New energy sources that reduce the volume of harmful gases such as SO_(x)and NO_(x)released into the atmosphere are in constant development.Natural gas,primarily made up of methane,is being widely used as one reliable...New energy sources that reduce the volume of harmful gases such as SO_(x)and NO_(x)released into the atmosphere are in constant development.Natural gas,primarily made up of methane,is being widely used as one reliable energy source for heating and electricity generation due to its high combustion value.Currently,natural gas accounts for a large portion of electricity generation and chemical feedstock in manufacturing plastics and other commercially important organic chemicals.In the near future,natural gas will be widely used as a fuel for vehicles.Therefore,a practical storage device for its storage and transportation is very beneficial to the deployment of natural gas as an energy source for new technologies.In this tutorial review,biomaterials-based carbon monoliths(CMs),one kind of carbonaceous material,was reviewed as an adsorbent for natural gas(methane)adsorption and storage.展开更多
Porous carbon materials with developed porosity,high surface area and good thermal-and chemicalresistance are advantageous for gas adsorption and separation.However,most carbon adsorbents are in powder form which exhi...Porous carbon materials with developed porosity,high surface area and good thermal-and chemicalresistance are advantageous for gas adsorption and separation.However,most carbon adsorbents are in powder form which exhibit high pressure drop when deployed in practical separation bed.While monolithic carbons have largely addressed the pulverization problem and preserved kinetics and usually suffer from abrasion during multiple adsorption-desorption cycles.Herein,we proposed the designed synthesis of mechanically robust carbon monoliths with hierarchical pores,solid nitrogen-containing framework.The synthesis started with the polymerization of resorcinol and formaldehyde under weakly acidic conditions generated from cyanuric acid,and then an appropriate amount of hexamethylenetetramine(HMTA)was added as a crosslinker to prompt the formation of three dimensional frameworks.After carbonization process,the as-obtained porous carbon monoliths have a high radial compressive strength of 886 N/cm as well as a BET specific surface area of up to 683 m2/g.At approximately 1 bar,the CO2 equilibrium capacities of the monoliths are in the range of 3.1–4.0 mmol/g at 273 K and of 2.3–3.0 mmol/g at 298 K,exhibiting high selectivity for the capture of CO2 over N2 from a stream which consists of 16.7%(v%)CO2 in N2.Meanwhile,they undergo a facile CO2 release in an argon stream at 298 K,indicating a good regeneration capacity.After cycle testing,sieving and regeneration,the adsorbent has no mass loss,compared to that of its fresh counterpart.展开更多
Hierarchically porous FAU monoliths were synthesized via the gel pre-aging route using seed gel as directing agent andα-Al2O3 as monolithic carrier.The as-synthesized samples were characterized by means of the Fourie...Hierarchically porous FAU monoliths were synthesized via the gel pre-aging route using seed gel as directing agent andα-Al2O3 as monolithic carrier.The as-synthesized samples were characterized by means of the Fourier transform infrared spectroscopy(FT-IR),X-ray powder diffraction(XRD),scanning electron microscopy(SEM),and N2 adsorption techniques.The effects of seed gel,gel pre-treatment,and gel pre-aging step were determined,while the possible mechanism for formation of alumina composites via different synthesis processes were discussed.The results showed that the crystal size,the shape,and the loading of the supported FAU could be readily tuned by varying the composition of the crystallization gel without notably changing the structure ofα-Al2O3.The proposed seed gel pre-treating and gel pre-aging route are simple,reproducible,and practically easy to integrate triple porous structures into large-dimension monoliths,which are proved to be very effective in depositing pure FAU crystals on theα-Al2O3 skeleton surface and strengthening the interfacial interaction between them.Moreover,it may provide inspiration to the synthesis of other hierarchical zeolites.展开更多
The various advantages of organic polymer monoliths, including relatively simple preparation processes,abundant monomer availability, and a wide application range of pH, have attracted the attention of chromatographer...The various advantages of organic polymer monoliths, including relatively simple preparation processes,abundant monomer availability, and a wide application range of pH, have attracted the attention of chromatographers. Organic polymer monoliths prepared by traditional methods only have macropores and mesopores, and micropores of less than 50 nm are not commonly available. These typical monoliths are suitable for the separation of biological macromolecules such as proteins and nucleic acids, but their ability to separate small molecular compounds is poor. In recent years, researchers have successfully modified polymer monoliths to achieve uniform compact pore structures. In particular, microporous materials with pores of 50 nm or less that can provide a large enough surface area are the key to the separation of small molecules. In this review, preparation methods of polymer monoliths for high-performance liquid chromatography, including ultra-high cross-linking technology, post-surface modification, and the addition of nanomaterials, are discussed. Modified monolithic columns have been used successfully to separate small molecules with obvious improvements in column efficiency.展开更多
