Currently, the electrochemical CO_(2) reduction reaction (CO_(2) RR) can realize the resource conversion of CO_(2) , which is a promising approach to carbon resource use. Important advancements have been made in explo...Currently, the electrochemical CO_(2) reduction reaction (CO_(2) RR) can realize the resource conversion of CO_(2) , which is a promising approach to carbon resource use. Important advancements have been made in exploring the CO_(2) RR performance and mechanism because of the rational design of electrolyzer systems, such as H-cells, flow cells, and catalysts. Considering the future development direction of this technology and large-scale application needs, membrane electrode assembly (MEA) systems can improve energy use efficiency and achieve large-scale CO_(2) conversion, which is considered the most promising technology for industrial applications. This review will concentrate on the research progress and present situation of the MEA component structure. This paper begins with the composition and construction of a gas diff usion electrode. Then, the application of ion-exchange membranes in MEA is introduced. Furthermore, the eff ects of pH and the anion and cation of the anolyte on MEA performance are explored. Additionally, we present the anode reaction type in MEA. Finally, the challenges in this field are summarized, and upcoming trends are projected. This review should offer researchers a clearer picture of MEA systems and provide important, timely, and valuable insights into rational electrolyzer design to facilitate further development of CO_(2) electrochemical reduction.展开更多
Catalytic membrane reactors(CMRs),which synergistically carry out separations and reactions,are expected to become a green and sustainable technology in chemical engineering.The use of ceramic membranes in CMRs is bei...Catalytic membrane reactors(CMRs),which synergistically carry out separations and reactions,are expected to become a green and sustainable technology in chemical engineering.The use of ceramic membranes in CMRs is being widely considered because it permits reactions and separations to be carried out under harsh conditions in terms of both temperature and the chemical environment.This article presents the two most important types of CMRs:those based on dense mixed-conducting membranes for gas separation,and those based on porous ceramic membranes for heterogeneous catalytic processes.New developments in and innovative uses of both types of CMRs over the last decade are presented,along with an overview of our recent work in this field.Membrane reactor design,fabrication,and applications related to energy and environmental areas are highlighted.First,the configuration of membranes and membrane reactors are introduced for each of type of membrane reactor.Next,taking typical catalytic reactions as model systems,the design and optimization of CMRs are illustrated.Finally,challenges and difficulties in the process of industrializing the two types of CMRs are addressed,and a view of the future is outlined.展开更多
Due to the scale effect, the uniform distribution of reagents in continuous flow reactor becomes bad when the channel is enlarged to tens of millimeters. Microfluidic field strategy was proposed to produce high mixing...Due to the scale effect, the uniform distribution of reagents in continuous flow reactor becomes bad when the channel is enlarged to tens of millimeters. Microfluidic field strategy was proposed to produce high mixing efficiency in large-scale channel. A 3D spiral baffle structure(3SBS) was designed and optimized to form microfluidic field disturbed by continuous secondary flow in millimeter scale Y-shaped tube mixer(YSTM). Enhancement effect of the 3SBS in liquid-liquid homogeneous chemical processes was verified and evaluated through the combination of simulation and experiment. Compared with 1 mm YSTM, 10 mm YSTM with 3SBS increased the treatment capacity by 100 times, shortened the basic complete mixing time by 0.85 times, which proves the potential of microfluidic field strategy in enhancement and scale-up of liquid-liquid homogeneous chemical process.展开更多
The increasing concentration of CO2 in the atmosphere has led to the greenhouse effect,which greatly affects the climate and the ecological balance of nature.Therefore,converting CO2 into renewable fuels via clean and...The increasing concentration of CO2 in the atmosphere has led to the greenhouse effect,which greatly affects the climate and the ecological balance of nature.Therefore,converting CO2 into renewable fuels via clean and economical chemical processes has become a great concern for scientists.Electrocatalytic CO2 conversion is a prospective path toward carbon cycling.Among the different electrocatalysts,Sn-based electrocatalysts have been demonstrated as promising catalysts for CO2 electroreduction,producing formate and CO,which are important industrial chemicals.In this review,various Sn-based electrocatalysts are comprehensively summarized in terms of synthesis,catalytic performance,and reaction mechanisms for CO2 electroreduction.Finally,we concisely discuss the current challenges and opportunities of Sn-based electrocatalysts.展开更多
In modern chemical engineering processes, the involvement of solid/fluid interface is the most important component of process intensification techniques, such as confined membrane separation and catalysis. In the revi...In modern chemical engineering processes, the involvement of solid/fluid interface is the most important component of process intensification techniques, such as confined membrane separation and catalysis. In the review, we summarized the research progress of the latest theoretical and experimental works to elucidate the contribution of interface to the fluid properties and structures at nano-and micro-scale. We mainly focused on water, alcohol aqueous solution, and ionic liquids, because they are classical systems in interfacial science and/or widely involved in the industrialization process. Surface-induced fluids were observed in all reviewed systems and played a critical role in physicochemical properties and structures of outside fluid. It can even be regarded as a new interface, when the adsorption layer has a strong interaction with the solid surface. Finally, we proposed a perspective on scientific challenges in the modern chemical engineering processes and outlined future prospects.展开更多
Severe fouling to poly(vinylidene fluoride)(PVDF)membrane is usually caused as filtrating the papermaking wastewater in the ultrafiltration(UF)process.In the paper,fouling behavior and mechanism were investigated,and ...Severe fouling to poly(vinylidene fluoride)(PVDF)membrane is usually caused as filtrating the papermaking wastewater in the ultrafiltration(UF)process.In the paper,fouling behavior and mechanism were investigated,and the low-concentration polyvinyl alcohol(PVA)contained in the sedimentation tank wastewater was found as the main foulant.Consequently,the corresponding cleaning approach was proposed.The experiment and modeling results elaborated that the fouling mode developed from pore blockage to cake layer along with filtration time.Chemical cleaning conditions including the composition and concentration of reagents,cleaning duration and trans-membrane pressure were investigated for their effect on cleaning efficiency.Pure water flux was recovered by over 95% after cleaning the PVDF membrane using the optimal conditions 0.5 wt% NaClO(as oxidant)and 0.1 wt% sodiumdodecyl benzene sulfonate(SDBS,as surfactant)at 0.04MPa for 100 min.In the chemical cleaning method,hypochlorite(ClO−)could first chain-scissor PVA macromolecules to small molecules and SDBS could wrap the fragments in micelles,so that the foulants were removed from the pores and surface of membrane.After eight cycling tests,pure water flux recovery maintained above 95% and the reused membrane was found intact without defects.展开更多
