Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from t...Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from the air,lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies.A structured adsorbent is essential for the implementation of gas-solid contactors for cost-and energy-efficient DAC systems.In this study,efficient adsorbent poly(ethyleneimine)(PEI)-functionalized Mg-Al-CO_(3)layered double hydroxide(LDH)-derived mixed metal oxides(MMOs)are three-dimensional(3D)printed into monoliths for the first time with more than 90%adsorbent loadings.The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths.This structure exhibits a 32.7%higher specific surface area and a 46.1%higher pore volume,as compared to the direct printing of the MMO powder into a monolith.After impregnation of PEI,the monolith demonstrates a large adsorption capacity(1.82 mmol/g)and fast kinetics(0.7 mmol/g/h)using a CO_(2)feed gas at 400 ppm at 25℃,one of the highest values among the shaped DAC adsorbents.Smearing of the amino-polymers during the post-printing process affects the diffusion of CO_(2),resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths.The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.展开更多
Due to the advantages of low energy consumption and high CO_(2) selectivity, the development of solid amine-based materials has been regarded as a hot research topic in the field of DAC for the past decades.The adsorp...Due to the advantages of low energy consumption and high CO_(2) selectivity, the development of solid amine-based materials has been regarded as a hot research topic in the field of DAC for the past decades.The adsorption capacity and stability over multiple cycles have been the top priorities for evaluation of practical application value. Herein, we synthesized a novel DAC material by loading TEPA onto defect-rich Mg_(0.55)Al-O MMOs with enhanced charge transfer effect. The optimal Mg_(0.55)Al-O-TEPA67% demonstrates the highest CO_(2)uptake of(3.0 mmol g^(-1)) and excellent regenerability, maintaining ~90% of the initial adsorption amount after 80 adsorption/desorption cycles. The in situ DRIFTS experiments suggested the formation of bicarbonate species under wet conditions. DFT calculations indicated that the stronger bonding between Mg_(0.55)Al-O support and solid amine was caused by the abundance of oxygen defects on MMOs confirmed by XPS and ESR, which favors the charge transfer between the support and amine,resulting in intense interaction and excellent regenerability. This work for the first time conducted comprehensive and systematic investigation on the stabilization mechanism for MMOs supported solid amine adsorbents with highest uptake and superior cyclic stability in depth, which is different from the most popular SiO_(2)-support, thus providing facile strategy and comprehensive theoretical mechanism support for future research about DAC materials.展开更多
Potassium carbonate-based sorbents are prospective materials for direct air capture(DAC).In the present study,we examined and revealed the influence of the temperature swing adsorption(TSA)cycle conditions on the CO_(...Potassium carbonate-based sorbents are prospective materials for direct air capture(DAC).In the present study,we examined and revealed the influence of the temperature swing adsorption(TSA)cycle conditions on the CO_(2) sorption properties of a novel aerogel-based K_(2)CO_(3)/ZrO_(2) sorbent in a DAC process.It was shown that the humidity and temperature drastically affect the sorption dynamic and sorption capacity of the sorbent.When a temperature at the sorption stage was 29℃ and a water vapor pressure P_(H2O) in the feed air was 5.2 mbar(1 bar=105 Pa),the composite material demonstrated a stable CO_(2) sorption capacity of 3.4%(mass).An increase in sorption temperature leads to a continuous decrease in the CO_(2) absorption capacity reaching a value of 0.7%(mass)at T=80℃.The material showed the retention of a stable CO_(2) sorption capacity for many cycles at each temperature in the range.Increasing PH2O in the inlet air from 5.2 to 6.8 mbar leads to instability of CO_(2) sorption capacity which decreases in the course of 3 consecutive TSA cycles from 1.7%to 0.8%(mass)at T=29℃.A further increase in air humidity only facilitates the deterioration of the CO_(2) sorption capacity of the material.A possible explanation for this phenomenon could be the filling of the porous system of the sorbent with solid reaction products and an aqueous solution of potassium salts,which leads to a significant slowdown in the CO_(2) diffusion in the composite sorbent grain.To investigate the regeneration step of the TSA cycle in situ,the macro ATRFTIR(attenuated total reflection Fourier-transform infrared)spectroscopic imaging was applied for the first time.It was shown that the migration of carbonate-containing species over the surface of sorbent occurs during the thermal regeneration stage of the TSA cycle.The movement of the active component in the porous matrix of the sorbent can affect the sorption characteristics of the composite material.The revealed features make it possible to formulate the requirements and limitations that need to be taken into account for the practical implementation of the DAC process using the K_(2)CO_(3)/ZrO_(2) composite sorbent.展开更多
A high-level technology is revealed that can effectively convert any distributed system into a globally programmable machine capable of operating without central resources and self-recovering from indiscriminate damag...A high-level technology is revealed that can effectively convert any distributed system into a globally programmable machine capable of operating without central resources and self-recovering from indiscriminate damages. Integral mission scenarios in Distributed Scenario Language (DSL) can be injected from any point, runtime covering & grasping the whole system or its parts, setting operational infrastructures, and orienting local and global behavior in the way needed. Many operational scenarios can be simultaneously injected into this spatial machine from different points, cooperating or competing over the shared distributed knowledge as overlapping fields of solutions. Distributed DSL interpreter organization and benefits of using this technology for integrated air and missile defense are discussed along with programming examples in this and other fields.展开更多
美国定向能机动近程防空(directed energy maneuver-short range air defense,DE M-SHORAD)计划通过击伤、摧毁或压制旋转翼无人机、固定翼无人机以及火箭弹、火炮炮弹、迫击炮弹(rockets,artillery and mortar,RAM)等威胁目标,为机动...美国定向能机动近程防空(directed energy maneuver-short range air defense,DE M-SHORAD)计划通过击伤、摧毁或压制旋转翼无人机、固定翼无人机以及火箭弹、火炮炮弹、迫击炮弹(rockets,artillery and mortar,RAM)等威胁目标,为机动部队提供伴随防空,对抗新兴威胁,属于美国陆军防空反导现代化的优先项目之一。首先介绍了DE M-SHORAD研制计划;其次详细分析了系统结构,并由系统参数评估了系统的作战性能;最后梳理了系统的研制进展。通过综合分析可知,DE M-SHORAD系统采用最佳组件,通过快速原型方法实现激光武器系统在装甲车上的集成;为降低技术风险,该计划在发展方式上分为两个阶段,首先集成、测试2 kW~5 kW机动实验型高能激光器(mobile experimental high-energy laser,MEHEL),然后再研制50 kW级的多任务高能激光器(multi-mission high-energy laser,MMHEL)。经计算可得:MEHEL和MMHEL对无人机的最大射程分别约为0.77 km、4.8 km。展开更多
Temperature and humidity are two important factors that influence both indoor thermal comfort and air quality.Through varying compressor and supply fan speeds of a direct expansion(DX)air conditioning(A/C)unit,the air...Temperature and humidity are two important factors that influence both indoor thermal comfort and air quality.Through varying compressor and supply fan speeds of a direct expansion(DX)air conditioning(A/C)unit,the air temperature and humidity in the conditioned space can be regulated simultaneously.However,most existing controllers are designed to minimize the tracking errors between the system outputs with their corresponding settings as quickly as possible.The energy consumption,which is directly influenced by the compressor and supply fan speeds,is not considered in the relevant controller formulations,and thus the system may not operate with the highest possible energy efficiency.To effectively control temperature and humidity while minimizing the system energy consumption,a model predictive control(MPC)strategy was developed for a DX A/C system,and the development results are presented in this paper.A physically-based dynamic model for the DX A/C system with both sensible and latent heat transfers being considered was established and validated by experiments.To facilitate the design of MPC,the physical model was further linearized.The MPC scheme was then developed by formulating the objective function which sought to minimize the tracking errors of temperature and moisture content while saving energy consumption.Based on the results of command following and disturbance rejection tests,the proposed MPC scheme was capable of controlling temperature and humidity with adequate control accuracy and sensitivity.In comparison to linear-quadratic-Gaussian(LQG)controller,better control accuracy and lower energy consumption could be realized when using the proposed MPC strategy to simultaneously control temperature and humidity.展开更多