Liquid metal(LM)has become an emerging material paradigm in the electromagnetic interference shielding field owing to its excellent electrical conductivity.However,the processing of lightweight bulk LM composites with...Liquid metal(LM)has become an emerging material paradigm in the electromagnetic interference shielding field owing to its excellent electrical conductivity.However,the processing of lightweight bulk LM composites with finite package without leakage is still a great challenge,due to high surface tension and pump-out issues of LM.Here,a novel confined thermal expansion strategy based on expandable microsphere(EM)is proposed to develop a new class of LM-based monoliths with 3D continuous conductive network.The EM/LM monolith(EM/LMm)presents outstanding performance of lightweight like metallic aerogel(0.104 g cm^(-1)),high strength(3.43 MPa),super elasticity(90%strain),as well as excellent tailor ability and recyclability,rely on its unique gas-filled closed-cellular structure and refined LM network.Moreover,the assembled highly conducting EM/LMm exhibits a recorded shielding effectiveness(98.7 dB)over a broad frequency range of 8.2-40 GHz among reported LM-based composites at an ultra-low content of LM,and demonstrates excellent electromagnetic sealing capacity in practical electronics.The ternary EM/LM/Ni monoliths fabricated by the same approach could be promising universal design principles for multifunctional LM composites,and applicable in magnetic responsive actuator.展开更多
For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectu...For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectures,3D networks,or aerogels.The intersupported structure of porous monolithic 3D graphene(3DG)can prevent aggregation or restacking of graphene individuals,and the interconnected sp^(2) network of 3DG not only can provide the highway for the transport of electron/phonon but also can present continual cavities/channels for mass transfer.This review summarizes the synthesis methodology of 3DG porous monoliths and highlights the application for electric double-layer capacitors.Present challenges and future prospects about the manufacture and application of 3DG are also discussed.展开更多
A novelty method,frontal polymerization(FP),was employed to directly produce a series of polyacrylamide (PAM),poly(N-isopropylacrylamide)(PNIPAM) and acrylamide-N-isopropylacrylamide copolymer macroporous monoliths. F...A novelty method,frontal polymerization(FP),was employed to directly produce a series of polyacrylamide (PAM),poly(N-isopropylacrylamide)(PNIPAM) and acrylamide-N-isopropylacrylamide copolymer macroporous monoliths. Field emission scanning electronic microscope and mercury intrusion method were adopted to measure some parameters of these monoliths,such as frame,pore size distribution as well as porosity.Effects of types of monomer,thicker and surfactant on porous structure of monoliths were studied.A variet...展开更多
Zwitterionic sulfobetaine-based monolithic stationary phases have attracted increasing attention for their use in hydrophilic interaction chromatography.In this study,a novel hydrophilic polymeric monolith was fabrica...Zwitterionic sulfobetaine-based monolithic stationary phases have attracted increasing attention for their use in hydrophilic interaction chromatography.In this study,a novel hydrophilic polymeric monolith was fabricated through photo-initiated copolymerization of 3-(3-vinyl-1-imidazolio)-1-propanesulfonate(SBVI)with pentaerythritol triacrylate using methanol and tetrahydrofuran as the porogenic system.Notably,the duration for the preparation of this novel monolith was as little as 5 min,which was significantly shorter than that required for previously reported sulfobetaine-based monoliths prepared via conventional thermally initiated copolymerization.Moreover,these monoliths showed good morphology,permeability,porosity(62.4%),mechanical strength(over 15 MPa),column efficiency(51,230 plates/m),and reproducibility(relative standard deviations for all analytes were lower than 4.6%).Mechanistic studies indicated that strong hydrophilic and negative electrostatic interactions might be responsible for the retention of polar analytes on the zwitterionic SBVI-based monolith.In particular,the resulting monolith exhibited good anti-protein adhesion ability and low nonspecific protein adsorption.These excellent features seem to favor its application in bioanalysis.Therefore,the novel zwitterionic sulfobetaine-based monolith was successfully employed for the highly selective separation of small bioactive compounds and the efficient enrichment of N-glycopeptides from complex samples.In this study,we prepared a novel zwitterionic sulfobetaine-based monolith with good performance and developed a simpler and faster method for preparation of zwitterionic monoliths.展开更多
In this paper,hierarchically porous Fe2O3 /CuO composite monoliths were first successfully synthesized by a mild method using silica monoliths as templates.The structure of composite monoliths was characterized by X-r...In this paper,hierarchically porous Fe2O3 /CuO composite monoliths were first successfully synthesized by a mild method using silica monoliths as templates.The structure of composite monoliths was characterized by X-ray diffraction,scanning electron microscopy,nitrogen adsorption-desorption.The results indicated that the molar ratio of Fe to Cu had a great influence on the crystal phase of Fe2O3,pore size and the structure of the macroporous wall.The Fe2O3 /CuO composite monoliths consist of hierarchically macroporous and mesoporous structure,while the sample with the Fe/Cu molar ratio of 2:1 possesses tighter wall structure than other samples.It is expected that asprepared Fe2O3/CuO composite monoliths have potential applications in several fields as catalysts,catalyst supports,chemical sensors and high-performance liquid chromatography (HPLC).展开更多
A new method for preparing LiLaNiO/γ(-Al2O3 monolithic catalyst was described and discussed. The catalyst, which was supported over the monolith, was evaluated in a POM to syngas process. Relative stable catalytic pr...A new method for preparing LiLaNiO/γ(-Al2O3 monolithic catalyst was described and discussed. The catalyst, which was supported over the monolith, was evaluated in a POM to syngas process. Relative stable catalytic properties during the 120 hours operation at atmospheric pressure were found for the catalyst. Under the high space velocity of 9.0×104l/(kg·(h)(CH4), the conversion of methane came to 95.5%, and the selectivity of carbon monoxide was not below 96.0% at 1123K when ratio of the feedstock (CH4/O2) was equal to 2.0.展开更多
