Low-energy-consumption temperature swing system for CO_(2) capture by combining passive radiative cooling and solar heating

Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative cooling.For desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for heating.The heating and cooling processes are completely driven by solar energy.Adsorption tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ones.Furthermore,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple cycles.The present work may inspire the development of new temperature swing procedures with little energy consumption.

Highly efficient CO_(2) capture using 2-methylimidazole aqueous solution on laboratory and pilot-scale

To date,the primary industrial carbon capture approach is still absorption using aqueous solutions of alkanolamines.Here,to pursue a substitute for the amine-based approach to improve the CO_(2) capture efficiency and decrease the energy cost further,we report a new carbon capture approach using a 2-methylimidazole(mIm)aqueous solution.The properties and sorption behaviors of this approach have been experimentally investigated.The results show that the mIm solution has higher CO_(2) absorption capacity under relatively higher equilibrium pressure(>130 kPa)and lower desorption heat than the methyldiethanolamine solution.91.6%sorption capacity of mIm solution can be recovered at 353.15 K and 80 kPa.The selectivity for CO_(2)/N_(2) and CO_(2)/CH_(4) can reach an exceptional 7609 and 4324,respectively.Furthermore,the pilot-scale tests were also performed,and the results demonstrate that more than 98%of CO_(2) in the feed gas could be removed and cyclic absorption capacity can reach 1 mol·L^(-1).This work indicates that mIm is an excellent alternative to alkanolamines for carbon capture in the industry.

Recent advances in intermediate-temperature CO_(2) capture: Materials,technologies and applications

Carbon capture,utilization and storage(CCUS) is widely recognized as a vital strategy for mitigating the impact of human induced climate change.Among various CO_(2) adsorbents,intermediate-temperature solid adsorbents have garnered significant attention due to their potential applications in hydrogen utilization,specifically in the water gas shift,steam reforming and gasification processes.These processes are crucial for achieving carbon neutrality.While laboratory-level studies have showcased the high adsorption capacity of these materials via various synthesis and modification methods,their practical application in complex industrial environments remains challenging,impeding the commercialization process.This review aims to critically summarize the recent research progress made in intermediatetemperature(200-400℃) solid CO_(2) adsorbents,particularly focusing on indicators such as cyclability,gas selectivity,and formability,which play vital roles in industrial application scenarios.Additionally,we provide an overview of laboratory-level advanced technologies specifically tailored for industrial applications.Furthermore,we highlight several industrial-ready advanced technologies that can pave the way for overcoming the challenges associated with large-scale implementation.The insights provided by this review aim to assist researchers in identifying the most relevant research directions for industrial applications.By promoting advances in the application of solid adsorbents,we strive to facilitate the ultimate goal of achieving carbon neutrality.

The Capture and Catalytic Conversion of CO_(2) by Dendritic Mesoporous Silica-Based Nanoparticles

Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar guest species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.

CO_(2)capture costs of chemical looping combustion of biomass:A comparison of natural and synthetic oxygen carrier

Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.

An integrated technology for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment

In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-gravity factor,gas/liquid ratio,and initial BaCl2concentration on the absorption rate and amount of CO_(2)and the preparation of BaCO_(3)are investigated.The results reveal that the absorption rate and amount of CO_(2)follow the order of ethyl alkanolamine(MEA)>diethanol amine(DEA)>N-methyldiethanolamine(MDEA),and thus MEA is the most effective absorbent for CO_(2)absorption.The absorption rate and amount of CO_(2)under high gravity are higher than that under normal gravity.Notably,the absorption rate at 75 min under high gravity is approximately 2 times that under normal gravity.This is because the centrifugal force resulting from the high-speed rotation of the packing can greatly increase gas-liquid mass transfer and micromixing.The particle size of BaCO_(3)prepared in the rotating packed bed is in the range of 57.2—89 nm,which is much smaller than that prepared in the bubbling reactor(>100.3 nm),and it also has higher purity(99.6%)and larger specific surface area(14.119 m^(2)·g^(-1)).It is concluded that the high-gravity technology has the potential to increase the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3).This study provides new insights into carbon emissions reduction and carbon utilization.

Hollow tubes constructed by carbon nanotubes self-assembly for CO_(2) capture

Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.

Scalable Jet-Based Fabrication of PEI-Hydrogel Particles for CO_(2)Capture

The capture,regeneration,and conversion of CO_(2)from ambient air and flue gas streams are critical aspects of mitigating global warming.Solid sorbents for CO_(2)absorption are very promising as they have high mass transfer areas without energy input and reduce emissions and minimize corrosion as compared to liquid sorbents.However,precisely tunable solid CO_(2)sorbents are difficult to produce.Here,we demonstrate the high-throughput production of hydrogel-based CO_(2)-absorbing particles via liquid jetting.By wrapping a liquid jet consisting of an aqueous solution of cross-linkable branched polyethylenimine(PEI)with a layer of suspension containing hydrophobic silica nanoparticles,monodisperse droplets with a silica nanoparticle coating layer was formed in the air.A stable Pickering emulsion containing PEI droplets was obtained after these ejected droplets were collected in a heated oil bath.The droplets turn into mm-sized particles after thermal curing in the bath.The diameter,PEI content,and silica content of the particles were systematically varied,and their CO_(2)absorption was measured as a function of time.Steam regeneration of the particles enabled cyclic testing,revealing a CO_(2)absorption capacity of 6.5±0.5 mol kg^(−1)solid PEI in pure CO_(2)environments and 0.7±0.3 mol kg^(−1)solid PEI for direct air capture.Several thousands of particles were produced per second at a rate of around 0.5 kg per hour,with a single nozzle.This process can be further scaled by parallelization.The complete toolbox for the design,fabrication,testing,and regeneration of functional hydrogel particles provides a powerful route toward novel solid sorbents for regenerative CO_(2)capture.

Regulation of interlayer channels of graphene oxide nanosheets in ultra-thin Pebax mixed-matrix membranes for CO_(2) capture

For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(MMMs)incorporated by graphene oxide(GO),in which the interlayer channels were regulated to optimize the CO_(2)/N_(2) separation performance.Various membrane preparation conditions were systematically investigated on the influence of the membrane structure and separation performance,including the lateral size of GO nanosheets,GO loading,thermal reduction temperature,and time.The results demonstrated that the precisely regulated interlayer channel of GO nanosheets can rapidly provide CO_(2)-selective transport channels due to the synergetic effects of size sieving and preferential adsorption.The GO/Pebax ultra-thin MMMs exhibited CO_(2)/N_(2) selectivity of 72 and CO_(2) permeance of 400 GPU(1 GPU=106 cm^(3)(STP)·cm^(2)·s^(-1)·cmHg^(-1)),providing a promising candidate for CO_(2) capture.

Assessing the Viability of Gandhar Field in India’s Cambay Basin for CO_(2) Storage

Our research is centered on the Gandhar oil field, which was discovered in 1983, where daily oil production has declined significantly over the years. The primary objective was to evaluate the feasibility of carbon dioxide(CO_(2)) storage through its injection into the siliciclastic reservoirs of Ankleshwar Formation. We aimed to obtain high-resolution acoustic impedance data to estimate porosity employing model-based poststack seismic inversion. We conducted an analysis of the density and effective porosity in the target zone through geostatistical techniques and probabilistic neural networks. Simultaneously, the work also involved geomechanical analysis through the computation of pore pressure and fracture gradient using well-log data, geological information, and drilling events in the Gandhar field. Our investigation unveiled spatial variations in effective porosity within the Hazad Member of the Ankleshwar Formation, with an effective porosity exceeding 25% observed in several areas, which indicates the presence of well-connected pore spaces conducive to efficient CO_(2) migration. Geomechanical analysis showed that the vertical stress(Sv) ranged from 55 MPa to 57 MPa in Telwa and from 63.7 MPa to 67.7 MPa in Hazad Member. The pore pressure profile displayed variations along the stratigraphic sequence, with the shale zone, particularly in the Kanwa Formation, attaining the maximum pressure gradient(approximately 36 MPa). However, consistently low pore pressure values(30-34 MPa) considerably below the fracture gradient curves were observed in Hazad Member due to depletion. The results from our analysis provide valuable insights into shaping future field development strategies and exploration of the feasibility of CO_(2) sequestration in Gandhar Field.

A review of interaction mechanisms and microscopic simulation methods for CO_(2)-water-rock system

This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscopic simulations of CO_(2)-water-rock system.The work points out the key issues in current research and provides suggestions for future research.After injection of CO_(2) into underground reservoirs,not only conventional pressure-driven flow and mass transfer processes occur,but also special physicochemical phenomena like dissolution,precipitation,and precipitate migration.The coupling of these processes causes complex changes in permeability and porosity parameters of the porous media.Pore-scale microscopic flow simulations can provide detailed information within the three-dimensional pore and throat space and explicitly observe changes in the fluid-solid interfaces of porous media during reactions.At present,the research has limitations in the decoupling of complex mechanisms,characterization of differential multi-mineral reactions,precipitation generation mechanisms and characterization(crystal nucleation and mineral detachment),simulation methods for precipitation-fluid interaction,and coupling mechanisms of multiple physicochemical processes.In future studies,it is essential to innovate experimental methods to decouple“dissolution-precipitation-precipitate migration”processes,improve the accuracy of experimental testing of minerals geochemical reaction-related parameters,build reliable characterization of various precipitation types,establish precipitation-fluid interaction simulation methods,coordinate the boundary conditions of different physicochemical processes,and,finally,achieve coupled flow simulation of“dissolution-precipitation-precipitate migration”within CO_(2)-water-rock systems.

Integrated vacuum pressure swing adsorption and Rectisol process for CO_(2) capture from underground coal gasification syngas

An integrated vacuum pressure swing adsorption(VPSA) and Rectisol process is proposed for CO_(2) capture from underground coal gasification(UCG) syngas. A ten-bed VPSA process with silica gel adsorbent is firstly designed to pre-separate and capture 74.57% CO_(2) with a CO_(2) purity of 98.35% from UCG syngas(CH_(4)/CO/CO_(2)/H_(2)/N_(2)= 30.77%/6.15%/44.10%/18.46%/0.52%, mole fraction, from Shaar Lake Mine Field,Xinjiang Province, China) with a feed pressure of 3.5 MPa. Subsequently, the Rectisol process is constructed to furtherly remove and capture the residual CO_(2)remained in light product gas from the VPSA process using cryogenic methanol(233.15 K, 100%(mass)) as absorbent. A final purified gas with CO_(2) concentration lower than 3% and a regenerated CO_(2) product with CO_(2) purity higher than 95% were achieved by using the Rectisol process. Comparisons indicate that the energy consumption is deceased from 2.143 MJ·kg^(-1) of the single Rectisol process to 1.008 MJ·kg^(-1) of the integrated VPSA & Rectisol process, which demonstrated that the deployed VPSA was an energy conservation process for CO_(2) capture from UCG syngas. Additionally, the high-value gas(e.g., CH_(4)) loss can be decreased and the effects of key operating parameters on the process performances were detailed.

Dynamic Modeling and Sensitivity Analysis for an MEA-Based CO_(2) Capture Absorber

The absorber is the key unit in the post-combustion monoethanolamine(MEA)-based carbon dioxide(CO_(2))capture process.A rate-based dynamic model for the absorber is developed and validated using steady-state experimental data reported in open literature.Sensitivity analysis is performed with respect to important model parameters associated with the reaction,mass transport and phy-sical property relationships.Then,a singular value decomposition(SVD)-based subspace parameter estimation method is proposed to improve the model accu-racy.Finally,dynamic simulations are carried out to investigate the effects of the feed rate of lean MEA solution and the flue inlet conditions.Simulation results indicate that the established dynamic model can reasonably reflect the physical behavior of the absorber.Some new insights are gained from the simulation results.

海洋CO_(2)地质封存研究进展与发展趋势

CO_(2)捕集、利用和封存是中国实现“双碳”目标的核心技术,也是全球研究的热点。CO_(2)地质封存是其中的关键环节,特别是海洋CO_(2)地质封存是今后的重点发展方向。以国内外海洋CO_(2)地质封存的发展历程为基础,结合典型CO_(2)海洋封存示范项目案例,系统梳理了国内外海洋CO_(2)地质封存理论研究进展,分析了CO_(2)在井筒流动、相变与传热、CO_(2)流体运移与储层物性参数展布规律、海洋地质封存机制及封存潜力、地质封存盖层完整性及安全性评估等方面的研究现状。认识到中国目前对海底地质结构中CO_(2)注入过程的多相态转化、溶解、捕获传质特征及动力学特性认识尚浅,对海洋封存机制及不同封存机制之间的相互作用机理尚不明确,未来应开展海洋CO_(2)动态地质封存空间重构机制研究,解决地质封存相态转化及流体动态迁移机理等关键科学问题,揭示海洋CO_(2)地质封存机制的相互作用机理,形成适用于中国海洋地质封存CO_(2)高效注入和增效封存方法。