Direct air capture(DAC)is one of the most potential technologies to mitigate CO_(2) emission.Adsorption technol-ogy is recognized as a promising CO_(2) capture method in view of its desirable characteristics including...Direct air capture(DAC)is one of the most potential technologies to mitigate CO_(2) emission.Adsorption technol-ogy is recognized as a promising CO_(2) capture method in view of its desirable characteristics including reusability of adsorbents and low capital investment.To further improve thermal performance,evaporation/condensation heat of vapor compression refrigeration(VCR)cycle in air condition system of buildings is adopted for adsorp-tion/desorption process of DAC.Thermal performance of a 4-step temperature swing adsorption process(TSA)is analyzed at various adsorption/desorption temperatures by using different adsorbents.Analysis on Coefficient of Performance(COP)of VCR cycle is also conducted in search for a balance between adsorbent and refrigerant.Taking both real working capacity and COP into consideration,Mg-MOF-74&R134a is the best choice for more amounts of CO_(2).Real working capacity of Mg-MOF-74 is up to 0.38 mol•kg−1 at 70°C,which is twice as much as that of zeolite 13X.While zeolite 13X&R134a shows the best performance of two cycles in view of exergy efficiency and COP,which could reach 81.9%and 7.21,respectively,at 35°C.These matches will provide some guidelines for the practical application of the combination of DAC with heating,ventilation and air conditioning(HVAC).展开更多
基金supported by the Shanghai Agricultural Science and Technology Program (2022-02-08-00-12-F01176)he National Natural Science Foundation of China (52006135)
文摘Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from the air,lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies.A structured adsorbent is essential for the implementation of gas-solid contactors for cost-and energy-efficient DAC systems.In this study,efficient adsorbent poly(ethyleneimine)(PEI)-functionalized Mg-Al-CO_(3)layered double hydroxide(LDH)-derived mixed metal oxides(MMOs)are three-dimensional(3D)printed into monoliths for the first time with more than 90%adsorbent loadings.The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths.This structure exhibits a 32.7%higher specific surface area and a 46.1%higher pore volume,as compared to the direct printing of the MMO powder into a monolith.After impregnation of PEI,the monolith demonstrates a large adsorption capacity(1.82 mmol/g)and fast kinetics(0.7 mmol/g/h)using a CO_(2)feed gas at 400 ppm at 25℃,one of the highest values among the shaped DAC adsorbents.Smearing of the amino-polymers during the post-printing process affects the diffusion of CO_(2),resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths.The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.
基金supported by the Fundamental Research Funds for the Central Universities (2019JQ03015)the National Natural Science Foundation of China (42075169, U1810209)the Beijing Municipal Education Commission through the Innovative Transdisciplinary Program “Ecological Restoration Engineering”。
文摘Due to the advantages of low energy consumption and high CO_(2) selectivity, the development of solid amine-based materials has been regarded as a hot research topic in the field of DAC for the past decades.The adsorption capacity and stability over multiple cycles have been the top priorities for evaluation of practical application value. Herein, we synthesized a novel DAC material by loading TEPA onto defect-rich Mg_(0.55)Al-O MMOs with enhanced charge transfer effect. The optimal Mg_(0.55)Al-O-TEPA67% demonstrates the highest CO_(2)uptake of(3.0 mmol g^(-1)) and excellent regenerability, maintaining ~90% of the initial adsorption amount after 80 adsorption/desorption cycles. The in situ DRIFTS experiments suggested the formation of bicarbonate species under wet conditions. DFT calculations indicated that the stronger bonding between Mg_(0.55)Al-O support and solid amine was caused by the abundance of oxygen defects on MMOs confirmed by XPS and ESR, which favors the charge transfer between the support and amine,resulting in intense interaction and excellent regenerability. This work for the first time conducted comprehensive and systematic investigation on the stabilization mechanism for MMOs supported solid amine adsorbents with highest uptake and superior cyclic stability in depth, which is different from the most popular SiO_(2)-support, thus providing facile strategy and comprehensive theoretical mechanism support for future research about DAC materials.
基金This work was supported by Russian Science Foundation(19-73-00079).The authors also thank Leonova A.A.for performing N2 adsorption measurements.
文摘Potassium carbonate-based sorbents are prospective materials for direct air capture(DAC).In the present study,we examined and revealed the influence of the temperature swing adsorption(TSA)cycle conditions on the CO_(2) sorption properties of a novel aerogel-based K_(2)CO_(3)/ZrO_(2) sorbent in a DAC process.It was shown that the humidity and temperature drastically affect the sorption dynamic and sorption capacity of the sorbent.When a temperature at the sorption stage was 29℃ and a water vapor pressure P_(H2O) in the feed air was 5.2 mbar(1 bar=105 Pa),the composite material demonstrated a stable CO_(2) sorption capacity of 3.4%(mass).An increase in sorption temperature leads to a continuous decrease in the CO_(2) absorption capacity reaching a value of 0.7%(mass)at T=80℃.The material showed the retention of a stable CO_(2) sorption capacity for many cycles at each temperature in the range.Increasing PH2O in the inlet air from 5.2 to 6.8 mbar leads to instability of CO_(2) sorption capacity which decreases in the course of 3 consecutive TSA cycles from 1.7%to 0.8%(mass)at T=29℃.A further increase in air humidity only facilitates the deterioration of the CO_(2) sorption capacity of the material.A possible explanation for this phenomenon could be the filling of the porous system of the sorbent with solid reaction products and an aqueous solution of potassium salts,which leads to a significant slowdown in the CO_(2) diffusion in the composite sorbent grain.To investigate the regeneration step of the TSA cycle in situ,the macro ATRFTIR(attenuated total reflection Fourier-transform infrared)spectroscopic imaging was applied for the first time.It was shown that the migration of carbonate-containing species over the surface of sorbent occurs during the thermal regeneration stage of the TSA cycle.The movement of the active component in the porous matrix of the sorbent can affect the sorption characteristics of the composite material.The revealed features make it possible to formulate the requirements and limitations that need to be taken into account for the practical implementation of the DAC process using the K_(2)CO_(3)/ZrO_(2) composite sorbent.
文摘A high-level technology is revealed that can effectively convert any distributed system into a globally programmable machine capable of operating without central resources and self-recovering from indiscriminate damages. Integral mission scenarios in Distributed Scenario Language (DSL) can be injected from any point, runtime covering & grasping the whole system or its parts, setting operational infrastructures, and orienting local and global behavior in the way needed. Many operational scenarios can be simultaneously injected into this spatial machine from different points, cooperating or competing over the shared distributed knowledge as overlapping fields of solutions. Distributed DSL interpreter organization and benefits of using this technology for integrated air and missile defense are discussed along with programming examples in this and other fields.
基金supports for the Science and Technology Project of Zhejiang Province(No.LGG21F030009)the Natural Science Foundation of Zhejiang Province(No.LY20F030010)the Key R&D Projects in Zhejiang Province(No.2020C01164)are gratefully acknowledged.
文摘Temperature and humidity are two important factors that influence both indoor thermal comfort and air quality.Through varying compressor and supply fan speeds of a direct expansion(DX)air conditioning(A/C)unit,the air temperature and humidity in the conditioned space can be regulated simultaneously.However,most existing controllers are designed to minimize the tracking errors between the system outputs with their corresponding settings as quickly as possible.The energy consumption,which is directly influenced by the compressor and supply fan speeds,is not considered in the relevant controller formulations,and thus the system may not operate with the highest possible energy efficiency.To effectively control temperature and humidity while minimizing the system energy consumption,a model predictive control(MPC)strategy was developed for a DX A/C system,and the development results are presented in this paper.A physically-based dynamic model for the DX A/C system with both sensible and latent heat transfers being considered was established and validated by experiments.To facilitate the design of MPC,the physical model was further linearized.The MPC scheme was then developed by formulating the objective function which sought to minimize the tracking errors of temperature and moisture content while saving energy consumption.Based on the results of command following and disturbance rejection tests,the proposed MPC scheme was capable of controlling temperature and humidity with adequate control accuracy and sensitivity.In comparison to linear-quadratic-Gaussian(LQG)controller,better control accuracy and lower energy consumption could be realized when using the proposed MPC strategy to simultaneously control temperature and humidity.
基金This research was supported by National Natural Science Foundation of China under contract number(51976178).
文摘Direct air capture(DAC)is one of the most potential technologies to mitigate CO_(2) emission.Adsorption technol-ogy is recognized as a promising CO_(2) capture method in view of its desirable characteristics including reusability of adsorbents and low capital investment.To further improve thermal performance,evaporation/condensation heat of vapor compression refrigeration(VCR)cycle in air condition system of buildings is adopted for adsorp-tion/desorption process of DAC.Thermal performance of a 4-step temperature swing adsorption process(TSA)is analyzed at various adsorption/desorption temperatures by using different adsorbents.Analysis on Coefficient of Performance(COP)of VCR cycle is also conducted in search for a balance between adsorbent and refrigerant.Taking both real working capacity and COP into consideration,Mg-MOF-74&R134a is the best choice for more amounts of CO_(2).Real working capacity of Mg-MOF-74 is up to 0.38 mol•kg−1 at 70°C,which is twice as much as that of zeolite 13X.While zeolite 13X&R134a shows the best performance of two cycles in view of exergy efficiency and COP,which could reach 81.9%and 7.21,respectively,at 35°C.These matches will provide some guidelines for the practical application of the combination of DAC with heating,ventilation and air conditioning(HVAC).