Methane adsorption by different forms of activated carbon obtained from coffee husks, including monolith honeycomb and disc types, was studied by activation with zinc salts and potassium hydroxide at 298.15 K and 303....Methane adsorption by different forms of activated carbon obtained from coffee husks, including monolith honeycomb and disc types, was studied by activation with zinc salts and potassium hydroxide at 298.15 K and 303.15 K and pressures up to 30.00 atm in a volumetric adsorption apparatus. We observed increased methane adsorption capacity on a mass basis in the different activated carbon monoliths with increasing surface area, total pore volume and micropore volume, with the honeycomb type displaying the highest methane absorption capacity. The maximum volumetric methane uptake by the synthesised carbon monoliths was observed to be 130 V/V at 298.15 K and 30.00 atm for honeycomb monoliths synthesised with zinc chloride (ZnCl2) and Polyvinyl alcohol (PVA) as the binder. Adsorption calorimetry results were used to describe the interaction between guest molecules and the adsorbent at low surface coverage and the energetic heterogeneous surface nature of the adsorbent.展开更多
Metal-organic frameworks(MOFs)have been extensively considered as one of the most promising types of porous and crystalline organic-inorganic materials,thanks to their large specific surface area,high porosity,tailora...Metal-organic frameworks(MOFs)have been extensively considered as one of the most promising types of porous and crystalline organic-inorganic materials,thanks to their large specific surface area,high porosity,tailorable structures and compositions,diverse functionalities,and well-controlled pore/size distribution.However,most developed MOFs are in powder forms,which still have some technical challenges,including abrasion,dustiness,low packing densities,clogging,mass/heat transfer limitation,environmental pollution,and mechanical instability during the packing process,that restrict their applicability in industrial applications.Therefore,in recent years,attention has focused on techniques to convert MOF powders into macroscopic materials like beads,membranes,monoliths,gel/sponges,and nanofibers to overcome these challenges.Three-dimensional(3D)printing technology has achieved much interest because it can produce many high-resolution macroscopic frameworks with complex shapes and geometries from digital models.Therefore,this review summarizes the combination of different 3D printing strategies with MOFs and MOF-based materials for fabricating 3D-printed MOF monoliths and their environmental applications,emphasizing water treatment and gas adsorption/separation applications.Herein,the various strategies for the fabrication of 3D-printed MOF monoliths,such as direct ink writing,seed-assisted in-situ growth,coordination replication from solid precursors,matrix incorporation,selective laser sintering,and digital light processing,are described with the relevant examples.Finally,future directions and challenges of 3D-printed MOF monoliths are also presented to better plan future trajectories in the shaping of MOF materials with improved control over the structure,composition,and textural properties of 3D-printed MOF monoliths.展开更多
Utilizing solar energy for sorbent regeneration during the CO_(2)swing adsorption process could potentially reduce CO_(2)capture costs.This study describes a new technique—solar thermal swing adsorption(STSA)for CO_(...Utilizing solar energy for sorbent regeneration during the CO_(2)swing adsorption process could potentially reduce CO_(2)capture costs.This study describes a new technique—solar thermal swing adsorption(STSA)for CO_(2)capture based on application of intermittent illumination onto porous carbon monolith(PCM)sorbents during the CO_(2)capture process.This allows CO_(2)to be selectively adsorbed on the sorbents during the light-off periods and thereafter released during the light-on periods due to the solar thermal effect.The freestanding and mechanically strong PCMs have rich ultramicropores with narrow pore size distributions,displaying relatively high CO_(2)adsorption capacity and high CO_(2)/N_(2) selectivity.Given the high CO_(2)capture performance,high solar thermal conversion efficiency,and high thermal conductivity,the PCM sorbents could achieve high CO_(2)capture rate of up to 0.226 kg·kgcarbon^(-1)·h^(-1)from a gas mixture of 20 vol.%CO_(2)/80 vol.%N_(2) under STSA conditions with a light intensity of 1000 W·m^(-2).In addition,the combination of STSA with the conventional vacuum swing adsorption technique further increases the CO_(2)working capacity.展开更多
Binary oxide systems(Cu Cr2O4, Cu Co2O4), deposited onto cordierite monoliths of honeycomb structure with a second support(finely dispersed Al2O3), were prepared as filters for catalytic combustion of diesel soot ...Binary oxide systems(Cu Cr2O4, Cu Co2O4), deposited onto cordierite monoliths of honeycomb structure with a second support(finely dispersed Al2O3), were prepared as filters for catalytic combustion of diesel soot using internal combustion engine’s gas exhausts(O2, NOx, H2 O, CO2) and O3 as oxidizing agents. It is shown that the second support increases soot capacity of aforementioned filters, and causes dispersion of the particles of spinel phases as active components enhancing thereby catalyst activity and selectivity of soot combustion to CO2. Oxidants used can be arranged with reference to decreasing their activity in a following series: O3 NO2〉 H2 O 〉 NO 〉 O2〉 CO2. Ozone proved to be the most efficient oxidizing agent: the diesel soot combustion by O3 occurs intensively(in the presence of copper chromite based catalyst) even at closing to ambient temperatures.Results obtained give a basis for the conclusion that using a catalytic coating on soot filters in the form of aforementioned binary oxide systems and ozone as the initiator of the oxidation processes is a promising approach in solving the problem of comprehensive purification of automotive exhaust gases at relatively low temperatures, known as the "cold start" problem.展开更多
Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and ...Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and functional surfaces,which have significant values in various application areas.The emerging 3D printing technology further provides MOF and COFs(M/COFs)with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths.However,the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’microstructural features,both during and after 3D printing.It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications.In this overview,the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths.Their differences in the properties,applications,and current research states are discussed.The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF.Throughout the analysis of the current states of 3D-printed M/COFs,the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.展开更多
The inverse and direct piezoelectric and circuit coupling are widely observed in advanced electro-mechanical systems such as piezoelectric energy harvesters.Existing strongly coupled analysis methods based on direct n...The inverse and direct piezoelectric and circuit coupling are widely observed in advanced electro-mechanical systems such as piezoelectric energy harvesters.Existing strongly coupled analysis methods based on direct numerical modeling for this phenomenon can be classified into partitioned or monolithic formulations.Each formulation has its advantages and disadvantages,and the choice depends on the characteristics of each coupled problem.This study proposes a new option:a coupled analysis strategy that combines the best features of the existing formulations,namely,the hybrid partitioned-monolithic method.The analysis of inverse piezoelectricity and the monolithic analysis of direct piezoelectric and circuit interaction are strongly coupled using a partitioned iterative hierarchical algorithm.In a typical benchmark problem of a piezoelectric energy harvester,this research compares the results from the proposed method to those from the conventional strongly coupled partitioned iterative method,discussing the accuracy,stability,and computational cost.The proposed hybrid concept is effective for coupled multi-physics problems,including various coupling conditions.展开更多
With the explosive development of artificial intelligence(AI),machine learning(ML),and high-performance comput-ing(HPC),the ever-growing data movement is asking for high density interconnects with higher bandwidth(BW)...With the explosive development of artificial intelligence(AI),machine learning(ML),and high-performance comput-ing(HPC),the ever-growing data movement is asking for high density interconnects with higher bandwidth(BW),lower power and lower latency[1−3].The optical I/O leverages silicon photonic(SiPh)technology to enable high-density large-scale integrated photonics.展开更多
Carbazole moiety-based 2PACz([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)self-assembled monolayers(SAMs)are excellent hole-selective contact(HSC)materials with abilities to excel the charge-transferdynamics of perovski...Carbazole moiety-based 2PACz([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)self-assembled monolayers(SAMs)are excellent hole-selective contact(HSC)materials with abilities to excel the charge-transferdynamics of perovskite solar cells(PSCs).Herein,we report a facile but powerful method to functionalize the surface of 2PACz-SAM,by which reproducible,highly stable,high-efficiency wide-bandgap PSCs can be obtained.The 2PACz surface treatment with various donor number solvents improves assembly of 2PACz-SAM and leave residual surface-bound solvent molecules on 2PACz-SAM,which increases perovskite grain size,retards halide segregation,and accelerates hole extraction.The surface functionalization achieves a high power conversion efficiency(PCE)of 17.62%for a single-junction wide-bandgap(~1.77 e V)PSC.We also demonstrate a monolithic all-perovskite tandem solar cell using surfaceengineered HSC,showing high PCE of 24.66%with large open-circuit voltage of 2.008 V and high fillfactor of 81.45%.Our results suggest this simple approach can further improve the tandem device,when coupled with a high-performance narrow-bandgap sub-cell.展开更多
Frame and rocking wall(FRW)structures have excellent resilient performance during earthquakes.However,the concrete at interfacial corners of rocking walls(RWs)is easily crushed due to local extreme compression during ...Frame and rocking wall(FRW)structures have excellent resilient performance during earthquakes.However,the concrete at interfacial corners of rocking walls(RWs)is easily crushed due to local extreme compression during the rocking process.An innovative RW with a curved interface is proposed to prevent interfacial corners from producing local damage,enhancing its earthquake resilient performance(ERP).The precast wall panel with a curved interface is assembled into an integral self-centering hybrid rocking wall(SCRW)by two post-tensioned unbonded prestressed tendons.Moreover,two ordinary energy dissipation steel rebars and two shear reinforcements are arranged to increase the energy dissipation capacity and lateral resistance.Two SCRW specimens and one monolithic reinforced concrete(RC)shear wall(SW)were tested under pseudo-static loading to compare the ERPs of the proposed SCRW and the SW,focusing on studying the effect of the curved interface on the SCRW.The key resilient performance of rocking effects,failure modes,and hysteretic properties of the SCRW were explored.The results show that nonlinear deformations of the SCRW are concentrated along the interface between the SCRW and the foundation,avoiding damage within the SCRW.The restoring force provided by the prestressed tendons can effectively realize self-centering capacity with small residual deformation,and the resilient performance of the SCRW is better than that of monolithic SW.In addition,the curved interface of the SCRW makes the rocking center change and move inward,partially relieving the stress concentration and crush of concrete.The rocking range of the rocking center is about 41.4%of the width of the SCRW.展开更多
基金Acknowledgment is made to the Donors of the American Chemical Society Petroleum Research Fund for support of this research.
文摘New energy sources that reduce the volume of harmful gases such as SO_(x)and NO_(x)released into the atmosphere are in constant development.Natural gas,primarily made up of methane,is being widely used as one reliable energy source for heating and electricity generation due to its high combustion value.Currently,natural gas accounts for a large portion of electricity generation and chemical feedstock in manufacturing plastics and other commercially important organic chemicals.In the near future,natural gas will be widely used as a fuel for vehicles.Therefore,a practical storage device for its storage and transportation is very beneficial to the deployment of natural gas as an energy source for new technologies.In this tutorial review,biomaterials-based carbon monoliths(CMs),one kind of carbonaceous material,was reviewed as an adsorbent for natural gas(methane)adsorption and storage.
基金financially supported by a Joint Sino-German Research Project(21761132011)the National Natural Science Foundation of China(No.21776041)the Cheung Kong Scholars Programme of China(T2015036).
文摘Porous carbon materials with developed porosity,high surface area and good thermal-and chemicalresistance are advantageous for gas adsorption and separation.However,most carbon adsorbents are in powder form which exhibit high pressure drop when deployed in practical separation bed.While monolithic carbons have largely addressed the pulverization problem and preserved kinetics and usually suffer from abrasion during multiple adsorption-desorption cycles.Herein,we proposed the designed synthesis of mechanically robust carbon monoliths with hierarchical pores,solid nitrogen-containing framework.The synthesis started with the polymerization of resorcinol and formaldehyde under weakly acidic conditions generated from cyanuric acid,and then an appropriate amount of hexamethylenetetramine(HMTA)was added as a crosslinker to prompt the formation of three dimensional frameworks.After carbonization process,the as-obtained porous carbon monoliths have a high radial compressive strength of 886 N/cm as well as a BET specific surface area of up to 683 m2/g.At approximately 1 bar,the CO2 equilibrium capacities of the monoliths are in the range of 3.1–4.0 mmol/g at 273 K and of 2.3–3.0 mmol/g at 298 K,exhibiting high selectivity for the capture of CO2 over N2 from a stream which consists of 16.7%(v%)CO2 in N2.Meanwhile,they undergo a facile CO2 release in an argon stream at 298 K,indicating a good regeneration capacity.After cycle testing,sieving and regeneration,the adsorbent has no mass loss,compared to that of its fresh counterpart.
基金This work was supported by the National Natural Science Foundation of China(No.61673004 and No.11472048)the Fundamental Research Funds for the Central Universities of China(XK1802-4).
文摘Hierarchically porous FAU monoliths were synthesized via the gel pre-aging route using seed gel as directing agent andα-Al2O3 as monolithic carrier.The as-synthesized samples were characterized by means of the Fourier transform infrared spectroscopy(FT-IR),X-ray powder diffraction(XRD),scanning electron microscopy(SEM),and N2 adsorption techniques.The effects of seed gel,gel pre-treatment,and gel pre-aging step were determined,while the possible mechanism for formation of alumina composites via different synthesis processes were discussed.The results showed that the crystal size,the shape,and the loading of the supported FAU could be readily tuned by varying the composition of the crystallization gel without notably changing the structure ofα-Al2O3.The proposed seed gel pre-treating and gel pre-aging route are simple,reproducible,and practically easy to integrate triple porous structures into large-dimension monoliths,which are proved to be very effective in depositing pure FAU crystals on theα-Al2O3 skeleton surface and strengthening the interfacial interaction between them.Moreover,it may provide inspiration to the synthesis of other hierarchical zeolites.
文摘The various advantages of organic polymer monoliths, including relatively simple preparation processes,abundant monomer availability, and a wide application range of pH, have attracted the attention of chromatographers. Organic polymer monoliths prepared by traditional methods only have macropores and mesopores, and micropores of less than 50 nm are not commonly available. These typical monoliths are suitable for the separation of biological macromolecules such as proteins and nucleic acids, but their ability to separate small molecular compounds is poor. In recent years, researchers have successfully modified polymer monoliths to achieve uniform compact pore structures. In particular, microporous materials with pores of 50 nm or less that can provide a large enough surface area are the key to the separation of small molecules. In this review, preparation methods of polymer monoliths for high-performance liquid chromatography, including ultra-high cross-linking technology, post-surface modification, and the addition of nanomaterials, are discussed. Modified monolithic columns have been used successfully to separate small molecules with obvious improvements in column efficiency.
基金This work was financially supported by the National Natural Science Foundation of China(62074154)China Postdoctoral Science Foundation(Grant No.2020M682983)+2 种基金Guangdong Basic and Applied Basic Research Fund(2020A1515110962,2020A1515110154)Shenzhen Basic Research Plan(JCYJ20180507182530279)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2017411).
文摘Liquid metal(LM)has become an emerging material paradigm in the electromagnetic interference shielding field owing to its excellent electrical conductivity.However,the processing of lightweight bulk LM composites with finite package without leakage is still a great challenge,due to high surface tension and pump-out issues of LM.Here,a novel confined thermal expansion strategy based on expandable microsphere(EM)is proposed to develop a new class of LM-based monoliths with 3D continuous conductive network.The EM/LM monolith(EM/LMm)presents outstanding performance of lightweight like metallic aerogel(0.104 g cm^(-1)),high strength(3.43 MPa),super elasticity(90%strain),as well as excellent tailor ability and recyclability,rely on its unique gas-filled closed-cellular structure and refined LM network.Moreover,the assembled highly conducting EM/LMm exhibits a recorded shielding effectiveness(98.7 dB)over a broad frequency range of 8.2-40 GHz among reported LM-based composites at an ultra-low content of LM,and demonstrates excellent electromagnetic sealing capacity in practical electronics.The ternary EM/LM/Ni monoliths fabricated by the same approach could be promising universal design principles for multifunctional LM composites,and applicable in magnetic responsive actuator.
基金The authors acknowledge the support from National Natural Science Foundation of China(51972168,51672124,21603096)Program for Innovative Talents and Entrepreneur in Jiangsu,State Key Laboratory of Catalytic Materials and Reaction Engineering(RIPP,SINOPEC),and Technical Center of Nano Fabrication and Characterization of Nanjing University.
文摘For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectures,3D networks,or aerogels.The intersupported structure of porous monolithic 3D graphene(3DG)can prevent aggregation or restacking of graphene individuals,and the interconnected sp^(2) network of 3DG not only can provide the highway for the transport of electron/phonon but also can present continual cavities/channels for mass transfer.This review summarizes the synthesis methodology of 3DG porous monoliths and highlights the application for electric double-layer capacitors.Present challenges and future prospects about the manufacture and application of 3DG are also discussed.
基金supported by the National Natural Science Foundation of China(No50772013)
文摘A novelty method,frontal polymerization(FP),was employed to directly produce a series of polyacrylamide (PAM),poly(N-isopropylacrylamide)(PNIPAM) and acrylamide-N-isopropylacrylamide copolymer macroporous monoliths. Field emission scanning electronic microscope and mercury intrusion method were adopted to measure some parameters of these monoliths,such as frame,pore size distribution as well as porosity.Effects of types of monomer,thicker and surfactant on porous structure of monoliths were studied.A variet...
基金supported by the National Natural Science Foundation of China(Grant Nos.:82173773 and 82073806)the Natural Science Foundation of Guangdong Province,China(Grant Nos.:2020A1515010569 and 2021A0505030039)Science and Technology Program of Guangzhou,China(Grant No.:202102020729).
文摘Zwitterionic sulfobetaine-based monolithic stationary phases have attracted increasing attention for their use in hydrophilic interaction chromatography.In this study,a novel hydrophilic polymeric monolith was fabricated through photo-initiated copolymerization of 3-(3-vinyl-1-imidazolio)-1-propanesulfonate(SBVI)with pentaerythritol triacrylate using methanol and tetrahydrofuran as the porogenic system.Notably,the duration for the preparation of this novel monolith was as little as 5 min,which was significantly shorter than that required for previously reported sulfobetaine-based monoliths prepared via conventional thermally initiated copolymerization.Moreover,these monoliths showed good morphology,permeability,porosity(62.4%),mechanical strength(over 15 MPa),column efficiency(51,230 plates/m),and reproducibility(relative standard deviations for all analytes were lower than 4.6%).Mechanistic studies indicated that strong hydrophilic and negative electrostatic interactions might be responsible for the retention of polar analytes on the zwitterionic SBVI-based monolith.In particular,the resulting monolith exhibited good anti-protein adhesion ability and low nonspecific protein adsorption.These excellent features seem to favor its application in bioanalysis.Therefore,the novel zwitterionic sulfobetaine-based monolith was successfully employed for the highly selective separation of small bioactive compounds and the efficient enrichment of N-glycopeptides from complex samples.In this study,we prepared a novel zwitterionic sulfobetaine-based monolith with good performance and developed a simpler and faster method for preparation of zwitterionic monoliths.
基金supported by the National Natural Science Foundation of China(No. 20977052)the Chinese Academy of Sciences(Grant No. KZCX2-YW-420)the National 973 Program(No. 2009CB421606)
文摘In this paper,hierarchically porous Fe2O3 /CuO composite monoliths were first successfully synthesized by a mild method using silica monoliths as templates.The structure of composite monoliths was characterized by X-ray diffraction,scanning electron microscopy,nitrogen adsorption-desorption.The results indicated that the molar ratio of Fe to Cu had a great influence on the crystal phase of Fe2O3,pore size and the structure of the macroporous wall.The Fe2O3 /CuO composite monoliths consist of hierarchically macroporous and mesoporous structure,while the sample with the Fe/Cu molar ratio of 2:1 possesses tighter wall structure than other samples.It is expected that asprepared Fe2O3/CuO composite monoliths have potential applications in several fields as catalysts,catalyst supports,chemical sensors and high-performance liquid chromatography (HPLC).
基金the National Advanced Materials Committee of China (Grant No. 715-006-0122) and the Ministry of Science and Technology, China (
文摘A new method for preparing LiLaNiO/γ(-Al2O3 monolithic catalyst was described and discussed. The catalyst, which was supported over the monolith, was evaluated in a POM to syngas process. Relative stable catalytic properties during the 120 hours operation at atmospheric pressure were found for the catalyst. Under the high space velocity of 9.0×104l/(kg·(h)(CH4), the conversion of methane came to 95.5%, and the selectivity of carbon monoxide was not below 96.0% at 1123K when ratio of the feedstock (CH4/O2) was equal to 2.0.
文摘Methane adsorption by different forms of activated carbon obtained from coffee husks, including monolith honeycomb and disc types, was studied by activation with zinc salts and potassium hydroxide at 298.15 K and 303.15 K and pressures up to 30.00 atm in a volumetric adsorption apparatus. We observed increased methane adsorption capacity on a mass basis in the different activated carbon monoliths with increasing surface area, total pore volume and micropore volume, with the honeycomb type displaying the highest methane absorption capacity. The maximum volumetric methane uptake by the synthesised carbon monoliths was observed to be 130 V/V at 298.15 K and 30.00 atm for honeycomb monoliths synthesised with zinc chloride (ZnCl2) and Polyvinyl alcohol (PVA) as the binder. Adsorption calorimetry results were used to describe the interaction between guest molecules and the adsorbent at low surface coverage and the energetic heterogeneous surface nature of the adsorbent.
文摘Metal-organic frameworks(MOFs)have been extensively considered as one of the most promising types of porous and crystalline organic-inorganic materials,thanks to their large specific surface area,high porosity,tailorable structures and compositions,diverse functionalities,and well-controlled pore/size distribution.However,most developed MOFs are in powder forms,which still have some technical challenges,including abrasion,dustiness,low packing densities,clogging,mass/heat transfer limitation,environmental pollution,and mechanical instability during the packing process,that restrict their applicability in industrial applications.Therefore,in recent years,attention has focused on techniques to convert MOF powders into macroscopic materials like beads,membranes,monoliths,gel/sponges,and nanofibers to overcome these challenges.Three-dimensional(3D)printing technology has achieved much interest because it can produce many high-resolution macroscopic frameworks with complex shapes and geometries from digital models.Therefore,this review summarizes the combination of different 3D printing strategies with MOFs and MOF-based materials for fabricating 3D-printed MOF monoliths and their environmental applications,emphasizing water treatment and gas adsorption/separation applications.Herein,the various strategies for the fabrication of 3D-printed MOF monoliths,such as direct ink writing,seed-assisted in-situ growth,coordination replication from solid precursors,matrix incorporation,selective laser sintering,and digital light processing,are described with the relevant examples.Finally,future directions and challenges of 3D-printed MOF monoliths are also presented to better plan future trajectories in the shaping of MOF materials with improved control over the structure,composition,and textural properties of 3D-printed MOF monoliths.
基金This study was supported byÅForsk research grant and Anhui Provincial Natural Science Foundation(No.2108085QB72)。
文摘Utilizing solar energy for sorbent regeneration during the CO_(2)swing adsorption process could potentially reduce CO_(2)capture costs.This study describes a new technique—solar thermal swing adsorption(STSA)for CO_(2)capture based on application of intermittent illumination onto porous carbon monolith(PCM)sorbents during the CO_(2)capture process.This allows CO_(2)to be selectively adsorbed on the sorbents during the light-off periods and thereafter released during the light-on periods due to the solar thermal effect.The freestanding and mechanically strong PCMs have rich ultramicropores with narrow pore size distributions,displaying relatively high CO_(2)adsorption capacity and high CO_(2)/N_(2) selectivity.Given the high CO_(2)capture performance,high solar thermal conversion efficiency,and high thermal conductivity,the PCM sorbents could achieve high CO_(2)capture rate of up to 0.226 kg·kgcarbon^(-1)·h^(-1)from a gas mixture of 20 vol.%CO_(2)/80 vol.%N_(2) under STSA conditions with a light intensity of 1000 W·m^(-2).In addition,the combination of STSA with the conventional vacuum swing adsorption technique further increases the CO_(2)working capacity.
文摘Binary oxide systems(Cu Cr2O4, Cu Co2O4), deposited onto cordierite monoliths of honeycomb structure with a second support(finely dispersed Al2O3), were prepared as filters for catalytic combustion of diesel soot using internal combustion engine’s gas exhausts(O2, NOx, H2 O, CO2) and O3 as oxidizing agents. It is shown that the second support increases soot capacity of aforementioned filters, and causes dispersion of the particles of spinel phases as active components enhancing thereby catalyst activity and selectivity of soot combustion to CO2. Oxidants used can be arranged with reference to decreasing their activity in a following series: O3 NO2〉 H2 O 〉 NO 〉 O2〉 CO2. Ozone proved to be the most efficient oxidizing agent: the diesel soot combustion by O3 occurs intensively(in the presence of copper chromite based catalyst) even at closing to ambient temperatures.Results obtained give a basis for the conclusion that using a catalytic coating on soot filters in the form of aforementioned binary oxide systems and ozone as the initiator of the oxidation processes is a promising approach in solving the problem of comprehensive purification of automotive exhaust gases at relatively low temperatures, known as the "cold start" problem.
基金the support by National Research Foundation of Singapore(NRF,Project:NRF-CRP262021RS-0002),for research conducted at the National University of Singapore(NUS)。
文摘Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and functional surfaces,which have significant values in various application areas.The emerging 3D printing technology further provides MOF and COFs(M/COFs)with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths.However,the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’microstructural features,both during and after 3D printing.It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications.In this overview,the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths.Their differences in the properties,applications,and current research states are discussed.The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF.Throughout the analysis of the current states of 3D-printed M/COFs,the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.
基金supported by the Japan Society for the Promotion of Science,KAKENHI Grant No.23H00475.
文摘The inverse and direct piezoelectric and circuit coupling are widely observed in advanced electro-mechanical systems such as piezoelectric energy harvesters.Existing strongly coupled analysis methods based on direct numerical modeling for this phenomenon can be classified into partitioned or monolithic formulations.Each formulation has its advantages and disadvantages,and the choice depends on the characteristics of each coupled problem.This study proposes a new option:a coupled analysis strategy that combines the best features of the existing formulations,namely,the hybrid partitioned-monolithic method.The analysis of inverse piezoelectricity and the monolithic analysis of direct piezoelectric and circuit interaction are strongly coupled using a partitioned iterative hierarchical algorithm.In a typical benchmark problem of a piezoelectric energy harvester,this research compares the results from the proposed method to those from the conventional strongly coupled partitioned iterative method,discussing the accuracy,stability,and computational cost.The proposed hybrid concept is effective for coupled multi-physics problems,including various coupling conditions.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.61925505,92373209 and 62235017).
文摘With the explosive development of artificial intelligence(AI),machine learning(ML),and high-performance comput-ing(HPC),the ever-growing data movement is asking for high density interconnects with higher bandwidth(BW),lower power and lower latency[1−3].The optical I/O leverages silicon photonic(SiPh)technology to enable high-density large-scale integrated photonics.
基金supported by the National Research Foundation of Korea (NRF)the Ministry of Science,ICT (2022M3J1A1085285,2019R1A2C1084010,and 2022R1A2C2006532)the Korea Electric Power Corporation (R20XO02-1)。
文摘Carbazole moiety-based 2PACz([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)self-assembled monolayers(SAMs)are excellent hole-selective contact(HSC)materials with abilities to excel the charge-transferdynamics of perovskite solar cells(PSCs).Herein,we report a facile but powerful method to functionalize the surface of 2PACz-SAM,by which reproducible,highly stable,high-efficiency wide-bandgap PSCs can be obtained.The 2PACz surface treatment with various donor number solvents improves assembly of 2PACz-SAM and leave residual surface-bound solvent molecules on 2PACz-SAM,which increases perovskite grain size,retards halide segregation,and accelerates hole extraction.The surface functionalization achieves a high power conversion efficiency(PCE)of 17.62%for a single-junction wide-bandgap(~1.77 e V)PSC.We also demonstrate a monolithic all-perovskite tandem solar cell using surfaceengineered HSC,showing high PCE of 24.66%with large open-circuit voltage of 2.008 V and high fillfactor of 81.45%.Our results suggest this simple approach can further improve the tandem device,when coupled with a high-performance narrow-bandgap sub-cell.
基金National Key Research and Development Program of China under Grant No.2018YFC0705602。
文摘Frame and rocking wall(FRW)structures have excellent resilient performance during earthquakes.However,the concrete at interfacial corners of rocking walls(RWs)is easily crushed due to local extreme compression during the rocking process.An innovative RW with a curved interface is proposed to prevent interfacial corners from producing local damage,enhancing its earthquake resilient performance(ERP).The precast wall panel with a curved interface is assembled into an integral self-centering hybrid rocking wall(SCRW)by two post-tensioned unbonded prestressed tendons.Moreover,two ordinary energy dissipation steel rebars and two shear reinforcements are arranged to increase the energy dissipation capacity and lateral resistance.Two SCRW specimens and one monolithic reinforced concrete(RC)shear wall(SW)were tested under pseudo-static loading to compare the ERPs of the proposed SCRW and the SW,focusing on studying the effect of the curved interface on the SCRW.The key resilient performance of rocking effects,failure modes,and hysteretic properties of the SCRW were explored.The results show that nonlinear deformations of the SCRW are concentrated along the interface between the SCRW and the foundation,avoiding damage within the SCRW.The restoring force provided by the prestressed tendons can effectively realize self-centering capacity with small residual deformation,and the resilient performance of the SCRW is better than that of monolithic SW.In addition,the curved interface of the SCRW makes the rocking center change and move inward,partially relieving the stress concentration and crush of concrete.The rocking range of the rocking center is about 41.4%of the width of the SCRW.