A novel methodology for the formulation design of the multi-component cement additive for the low early strength blend cement was presented by using engineering statistics.Components of cement additive such as trietha...A novel methodology for the formulation design of the multi-component cement additive for the low early strength blend cement was presented by using engineering statistics.Components of cement additive such as triethanolamine,chloride,saccharide and a kind of divalent alcohol were simultaneously tested according to the arrangement of response surface methodology.Mathematical models were established to express the quantitative relationship between the chemical components of cement additive and the compressive strength of treated blend cement.The effectiveness and the possible interactions of these four chemicals contributing to the strength development of blend cement were further explored by the pareto chart and the contour plot.Finally according the performance analysis of four chemicals,the optimized formulations were brought forward and were validated in practical trials by Turkey's multiple comparison.展开更多
Electrochemical reduction of CO_(2) is a novel research field towards a CO_(2)-neutral global economy and combating fast accelerating and disastrous climate changes while finding new solutions to store renewable energ...Electrochemical reduction of CO_(2) is a novel research field towards a CO_(2)-neutral global economy and combating fast accelerating and disastrous climate changes while finding new solutions to store renewable energy in value-added chemicals and fuels.Ionic liquids(ILs),as medium and catalysts(or supporting part of catalysts)have been given wide attention in the electrochemical CO_(2) reduction reaction(CO_(2) RR)due to their unique advantages in lowering overpotential and improving the product selectivity,as well as their designable and tunable properties.In this review,we have summarized the recent progress of CO_(2) electro-reduction in IL-based electrolytes to produce higher-value chemicals.We then have highlighted the unique enhancing effect of ILs on CO_(2) RR as templates,precursors,and surface functional moieties of electrocatalytic materials.Finally,computational chemistry tools utilized to understand how the ILs facilitate the CO_(2) RR or to propose the reaction mechanisms,generated intermediates and products have been discussed.展开更多
Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2...Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2)RR)is still challenging owing to the sluggish kinetics or unfavorable thermodynamics for basic chemical processes of CO_(2)RR,such as adsorption,activation,conversion and product desorption.To overcome these shortcomings,recent works have demonstrated that surface engineering of semiconductors,such as introducing surface vacancy,surface doping,and cocatalyst loading,serves as effective or promising strategies for improved photocatalytic CO_(2)RR with high activity and selectivity.The essential reason lies in the activation and reaction pathways can be optimized and regulated through the reconstruction of surface atomic and electronic structures.Herein,in this review,we focus on recent research advances about rational design of semiconductor surface for photocatalytic CO_(2)RR.The surface engineering strategies for improved CO_(2)adsorption,activation,and product selectivity will be reviewed.In addition,theoretical calculations along with in situ characterization techniques will be in the spotlight to clarify the kinetics and thermodynamics of the reaction process.The aim of this review is to provide deep understanding and rational guidance on the design of semiconductors for photocatalytic CO_(2)RR.展开更多
Reversible proton ceramic electrochemical cell(R-PCEC)is regarded as the most promising energy conversion device,which can realize efficient mutual conversion of electrical and chemical energy and to solve the problem...Reversible proton ceramic electrochemical cell(R-PCEC)is regarded as the most promising energy conversion device,which can realize efficient mutual conversion of electrical and chemical energy and to solve the problem of large-scale energy storage.However,the development of robust electrodes with high catalytic activity is the main bottleneck for the commercialization of R-PCECs.Here,a novel type of high-entropy perovskite oxide consisting of six equimolar metals in the A-site,Pr_(1/6)La_(1/6)Nd_(1/6)Ba_(1/6)Sr_(1/6)Ca_(1/6)CoO_(3−δ)(PLN-BSCC),is reported as a high-performance bifunctional air electrode for R-PCEC.By harnessing the unique functionalities of multiple ele-ments,high-entropy perovskite oxide can be anticipated to accelerate reaction rates in both fuel cell and electrolysis modes.Especially,an R-PCEC utilizing the PLNBSCC air electrode achieves exceptional electrochemical performances,demonstrating a peak power density of 1.21 W cm^(−2)for the fuel cell,while simultaneously obtaining an astonishing current density of−1.95 A cm^(−2)at an electrolysis voltage of 1.3 V and a temperature of 600℃.The significantly enhanced electrochemical performance and durability of the PLNBSCC air electrode is attributed mainly to the high electrons/ions conductivity,fast hydration reactivity and high configurational entropy.This research explores to a new avenue to develop optimally active and stable air electrodes for R-PCECs.展开更多
Solid oxide fuel cells(SOFCs)and electrolysis cells(SOECs)are promising energy conversion devices,on whose basis green hydrogen energy technologies can be developed to support the transition to a carbon-free future.As...Solid oxide fuel cells(SOFCs)and electrolysis cells(SOECs)are promising energy conversion devices,on whose basis green hydrogen energy technologies can be developed to support the transition to a carbon-free future.As compared with oxygen-conducting cells,the operational temperatures of protonic ceramic fuel cells(PCFCs)and electrolysis cells(PCECs)can be reduced by several hundreds of degrees(down to low-and intermediatetemperature ranges of 400–700C)while maintaining high performance and efficiency.This is due to the distinctive characteristics of charge carriers for proton-conducting electrolytes.However,despite achieving outstanding lab-scale performance,the prospects for industrial scaling of PCFCs and PCECs remain hazy,at least in the near future,in contrast to commercially available SOFCs and SOECs.In this review,we reveal the reasons for the delayed technological development,which need to be addressed in order to transfer fundamental findings into industrial processes.Possible solutions to the identified problems are also highlighted.展开更多
Flexible solid-state battery has several unique characteristics including high flexibility,easy portability,and high safety,which may have broad application prospects in new technology products such as rollup displays...Flexible solid-state battery has several unique characteristics including high flexibility,easy portability,and high safety,which may have broad application prospects in new technology products such as rollup displays,power implantable medical devices,and wearable equipments.The interfacial mechanical and electrochemical problems caused by bending deformation,resulting in the battery damage and failure,are particularly interesting.Herein,a fully coupled electro-chemo-mechanical model is developed based on the actual solid-state battery structure.Concentration-dependent material parameters,stress-dependent diffusion,and potential shift are considered.According to four bending forms(k=8/mm,0/mm,-8/mm,and free),the results show that the negative curvature bending is beneficial to reducing the plastic strain during charging/discharging,while the positive curvature is detrimental.However,with respect to the electrochemical performance,the negative curvature bending creates a negative potential shift,which causes the battery to reach the cut-off voltage earlier and results in capacity loss.These results enlighten us that suitable electrode materials and charging strategy can be tailored to reduce plastic deformation and improve battery capacity for different forms of battery bending.展开更多
Methanol is becoming an attractive fermentation feedstock for large-scale bioproduction of chemicals,due to its natural abundance and mature production technology.Native methylotrophs,which can utilize methanol as the...Methanol is becoming an attractive fermentation feedstock for large-scale bioproduction of chemicals,due to its natural abundance and mature production technology.Native methylotrophs,which can utilize methanol as the only source of carbon and energy,are ideal hosts for methanol bioconversion due to their high methanol utili-zation rate and have been extensively employed in the production of value-added chemicals from methanol.Here,we review the natural methanol utilization pathways in native methylotrophs,describing the available synthetic biology tools developed for engineering native methylotrophs,and discuss the strategies for improving their methanol utilization efficiency.Finally,the representative examples of engineering the native methylotrophs to produce value-added products from methanol are summarized.Furthermore,we also discuss the major challenges and possible solutions for the application of native methylotrophs in methanol-based biomanufacturing.展开更多
Sodium-contained compounds are promising sintering additives for the low-temperature preparation of reaction bonded SiC membranes.Although sodium-based sintering additives in various original states were attempted,the...Sodium-contained compounds are promising sintering additives for the low-temperature preparation of reaction bonded SiC membranes.Although sodium-based sintering additives in various original states were attempted,their effects on microstructure and surface properties have rarely been studied.In this work,three types of sodium-based additives,including solid-state NaA zeolite residue(NaA)and liquidstate dodecylbenzene sulfonate(SDBS)and water glass(WG),were separately adopted to prepare SiC membranes,and the microstructure,surface characteristics and filtration performance of these SiC membranes were comparatively studied.Results showed that the SiC membranes prepared with liquid-state SDBS and WG(S-SDBS and S-WG)showed lower open porosity yet higher bending strength compared to those prepared with solid-state NaA(S-NaA).The observed differences in bending strength were further interpreted by analyzing the reaction process of each sintering additive and the composition of the bonding phase in the reaction bonded SiC membranes.Meanwhile,the microstructural differentiation was correlated to the original state of the additives.In addition,their surface characteristics and filtration performance for oil-in-water emulsion were examined and correlated to the membrane microstructure.The S-NaA samples showed higher hydrophilicity,lower surface roughness(1.80μm)and higher rejection ratio(99.99%)in O/W emulsion separation than those of S-WG and S-SDBS.This can be attributed to the smaller mean pore size and higher open porosity,resulting from the originally solid-state NaA additives.Therefore,this work revealed the comprehensive effects of original state of sintering additives on the prepared SiC membranes,which could be helpful for the application-oriented fabrication by choosing additives in suitable state.展开更多
β-lactoglobulin is an effective indicator of allergic protein detection.Herein,we produced a copper-based metal-organic framework coated with methylene blue,to realize the optical and electrochemical dual detection o...β-lactoglobulin is an effective indicator of allergic protein detection.Herein,we produced a copper-based metal-organic framework coated with methylene blue,to realize the optical and electrochemical dual detection ofβ-lactoglobulin.Methylene blue was successfully encapsulated inside the copper-based metal-organic framework and released after addition ofβ-lactoglobulin.As the concentration ofβ-lactoglobulin increased,the intensity of the ultraviolet absorption band and the response current increased with the increasing concentration of methylene blue released from the copper-based metal-organic framework.The optical detection range is from 0.10 mg/mL to 10 mg/mL,and the detection limit is 0.10 mg/mL.The electrochemical detection range is from 1.0×10^(-7) mg/mL to 8.0×10^(-7) mg/mL,the detection limit is 2.0×10^(-8) mg/mL.The dual detection strategy,with no interfere with each other,played a synergetic role in the quick qualitative and precise quantitative analyses ofβ-lactoglobulin in a wide range of applications.展开更多
The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability,environmental friendliness,and non-toxicity is of great importance.Herein,a series of Co-based catalysts,named...The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability,environmental friendliness,and non-toxicity is of great importance.Herein,a series of Co-based catalysts,named Co@NCNTs,were designed and constructed by direct pyrolysis of hollow ZIF-67(HZIF-67)under H_(2)/Ar atmosphere.The evolution of the catalyst surface from the shell layer assembled by ZIF-67-derived particles to the in situ-grown hollow nitrogen-doped carbon nanotubes(NCNTs)with certain length and density is achieved by adjusting the pyrolysis atmosphere and temperature.Due to the synergistic effects of in situ-formed hollow NCNTs,well-dispersed Co nanoparticles,and intact carbon matrix,the as-prepared Co@NCNTs-0.10-450 catalyst exhibits superior catalytic performance in the hydrogenation of phenolic compounds to alcohols.The turnover frequency value of Co@NCNTs-0.10-450is 3.52 h^(-1),5.9 times higher than that of Co@NCNTs-0.40-450 and 4.5 times higher than that of Co@NCNTs-0.10-550,exceeding most previously reported non-noble metal catalysts.Our findings provide new insights into the development of non-precious metal,efficient,and cost-effective metal-organic framework-derived catalysts for the hydrogenation of phenolic compounds to alcohols.展开更多
Water-quenched copper-nickel metallurgical slag enriched with olivine minerals exhibits promising potential for the production of CO_(2)-mineralized cementitious materials.In this work,copper-nickel slag-based cementi...Water-quenched copper-nickel metallurgical slag enriched with olivine minerals exhibits promising potential for the production of CO_(2)-mineralized cementitious materials.In this work,copper-nickel slag-based cementitious material(CNCM)was synthesized by using different chemical activation methods to enhance its hydration reactivity and CO_(2) mineralization capacity.Different water curing ages and carbonation conditions were explored related to their carbonation and mechanical properties development.Meanwhile,thermogravimetry differential scanning calorimetry and X-ray diffraction methods were applied to evaluate the CO_(2) adsorption amount and carbonation products of CNCM.Microstructure development of carbonated CNCM blocks was examined by backscattered electron imaging(BSE)with energy-dispersive X-ray spectrometry.Results showed that among the studied samples,the CNCM sample that was subjected to water curing for 3 d exhibited the highest CO_(2) sequestration amount of 8.51wt%at 80℃and 72 h while presenting the compressive strength of 39.07 MPa.This result indicated that 1 t of this CNCM can sequester 85.1 kg of CO_(2) and exhibit high compressive strength.Although the addition of citric acid did not improve strength development,it was beneficial to increase the CO_(2) diffusion and adsorption amount under the same carbonation conditions from BSE results.This work provides guidance for synthesizing CO_(2)-mineralized cementitious materials using large amounts of metallurgical slags containing olivine minerals.展开更多
Particle engineering has opened the floodgates to material science in both fundamental and application field. However, covalent interactions have not yet been adequately designed in the particle engineering for functi...Particle engineering has opened the floodgates to material science in both fundamental and application field. However, covalent interactions have not yet been adequately designed in the particle engineering for functional colloidal photonic crystals(CPCs). Herein, we achieved covalent coupling between carboxylrich poly(styrene-acrylic acid)(P(St-AA)) monodispersed colloidal particles and amine-rich carbon dots(CDs) based on an feasible and universal particle engineering strategy. The designed CDs-grafted P(St-AA)monodispersed colloidal particles initiate a hydrogen bond-driven assembly mode and ensure the construction of large-scale crack-free CPCs. Moreover, the CDs equipped with selective broad-band absorption capacity could improve the saturation of structural colors for high-visibility CPCs. Furthermore, an injectable photonic hydrogel(IPH) is developed to design CPC supraball hydrogel via integrating the CDsgrafted P(St-AA) CPC supraballs with supramolecular hydrogel. Combining superior flexibility, sufficient self-healing capacity of supramolecular hydrogel with visual optical information of our CPC supraballs, a cyclically reversible coding and decoding system was developed. Meanwhile, we firstly demonstrated the novel strategy of 3D supraballs-based passive cooling. The designed 3D CPC supraball hydrogel presents nearly full observation angle reflections behavior and excellent water evaporation capacity and achieves3.6 ℃ temperature drops, showing the application advantages in 3D thermal management. This work not only provides a new insight for manipulating optical properties of CPCs, but also demonstrates an easyto-perform platform, as well as indicates the direction for the promising application of CPCs.展开更多
Membrane technology has become the mainstream process for the production of electronic grade hydrogen peroxide(H_(2)O_(2)).But due to the oxidation degradation of the organic membranes(e.g.polyamide)by the strong oxid...Membrane technology has become the mainstream process for the production of electronic grade hydrogen peroxide(H_(2)O_(2)).But due to the oxidation degradation of the organic membranes(e.g.polyamide)by the strong oxidative radicals(e.g.OH)generated via the activation of H_(2)O_(2)by iron ions(Fe^(3+)),the short effective lifetime of membranes remains a challenge.Inorganic nano tin oxide(SnO_(2))has great potential for the removal of Fe^(3+)in strongly oxidative H_(2)O_(2)because of its ability to stabilize H2O_(2)and preferentially adsorb Fe^(3+).Herein,we have designed for the first time a flower-like robust SnO_(2)membrane on the ceramic support by in situ template-free one-step hydrothermal method.The three-dimensional loose pore structure in the membrane built by interlacing SnO_(2)nanosheets endows the SnO_(2)membrane with a high specific surface area and abundant adsorption sites(AOH).Based on the coordination complexation and electrostatic attraction between the SnO_(2)surface and Fe^(3+),the membrane shows a high Fe3+removal efficiency(83%)and permeability(24 L·m^(-2)·h^(-1)·MPa^(-1))in H_(2)O_(2).This study provides an innovative and simple approach to designing robust SnO_(2)membranes for highly efficient removal of Fe^(3+)in harsh environments,such as strong oxidation conditions.展开更多
基金The financial assistance for this work was provided by the National Natural Science Foundation of China (Nos. 51773092, 21975124, 20210283, and 22109070)the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (No. SKL201911SIC).
文摘Currently, the electrochemical CO_(2) reduction reaction (CO_(2) RR) can realize the resource conversion of CO_(2) , which is a promising approach to carbon resource use. Important advancements have been made in exploring the CO_(2) RR performance and mechanism because of the rational design of electrolyzer systems, such as H-cells, flow cells, and catalysts. Considering the future development direction of this technology and large-scale application needs, membrane electrode assembly (MEA) systems can improve energy use efficiency and achieve large-scale CO_(2) conversion, which is considered the most promising technology for industrial applications. This review will concentrate on the research progress and present situation of the MEA component structure. This paper begins with the composition and construction of a gas diff usion electrode. Then, the application of ion-exchange membranes in MEA is introduced. Furthermore, the eff ects of pH and the anion and cation of the anolyte on MEA performance are explored. Additionally, we present the anode reaction type in MEA. Finally, the challenges in this field are summarized, and upcoming trends are projected. This review should offer researchers a clearer picture of MEA systems and provide important, timely, and valuable insights into rational electrolyzer design to facilitate further development of CO_(2) electrochemical reduction.
基金the National Natural Science Foundation of China(20990222,21006047,21706117,and 21706118)the Natural Science Foundation of Jiangsu(BK20170978 and BK20170970)+1 种基金the State Key Laboratory of Material-Oriented Chemical Engineering(ZK201609)the Innovative Research Team Program by the Ministry of Education of China(IRT17R54).
文摘Catalytic membrane reactors(CMRs),which synergistically carry out separations and reactions,are expected to become a green and sustainable technology in chemical engineering.The use of ceramic membranes in CMRs is being widely considered because it permits reactions and separations to be carried out under harsh conditions in terms of both temperature and the chemical environment.This article presents the two most important types of CMRs:those based on dense mixed-conducting membranes for gas separation,and those based on porous ceramic membranes for heterogeneous catalytic processes.New developments in and innovative uses of both types of CMRs over the last decade are presented,along with an overview of our recent work in this field.Membrane reactor design,fabrication,and applications related to energy and environmental areas are highlighted.First,the configuration of membranes and membrane reactors are introduced for each of type of membrane reactor.Next,taking typical catalytic reactions as model systems,the design and optimization of CMRs are illustrated.Finally,challenges and difficulties in the process of industrializing the two types of CMRs are addressed,and a view of the future is outlined.
基金supported by the National Key Research and Development Program of China (2021YFC2101900 and 2019YFA0905000)National Natural Science Foundation of China (21908094, 21776130 and 22078150)+1 种基金Nanjing International Joint Research and Development Project (202002037)Top-notch Academic Programs Project of Jiangsu Higher Education Institutions。
文摘Due to the scale effect, the uniform distribution of reagents in continuous flow reactor becomes bad when the channel is enlarged to tens of millimeters. Microfluidic field strategy was proposed to produce high mixing efficiency in large-scale channel. A 3D spiral baffle structure(3SBS) was designed and optimized to form microfluidic field disturbed by continuous secondary flow in millimeter scale Y-shaped tube mixer(YSTM). Enhancement effect of the 3SBS in liquid-liquid homogeneous chemical processes was verified and evaluated through the combination of simulation and experiment. Compared with 1 mm YSTM, 10 mm YSTM with 3SBS increased the treatment capacity by 100 times, shortened the basic complete mixing time by 0.85 times, which proves the potential of microfluidic field strategy in enhancement and scale-up of liquid-liquid homogeneous chemical process.
基金financial support from the 1000 Youth Talents Plan of National Natural Science Foundation of China(No.51773092)Research Foundation of State Key Lab(ZK201717)+2 种基金the Distinguished Young Scientists Program of the National Natural Science Foundation of China(Nos.51425301,21374021,51673096,and U1601214)the China Postdoctoral Science Foundation(2019M651813)the Youth Project of the Natural Science Foundation of Jiangsu Province,China(BK20171008).
文摘The increasing concentration of CO2 in the atmosphere has led to the greenhouse effect,which greatly affects the climate and the ecological balance of nature.Therefore,converting CO2 into renewable fuels via clean and economical chemical processes has become a great concern for scientists.Electrocatalytic CO2 conversion is a prospective path toward carbon cycling.Among the different electrocatalysts,Sn-based electrocatalysts have been demonstrated as promising catalysts for CO2 electroreduction,producing formate and CO,which are important industrial chemicals.In this review,various Sn-based electrocatalysts are comprehensively summarized in terms of synthesis,catalytic performance,and reaction mechanisms for CO2 electroreduction.Finally,we concisely discuss the current challenges and opportunities of Sn-based electrocatalysts.
基金supported by the National Natural Science Foundation of China [21878144, 21729601, 21838004]the Foundation for Innovative Research Groups of the National Natural Science Foundation of China [21921006]+3 种基金Project of Jiangsu Natural Science Foundation of China [BK20171464]Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)the Kempe Foundation in Swedengrant of Ministry of Research and Innovation, CNCS-UEFISCDI, Romania, project number PN-III-P4-ID-PCCF-2016-0050, within PNCDI III and the Swedish Science Council (VR)。
文摘In modern chemical engineering processes, the involvement of solid/fluid interface is the most important component of process intensification techniques, such as confined membrane separation and catalysis. In the review, we summarized the research progress of the latest theoretical and experimental works to elucidate the contribution of interface to the fluid properties and structures at nano-and micro-scale. We mainly focused on water, alcohol aqueous solution, and ionic liquids, because they are classical systems in interfacial science and/or widely involved in the industrialization process. Surface-induced fluids were observed in all reviewed systems and played a critical role in physicochemical properties and structures of outside fluid. It can even be regarded as a new interface, when the adsorption layer has a strong interaction with the solid surface. Finally, we proposed a perspective on scientific challenges in the modern chemical engineering processes and outlined future prospects.
基金financially supported by the National Natural Science Foundation of China(21921006).
文摘Severe fouling to poly(vinylidene fluoride)(PVDF)membrane is usually caused as filtrating the papermaking wastewater in the ultrafiltration(UF)process.In the paper,fouling behavior and mechanism were investigated,and the low-concentration polyvinyl alcohol(PVA)contained in the sedimentation tank wastewater was found as the main foulant.Consequently,the corresponding cleaning approach was proposed.The experiment and modeling results elaborated that the fouling mode developed from pore blockage to cake layer along with filtration time.Chemical cleaning conditions including the composition and concentration of reagents,cleaning duration and trans-membrane pressure were investigated for their effect on cleaning efficiency.Pure water flux was recovered by over 95% after cleaning the PVDF membrane using the optimal conditions 0.5 wt% NaClO(as oxidant)and 0.1 wt% sodiumdodecyl benzene sulfonate(SDBS,as surfactant)at 0.04MPa for 100 min.In the chemical cleaning method,hypochlorite(ClO−)could first chain-scissor PVA macromolecules to small molecules and SDBS could wrap the fragments in micelles,so that the foulants were removed from the pores and surface of membrane.After eight cycling tests,pure water flux recovery maintained above 95% and the reused membrane was found intact without defects.
基金Funded by National Basic Research Program of China (No.2009CB623100)
文摘A novel methodology for the formulation design of the multi-component cement additive for the low early strength blend cement was presented by using engineering statistics.Components of cement additive such as triethanolamine,chloride,saccharide and a kind of divalent alcohol were simultaneously tested according to the arrangement of response surface methodology.Mathematical models were established to express the quantitative relationship between the chemical components of cement additive and the compressive strength of treated blend cement.The effectiveness and the possible interactions of these four chemicals contributing to the strength development of blend cement were further explored by the pareto chart and the contour plot.Finally according the performance analysis of four chemicals,the optimized formulations were brought forward and were validated in practical trials by Turkey's multiple comparison.
基金F.Li and X.Ji thank the financial support from the Swedish Energy Agency(P47500-1)A.Laaksonen acknowledges the Swedish Research Council for financial support(2019-03865)+1 种基金partial support from a grant from Ministry of Research and Innovation of Romania(CNCS-UEFISCDI,project number PN-IIIP4-ID-PCCF-2016-0050,within PNCDI III)F.Mocci thanks the Fondazione di Sardegna,Project:“Precious metal-free complexes for catalytic CO2 reduction”(CUP:F71I17000170002)for the financial support.
文摘Electrochemical reduction of CO_(2) is a novel research field towards a CO_(2)-neutral global economy and combating fast accelerating and disastrous climate changes while finding new solutions to store renewable energy in value-added chemicals and fuels.Ionic liquids(ILs),as medium and catalysts(or supporting part of catalysts)have been given wide attention in the electrochemical CO_(2) reduction reaction(CO_(2) RR)due to their unique advantages in lowering overpotential and improving the product selectivity,as well as their designable and tunable properties.In this review,we have summarized the recent progress of CO_(2) electro-reduction in IL-based electrolytes to produce higher-value chemicals.We then have highlighted the unique enhancing effect of ILs on CO_(2) RR as templates,precursors,and surface functional moieties of electrocatalytic materials.Finally,computational chemistry tools utilized to understand how the ILs facilitate the CO_(2) RR or to propose the reaction mechanisms,generated intermediates and products have been discussed.
基金financially supported by JSPS KAKENHI(JP18H02065)Photo-excitonic Project in Hokkaido University,National Natural Science Foundation of China(21633004,22002060,and 51872138)+4 种基金Natural Science Foundation of Jiangsu Province(BK20181380)Qing Lan Project,Six Talent Peaks Project in Jiangsu Province(XCL-029)Priority Academic Program Development of the Jiangsu Higher Education Institutions(PAPD)the support provided by the China Scholarships Council(202008320109)China Postdoctoral Science Foundation(2020M681564)。
文摘Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2)RR)is still challenging owing to the sluggish kinetics or unfavorable thermodynamics for basic chemical processes of CO_(2)RR,such as adsorption,activation,conversion and product desorption.To overcome these shortcomings,recent works have demonstrated that surface engineering of semiconductors,such as introducing surface vacancy,surface doping,and cocatalyst loading,serves as effective or promising strategies for improved photocatalytic CO_(2)RR with high activity and selectivity.The essential reason lies in the activation and reaction pathways can be optimized and regulated through the reconstruction of surface atomic and electronic structures.Herein,in this review,we focus on recent research advances about rational design of semiconductor surface for photocatalytic CO_(2)RR.The surface engineering strategies for improved CO_(2)adsorption,activation,and product selectivity will be reviewed.In addition,theoretical calculations along with in situ characterization techniques will be in the spotlight to clarify the kinetics and thermodynamics of the reaction process.The aim of this review is to provide deep understanding and rational guidance on the design of semiconductors for photocatalytic CO_(2)RR.
基金The work was supported by National Natural Science Foundation of China(21878158 and 21706129)State Key Laboratory of Clean Energy Utilization(Open Fund Project No.ZJUCEU2021001)Natural Science Foundation of Jiangsu Province(BK20221312).
文摘Reversible proton ceramic electrochemical cell(R-PCEC)is regarded as the most promising energy conversion device,which can realize efficient mutual conversion of electrical and chemical energy and to solve the problem of large-scale energy storage.However,the development of robust electrodes with high catalytic activity is the main bottleneck for the commercialization of R-PCECs.Here,a novel type of high-entropy perovskite oxide consisting of six equimolar metals in the A-site,Pr_(1/6)La_(1/6)Nd_(1/6)Ba_(1/6)Sr_(1/6)Ca_(1/6)CoO_(3−δ)(PLN-BSCC),is reported as a high-performance bifunctional air electrode for R-PCEC.By harnessing the unique functionalities of multiple ele-ments,high-entropy perovskite oxide can be anticipated to accelerate reaction rates in both fuel cell and electrolysis modes.Especially,an R-PCEC utilizing the PLNBSCC air electrode achieves exceptional electrochemical performances,demonstrating a peak power density of 1.21 W cm^(−2)for the fuel cell,while simultaneously obtaining an astonishing current density of−1.95 A cm^(−2)at an electrolysis voltage of 1.3 V and a temperature of 600℃.The significantly enhanced electrochemical performance and durability of the PLNBSCC air electrode is attributed mainly to the high electrons/ions conductivity,fast hydration reactivity and high configurational entropy.This research explores to a new avenue to develop optimally active and stable air electrodes for R-PCECs.
文摘Solid oxide fuel cells(SOFCs)and electrolysis cells(SOECs)are promising energy conversion devices,on whose basis green hydrogen energy technologies can be developed to support the transition to a carbon-free future.As compared with oxygen-conducting cells,the operational temperatures of protonic ceramic fuel cells(PCFCs)and electrolysis cells(PCECs)can be reduced by several hundreds of degrees(down to low-and intermediatetemperature ranges of 400–700C)while maintaining high performance and efficiency.This is due to the distinctive characteristics of charge carriers for proton-conducting electrolytes.However,despite achieving outstanding lab-scale performance,the prospects for industrial scaling of PCFCs and PCECs remain hazy,at least in the near future,in contrast to commercially available SOFCs and SOECs.In this review,we reveal the reasons for the delayed technological development,which need to be addressed in order to transfer fundamental findings into industrial processes.Possible solutions to the identified problems are also highlighted.
基金the National Natural Science Foundation of China(No.11902144)the Postgraduate Research&Practice Innovation Program of Jiangsu Province of China(No.KYCX201074)+1 种基金the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.19KJB430022)the Guizhou Provincial General Undergraduate Higher Education Technology Supporting Talent Support Program(No.KY(2018)043)。
文摘Flexible solid-state battery has several unique characteristics including high flexibility,easy portability,and high safety,which may have broad application prospects in new technology products such as rollup displays,power implantable medical devices,and wearable equipments.The interfacial mechanical and electrochemical problems caused by bending deformation,resulting in the battery damage and failure,are particularly interesting.Herein,a fully coupled electro-chemo-mechanical model is developed based on the actual solid-state battery structure.Concentration-dependent material parameters,stress-dependent diffusion,and potential shift are considered.According to four bending forms(k=8/mm,0/mm,-8/mm,and free),the results show that the negative curvature bending is beneficial to reducing the plastic strain during charging/discharging,while the positive curvature is detrimental.However,with respect to the electrochemical performance,the negative curvature bending creates a negative potential shift,which causes the battery to reach the cut-off voltage earlier and results in capacity loss.These results enlighten us that suitable electrode materials and charging strategy can be tailored to reduce plastic deformation and improve battery capacity for different forms of battery bending.
基金supported by the National Key Research and Development Program of China(Grant No.2018YFA0901500)the Jiangsu Synergetic Innovation Center for Advanced Bio-Manufacture(XTD2218).
文摘Methanol is becoming an attractive fermentation feedstock for large-scale bioproduction of chemicals,due to its natural abundance and mature production technology.Native methylotrophs,which can utilize methanol as the only source of carbon and energy,are ideal hosts for methanol bioconversion due to their high methanol utili-zation rate and have been extensively employed in the production of value-added chemicals from methanol.Here,we review the natural methanol utilization pathways in native methylotrophs,describing the available synthetic biology tools developed for engineering native methylotrophs,and discuss the strategies for improving their methanol utilization efficiency.Finally,the representative examples of engineering the native methylotrophs to produce value-added products from methanol are summarized.Furthermore,we also discuss the major challenges and possible solutions for the application of native methylotrophs in methanol-based biomanufacturing.
基金financially supported by the National Key Research and Development Program of China(2022YFB3805002)the National Natural Science Foundation of China(21838005)+2 种基金the Innovative Research Groups of the National Natural Science Foundation of China(21921006)the Natural Science Foundation of Jiangsu Province(BK20220345)Youth Science and Technology Talents Lifting Project of Jiangsu Association of Science and Technology(105019ZS_007)。
文摘Sodium-contained compounds are promising sintering additives for the low-temperature preparation of reaction bonded SiC membranes.Although sodium-based sintering additives in various original states were attempted,their effects on microstructure and surface properties have rarely been studied.In this work,three types of sodium-based additives,including solid-state NaA zeolite residue(NaA)and liquidstate dodecylbenzene sulfonate(SDBS)and water glass(WG),were separately adopted to prepare SiC membranes,and the microstructure,surface characteristics and filtration performance of these SiC membranes were comparatively studied.Results showed that the SiC membranes prepared with liquid-state SDBS and WG(S-SDBS and S-WG)showed lower open porosity yet higher bending strength compared to those prepared with solid-state NaA(S-NaA).The observed differences in bending strength were further interpreted by analyzing the reaction process of each sintering additive and the composition of the bonding phase in the reaction bonded SiC membranes.Meanwhile,the microstructural differentiation was correlated to the original state of the additives.In addition,their surface characteristics and filtration performance for oil-in-water emulsion were examined and correlated to the membrane microstructure.The S-NaA samples showed higher hydrophilicity,lower surface roughness(1.80μm)and higher rejection ratio(99.99%)in O/W emulsion separation than those of S-WG and S-SDBS.This can be attributed to the smaller mean pore size and higher open porosity,resulting from the originally solid-state NaA additives.Therefore,this work revealed the comprehensive effects of original state of sintering additives on the prepared SiC membranes,which could be helpful for the application-oriented fabrication by choosing additives in suitable state.
基金supported by the National Key R&D Program of China (2017YFC1600404)the National Natural Science Foundation of China (31922070,U2106228)the Jiangsu Synergetic Innovation Center for Advanced Bio-Manufacture (XTC2205).
文摘β-lactoglobulin is an effective indicator of allergic protein detection.Herein,we produced a copper-based metal-organic framework coated with methylene blue,to realize the optical and electrochemical dual detection ofβ-lactoglobulin.Methylene blue was successfully encapsulated inside the copper-based metal-organic framework and released after addition ofβ-lactoglobulin.As the concentration ofβ-lactoglobulin increased,the intensity of the ultraviolet absorption band and the response current increased with the increasing concentration of methylene blue released from the copper-based metal-organic framework.The optical detection range is from 0.10 mg/mL to 10 mg/mL,and the detection limit is 0.10 mg/mL.The electrochemical detection range is from 1.0×10^(-7) mg/mL to 8.0×10^(-7) mg/mL,the detection limit is 2.0×10^(-8) mg/mL.The dual detection strategy,with no interfere with each other,played a synergetic role in the quick qualitative and precise quantitative analyses ofβ-lactoglobulin in a wide range of applications.
基金the National Key Research and Development Program(2021YFC3001103)the National Natural Science Foundation(22278209,22178165,21921006,22208149)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20211262,BK20220354)a project funded by the priority academic program development of Jiangsu higher education institutions(PAPD)of China。
文摘The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability,environmental friendliness,and non-toxicity is of great importance.Herein,a series of Co-based catalysts,named Co@NCNTs,were designed and constructed by direct pyrolysis of hollow ZIF-67(HZIF-67)under H_(2)/Ar atmosphere.The evolution of the catalyst surface from the shell layer assembled by ZIF-67-derived particles to the in situ-grown hollow nitrogen-doped carbon nanotubes(NCNTs)with certain length and density is achieved by adjusting the pyrolysis atmosphere and temperature.Due to the synergistic effects of in situ-formed hollow NCNTs,well-dispersed Co nanoparticles,and intact carbon matrix,the as-prepared Co@NCNTs-0.10-450 catalyst exhibits superior catalytic performance in the hydrogenation of phenolic compounds to alcohols.The turnover frequency value of Co@NCNTs-0.10-450is 3.52 h^(-1),5.9 times higher than that of Co@NCNTs-0.40-450 and 4.5 times higher than that of Co@NCNTs-0.10-550,exceeding most previously reported non-noble metal catalysts.Our findings provide new insights into the development of non-precious metal,efficient,and cost-effective metal-organic framework-derived catalysts for the hydrogenation of phenolic compounds to alcohols.
基金supported by the Intergovernmental International Science and Technology Innovation Cooperation Key Project of the National Key Research and Development Program of China (No.2022YFE0135100)the National Natural Science Foundation of China (No.52072171)+1 种基金the Beijing Nova Program (No.20220484057)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).
文摘Water-quenched copper-nickel metallurgical slag enriched with olivine minerals exhibits promising potential for the production of CO_(2)-mineralized cementitious materials.In this work,copper-nickel slag-based cementitious material(CNCM)was synthesized by using different chemical activation methods to enhance its hydration reactivity and CO_(2) mineralization capacity.Different water curing ages and carbonation conditions were explored related to their carbonation and mechanical properties development.Meanwhile,thermogravimetry differential scanning calorimetry and X-ray diffraction methods were applied to evaluate the CO_(2) adsorption amount and carbonation products of CNCM.Microstructure development of carbonated CNCM blocks was examined by backscattered electron imaging(BSE)with energy-dispersive X-ray spectrometry.Results showed that among the studied samples,the CNCM sample that was subjected to water curing for 3 d exhibited the highest CO_(2) sequestration amount of 8.51wt%at 80℃and 72 h while presenting the compressive strength of 39.07 MPa.This result indicated that 1 t of this CNCM can sequester 85.1 kg of CO_(2) and exhibit high compressive strength.Although the addition of citric acid did not improve strength development,it was beneficial to increase the CO_(2) diffusion and adsorption amount under the same carbonation conditions from BSE results.This work provides guidance for synthesizing CO_(2)-mineralized cementitious materials using large amounts of metallurgical slags containing olivine minerals.
基金supported by the National Natural Science Foundation of China (No. 22278225)Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)。
文摘Particle engineering has opened the floodgates to material science in both fundamental and application field. However, covalent interactions have not yet been adequately designed in the particle engineering for functional colloidal photonic crystals(CPCs). Herein, we achieved covalent coupling between carboxylrich poly(styrene-acrylic acid)(P(St-AA)) monodispersed colloidal particles and amine-rich carbon dots(CDs) based on an feasible and universal particle engineering strategy. The designed CDs-grafted P(St-AA)monodispersed colloidal particles initiate a hydrogen bond-driven assembly mode and ensure the construction of large-scale crack-free CPCs. Moreover, the CDs equipped with selective broad-band absorption capacity could improve the saturation of structural colors for high-visibility CPCs. Furthermore, an injectable photonic hydrogel(IPH) is developed to design CPC supraball hydrogel via integrating the CDsgrafted P(St-AA) CPC supraballs with supramolecular hydrogel. Combining superior flexibility, sufficient self-healing capacity of supramolecular hydrogel with visual optical information of our CPC supraballs, a cyclically reversible coding and decoding system was developed. Meanwhile, we firstly demonstrated the novel strategy of 3D supraballs-based passive cooling. The designed 3D CPC supraball hydrogel presents nearly full observation angle reflections behavior and excellent water evaporation capacity and achieves3.6 ℃ temperature drops, showing the application advantages in 3D thermal management. This work not only provides a new insight for manipulating optical properties of CPCs, but also demonstrates an easyto-perform platform, as well as indicates the direction for the promising application of CPCs.
基金support from the National Key Research and Development Program(2021YFB3801303)the National Natural Science Foundation of China(21838005,21921006)+1 种基金the State Key Laboratory of Materials-Oriented Chemical Engineering(SKL-MCE-22A03)the Key Research and Development Program of Jiangsu Provincial Department of Science and Technology(BE2022033-3).
文摘Membrane technology has become the mainstream process for the production of electronic grade hydrogen peroxide(H_(2)O_(2)).But due to the oxidation degradation of the organic membranes(e.g.polyamide)by the strong oxidative radicals(e.g.OH)generated via the activation of H_(2)O_(2)by iron ions(Fe^(3+)),the short effective lifetime of membranes remains a challenge.Inorganic nano tin oxide(SnO_(2))has great potential for the removal of Fe^(3+)in strongly oxidative H_(2)O_(2)because of its ability to stabilize H2O_(2)and preferentially adsorb Fe^(3+).Herein,we have designed for the first time a flower-like robust SnO_(2)membrane on the ceramic support by in situ template-free one-step hydrothermal method.The three-dimensional loose pore structure in the membrane built by interlacing SnO_(2)nanosheets endows the SnO_(2)membrane with a high specific surface area and abundant adsorption sites(AOH).Based on the coordination complexation and electrostatic attraction between the SnO_(2)surface and Fe^(3+),the membrane shows a high Fe3+removal efficiency(83%)and permeability(24 L·m^(-2)·h^(-1)·MPa^(-1))in H_(2)O_(2).This study provides an innovative and simple approach to designing robust SnO_(2)membranes for highly efficient removal of Fe^(3+)in harsh environments,such as strong oxidation conditions.
