gibberellic Acid-stimulated Arabidopsis(GASA)gene family is involved in the regulation of gene expression and plant growth,development,and stress responses.To investigate the function of loquat GASA genes in the growth and developmental regulation of plants,a loquat EjGASA6 gene homologous to Arabidopsis AtGASA6 was cloned.EjGASA6 expression was induced by gibberellin,and ectopic transgenic plants containing this gene exhibited earlier bloom and longer primary roots since these phenotypic characteristics are related to higher gibberellin content.Transcriptome analysis and qRT-PCR results showed that the expression levels of GA3ox1 and GA20ox1,which encode key enzymes in gibberellin biosynthesis,were significantly increased.Furthermore,we confirmed that EjGASA6 could promote the expression of GA20ox1 via the luciferase reporter system.Overall,our results suggest that EjGASA6 promotes blooming and main-root elongation by positively regulating gibberellin biosynthesis.These findings broaden our understanding of the role of GASAs in plant development and growth,and lay the groundwork for future research into the functions of EjGASA6 in regulating loquat growth and development.
基金supported by the National Natural Science Foundation of China(Grant Nos.22175060 and 21975067)the Natural Science Foundation of Hunan Province of China(Grant Nos.2021JJ10014 and 2021JJ30092).
文摘Two-dimensional(2D)magnetic materials have been demonstrated to have excellent chemical,optical,electrical,and magnetic properties,particularly in the development of multifunctional electronic and spin electronic devices,showcasing tremendous potential.Therefore,corresponding synthesis techniques for 2D magnetic materials that offer high quality,high yield,low cost,time-saving,and simplicity are highly desired.This review provides a comprehensive overview of recent research advances in preparation of magnetic 2D materials,with a particular focus on the preparation methods employed.Moreover,the characteristics and applications of these magnetic materials are also discussed.Finally,the challenges and prospects of synthesis methods for magnetic 2D materials are briefly addressed.This review serves as a guiding reference for the controlled synthesis of 2D magnetic materials.
文摘In the realm of the synthesis of heat-integrated distillation configurations,the conventional approach for exploring more heat integration possibilities typically entails the splitting of a single column into a twocolumn configuration.However,this approach frequently necessitates tedious enumeration procedures,resulting in a considerable computational burden.To surmount this formidable challenge,the present study introduces an innovative remedy:The proposition of a superstructure that encompasses both single-column and multiple two-column configurations.Additionally,a simultaneous optimization algorithm is applied to optimize both the process parameters and heat integration structures of the twocolumn configurations.The effectiveness of this approach is demonstrated through a case study focusing on industrial organosilicon separation.The results underscore that the superstructure methodology not only substantially mitigates computational time compared to exhaustive enumeration but also furnishes solutions that exhibit comparable performance.
基金supported by the National Key R&D Program of China(2018YFA0901700)the National Natural Science Foundation of China(31970038,22278241)+1 种基金a grant from the Institute Guo Qiang,Tsinghua University(2021GQG1016)the Department of Chemical Engineering-i BHE Joint Cooperation Fund。
文摘The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.
基金financially supported by the National Key Research&Development Program of China(Nos.2020YFB2008300,2020YFB2008303)。
文摘Titanium matrix composites reinforced with ceramic particles are considered a promising engineering material due to their combination of high specific strength,low density,and high modulus.In this study,the TA15-based composites reinforced with a volume fraction of 10% to 25%(TiB+TiC)were prepared using powder metallurgy and casting technique.Microstructural characterization and phase constitution were examined using optical microscopy(OM),scanning electron microscopy(SEM),and X-ray diffraction(XRD).In addition,the microhardness,room temperature(RT)and high temperature(HT)tensile properties of the composites were evaluated.Results revealed that the reinforcements are distributed uniformly even in the composites with a high volume of TiB and TiC.However,as the volume fraction exceeds 15%,TiB and TiC particles become coarsening and exhibit rod-like and dendritic-like morphology.Microhardness increases gradually from 321.2 HV for the base alloy to a maximum of 473.3 HV as the reinforcement increases to 25vol.%.Tensile test results indicate that a reinforcement volume fraction above 20% is beneficial for enhancing tensile strength and yield strength at high temperatures,but it has an adverse effect on room temperature elongation.Conversely,if the reinforcement volume fraction is below 20%,it can improve high-temperature elongation when the temperature exceeds 600℃.
基金supported by the National Natural Science Foundation of China[Nos.U21A20332,52103226,52202275,52203314,and 12204253]the Distinguished Young Scholars Fund of Jiangsu Province[No.BK20220061]the Fellowship of China Postdoctoral Science Foundation[No.2021M702382]。
文摘Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.
基金supported by the National Natural Science Foundation of China(22025801)and(22208190)National Postdoctoral Program for Innovative Talents(BX2021146)Shuimu Tsinghua Scholar Program(2021SM055).
文摘Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.
基金the financial supports from the National Natural Science Foundation of China(22322803,22178059,22208054,22221005,22072019)Key Technologies Innovation and Industrialization Projects of Fujian Province(2022G031)Qingyuan Innovation Laboratory(00121002,00523005)。
文摘A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composition and synthesis conditions.Characterizations show that Fe ZSM-22 zeolite synthesized with OSDA-free owns high crystallinity,obvious thin needle-shaped morphology and high Bronsted/Lewis acid ratio.Significantly,when used for n-octane hydroisomerization reaction,its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C_(8)isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals,respectively.This work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance.