查看更多>>摘要：Membrane separation technology provides an effective alternative to mitigate the massive carbon emission with high carbon capture productivity and efficiency.In the context of operating membranes under high CO2 pressures allows increased separation productivity and reduced gas compression cost,which,however,often leads to CO2 induced plasticization,a key hurdle for current gas separation membranes.In this review,we reviewed the latest development of membranes with anti-plasticization resistance,potentially suited for operation under high CO2 feed streams.Specifically,the separation performance of polymeric membranes,inorganic membranes,and mixed matrix membranes under high CO2 feed pressures are discussed.Approaches to enhance CO2 induced plastici-zation of those membranes are also summarized.We conclude the recent progress of membranes for high CO2 pressures with perspectives and an outlook for future development.
查看更多>>摘要：Electricity-driven water splitting to convert water into hydrogen(H2)has been widely regarded as an efficient approach for H2 production.Nevertheless,the energy conversion efficiency of it is greatly limited due to the disadvantage of the sluggish kinetic of oxidation evolution reaction(OER).To effectively address the issue,a novel concept of hybrid water electrolysis has been developed for energy-saving H2 production.This strategy aims to replace the sluggish kinetics of OER by utilizing thermodynamically favorable organics oxidation reaction to replace OER.Herein,recent advances in such water splitting system for boosting H2 evolution under low cell voltage are systematically summarized.Some notable progress of different organics oxidation reactions coupled with hydrogen evolution reaction(HER)are discussed in detail.To facilitate the development of hybrid water electrolysis,the major challenges and perspectives are also proposed.
查看更多>>摘要：The worldwide application of organophosphorus pesticides(OPs)has promoted agricultural development,but their gradual accumulation in soil and water can seriously affect the central nervous system of humans and other mammals.Organophosphorus hydrolase(OPH)is an effective enzyme that can catalyze the degradation of the residual OPs.However,the degradation products such as p-nitrophenol(p-NP)is still toxic.Thus,it is of great significance to develop a multi-functional support that can be simultaneously used for the immobilization of OPH and the further degradation of p-NP.Herein,a visible light assisted enzyme-photocatalytic integrated catalyst was constructed by immobilizing OPH on hollow structured Au-TiO2(named OPH@H-Au-TiO2)for the degradation of OPs.The obtained OPH@H-Au-TiO2 can degrade methyl parathion to p-NP by OPH and then degrade p-NP to hydroquinone with low toxicity by using H-Au-TiO2 under visible light.OPH molecules were immobilized on H-Au-TiO2 through adsorption method to prepare OPH@H-Au-TiO2.After 2.5 h of reaction,methyl parathion is completely degraded,and about 82.64％of the generated p-NP is further degraded into hydroquinone.After reused for 4 times,the OPH@H-Au-TiO2 retains more than 80％of the initial degradation activity.This research presents a new insight in designing and constructing multi-functional biocatalyst,which greatly expands the application scenarios and industrial value of enzyme catalysis.
查看更多>>摘要：Modular bioreactors can provide a flexible platform for constructing complex multi-step pathways,which may be a solution for maximizing reactions and overcoming the complexity of multi-enzyme systems.Here,we selected wood-derived cellulose scaffold as a support for enzyme immobilization and constructed the modular bioreactor.Cellulose scaffold was prepared after removing lignin from wood,followed by citric acid functionalization and the addition of glutaraldehyde finally allowed the cross-linking of enzymes.Three enzymes,horseradish peroxidase(HRP),glucose oxidase(GOD),and catalase(CAT),were separately immobilized,resulting in the immobilized enzyme amount to over 40 mg/g.The introduction of carboxyl groups from citric acid facilitated the rapid enzyme adsorption on the support surface and immobilized enzymes possess～65％expressed activity.Modular bio-reactors were constructed by using the immobilized enzymes.With the immobilized HRP module,reactor showed desired catalytic performance with the phenol degradation rate of＞90％.Also,a pH regulation can occur in the bioreactors for preserving enzyme activities and neutralizing acid products.In the GOD/CAT modular bioreactor,the cascade reaction with adjusting pH values can achieve a 95％yield of sodium gluconate and exhibit a favorable reusability of 5 operation cycles.
查看更多>>摘要：One of the bottlenecks limiting the cycling stability of high voltage lithium metal batteries(LMBs)is the lack of suitable electrolytes.Herein,phenyl vinyl sulfone(PVS)is proposed as a multifunctional additive to stabilize both cathode and anode interfaces as it can be preferentially oxidized/reduced on the electrode surfaces.The PVS derived solid electrolyte interphase films can not only reduce the transition metal dissolution on the cathode side,but also suppress the Li dendrite spread on the lithium anode side.The Li‖Li symmetric battery with PVS addition delivers longer cycle life and a higher critical current density of over 3.0 mAh cm-2.The LiNi0.8Co0.1Mn0.1O2(NCM811)‖Li full cell exhibits excellent capacity retention of 80.8％or 80.0％after 400 cycles at 0.5 C or 1 C rate with the voltage range of 3.0-4.3 V.In particular,the NCM811‖Li cell under constrained conditions remains operation over 150 cycles.This work offers new insights into the electrolyte formulations for the next generation of LMBs.
查看更多>>摘要：The sustainable synthesis of dimethyl maleate via diesterification through the utilization of ionic liquid(IL)is of great importance.However,the relationship between the ILs nature and the reactivity of diesterification is still unclear.Herein,a series of ILs with different structures were selected for the comprehensive investigation of diesterification.The acidity(H0)and Kamlet-Taft solvent parameters(hydrogen bond donor ability(α),hydrogen bond acceptor ability(β),and polarizability(π*))of ILs were measured by UV-Visible spectroscopy,and the effects of them on the diesterification of maleic anhydride were also studied in detail.The results indicated that not only H0 of the IL-based catalysis system,but also its α,β,and π* influenced the reaction activity of die-sterification.Furthermore,a quantifiable correlation was fitted between the natural logarithm of the rate constant and multiple parameters of ILs,indicating that the diesterification rate had a positive correlation with the H0,α,and π*,and inverse correlation with the β of the IL.A plausible synergetic reaction mechanism for the excellent performance of[(HSO3)PMim][HSO4]has been proposed.Overall,this work thoroughly explored the relationship between the nature of ILs on diesterification in-depth,which will reveal the nature of diesterification in detail.
查看更多>>摘要：Green synthesis of metal-organic frameworks(MOFs)in water with alleviated environmental influence and reduced cost is an essential step to transfer laboratory MOFs research to industrial application.Switching from the commonly used organic solvents to pure water encounters challenges of the poor solubility of organic linkers,slow reaction kinetics,and the formation of polymorphic products.So far,a universal MOFs synthetic strategy in water system has yet to be developed.This study reports the seed-aided synthesis of eleven MOFs with diverse compositions and structures while pure water serving as solvent.The corresponding reaction temperature and time of using this new strategy were reduced compared with original synthetic approaches,while the products maintain porous structure and high crystallinity.The success of this strategy relies on the addition of parent MOFs as seeds which could promote crystallization process by skipping the time-consuming induction period and avoiding the formation of polymorphic impurities.
查看更多>>摘要：The construction of rapid prototyping for structured ceramics has a promoting effect on potential applications.In this work,engineering slurry with different formulations were used to develop aqueous colloidal ceramic slurry for direct ink writing(DIW).Optimized slurry of Formulation 5 possessed good printing effect for DIW with stable mechanical properties.Related characteristics,including shrinkage,compressive strength,rheological behavior,and chemical property,were also examined.DIW ceramics prepared from optimized slurry can be preliminarily applied to adsorption of Rhodamine B and chlortetracycline,and possessed the advantages of easy separation and operation compared with powder adsorbents.This work provides a strategy for the design of 3D-printed kaolin ceramic slurry,and also extends to potential application in adsorption.
查看更多>>摘要：Natural gas processing involves the separation of higher hydrocarbons(C2-C3)from methane,which is an important and energy-intensive operation.In this paper,we present a comprehensive study of an innovative copper-based MOF(Cu-MOF)for the separation of propane and ethane from methane.The material exhibits a high adsorption capacity and selectivity for C2-C3 hydrocarbons over methane,which is primarily due to its preferential C2-C3 hydrocarbon adsorption.The adsorption isotherms at ambient conditions showed a remark-able uptake of C3H8 of 134.0 cm3/g,as well as excellent selectivity of 204 and 9 for C3H8/CH4 and C2H6/CH4.According to the theoretical calculations,differences in van der Waals interactions and polarizability of the guest molecules were responsible for influencing separation performance.In addition,we conducted adsorption kinetic experiments,dynamic breakthrough,and cycling experiments to further examine the separation performance.Overall,this research establishes an energy-efficient adsorbent for upgrading natural gas.
查看更多>>摘要：Water pollution caused by dye is a serious challenge.Herein,we use a novel discharge process to functionalize carbon nanotube(CNT)by COOH groups to form CNT30 for removing methyl red(MR)from water.By pristine CNT,75％MR is removed in 60 min,with an adsorption capacity of 68.44 mg g-1.By CNT30,85％MR is fast removed in only 5 min,and the removal efficiency reaches to 95％after 30 min,with an adsorption capacity of 80.33 mg g1.Thus,a higher MR removal efficiency is achieved in a much shorter time on CNT30.Moreover,CNT30 has an outstanding reusability,with the MR removal efficiency decreasing by only 7％after ten cycles.The COOH groups on CNT30 improve the hydrophilicity of CNT30,thus promoting the interaction of MR in water with CNT30.The hydrogen bonding and electrostatic interaction of MR with the COOH groups on CNT30 could be the force to drive MR adsorption on CNT30.The higher COOH content could be the origin for the better performance of CNT30 in removing dye from water.The discharge process developed herein is operated in O2,without using harmful substances,and the COOH content on CNT can be efficiently tuned by simply changing discharge time.This is different from the chemical modification widely used to functionalize CNT by strong oxidants,e.g.,HNO3.The present work is of great significance to realize green construction of materials for more efficiently removing dye from water.
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