工业固废CO_(2)矿化协同减污降碳关键技术进展

针对工业过程CO_(2)和固废排放的问题,减污降碳刻不容缓。CO_(2)矿化技术在封存CO_(2)的同时固废得到资源化利用,受到广泛关注。论述了不同工业固废作为CO_(2)矿化原料的利用情况,对比分析了不同矿化工艺优缺点及CO_(2)矿化机理,总结了不同CO_(2)矿化工艺研究现状和工业化应用情况。研究发现,目前针对固废CO_(2)矿化缺乏机制性解释,无法有效控制金属离子的浸取过程和矿化过程中气液固传质的效率,同时矿化形成的碳酸盐产品存在粒径大、易团聚、功能单一等问题。未来需进一步研究浸渍过程中表面溶剂扩散等控制浸取速率和程度的机制;深入研究碳酸盐成核结晶动力学机制及碳酸盐晶体形貌、粒度调控方法;构建煤基固废浸取、矿化溶质气-液-固传输模型,进行工艺参数优化和过程强化并确定放大规律;进一步加强CO_(2)矿化利用技术全生命周期和经济评价;最后,需加大CO_(2)矿化利用技术的中试、示范技术集成和成套工艺建设,为规模化减污降碳技术的工业化发展奠定技术支撑。

失活石灰石自活化增强循环捕集CO_(2)特性

钙循环工艺是一种低成本高效率捕集CO_(2)技术,运行过程需不断补充新鲜吸收剂并排出失活吸收剂,实现失活钙基吸收剂原位资源化利用具有重要意义。为研究颗粒状石灰石失活后自活化特性,运用双固定床反应器制备了失活石灰石,分析了自活化后石灰石碳酸化转化率随循环次数的变化规律,采用XRD、SEM、N_(2)吸附等分析测试手段探究了自活化提高失活石灰石循环捕集CO_(2)性能机理。结果表明,失活石灰石置于环境中可吸收空气中水分生成Ca(OH)_(2),吸水率φ达100%后,继续吸水生成氢氧化钙水合物,极限吸水率为130%。不同程度自活化后的石灰石循环捕集CO_(2)性能均有不同程度提高,随吸水率变化呈线性升高趋势。与分析纯CaCO3相比,失活石灰石对吸水率变化更敏感,随吸水率升高其循环捕集CO_(2)性能提高更快。吸水率为130%时,自活化后石灰石循环捕集CO_(2)性能甚至优于新鲜石灰石。微观结构分析结果显示:新鲜石灰石因高温烧结而失活过程中,CaO晶粒尺寸由41.9 nm长大至72.2 nm,孔隙结构发生坍塌阻塞,比孔容和比表面积显著降低。经过自活化,煅烧后的石灰石中CaO晶粒尺寸降低,原本密实的表面重新生成孔隙结构;吸水率为130%时,晶粒尺寸降至35.1 nm,比孔容和比表面积分别恢复至新鲜石灰石的70.5%和107.6%,特别是10~100 nm孔隙得以再生,因此失活石灰石循环捕集CO_(2)性能恢复。虽然自活化过程会加剧失活石灰石颗粒磨损速率,但吸水率100%的自活化石灰石磨损导致直径每小时减小量仅为颗粒直径的0.55%。综上所述,自活化后的失活石灰石完全可替代新鲜石灰石,作为补充钙基吸收剂用于钙循环捕集CO_(2)。

石灰回转窑真实烟气条件下有机胺法CO_(2)捕集试验

为推动有机胺法CO_(2)捕集工艺在钢铁行业的应用,在石灰石回转窑炉真实烟气条件下开展了有机胺法CO_(2)捕集侧线试验,考察了有机胺溶液质量分数、烟气流量、溶液喷淋量、吸收温度、油浴温度和再生压力等关键参数对捕集系统CO_(2)捕集性能的影响。结果表明,在最优试验条件(有机胺溶液质量分数为25.0%、烟气流量为20m^(3)/h、溶液喷淋量为70L/h、吸收温度为30℃、油浴温度为115℃以及再生压力为10kPa)下,捕集系统CO_(2)捕集率和解吸酸气量分别为94%和1.22m^(3)/h。在最优试验条件下进行的480h连续试验结果显示,捕集系统CO_(2)捕集率平均值为94%,解吸酸气量平均值为1.22m^(3)/h,CO_(2)捕集系统表现出良好的稳定性,证明有机胺法应用于石灰回转窑烟气CO_(2)捕集技术可行。

CO_(2)捕捉技术在船舶减碳中的应用分析及展望

船舶碳捕集技术成为当前减少船舶碳排放的重要解决方案之一。针对短期内减少船舶尾气CO_(2)排放的问题,本文系统梳理了CO_(2)捕捉技术及其在船岸的应用和发展;通过对比分析法得出不同方式的CO_(2)捕捉技术的成熟度及优缺点,并在此基础上深入分析了目前CO_(2)捕捉技术在船舶应用中存在的捕捉效率不高、运行成本较高、政策标准不完善等方面的问题;提出了未来船舶尾气碳捕捉技术发展方向及建议,为商船碳捕集技术的更深入研究和推广应用提供更多思路和参考依据。

具有自萃取功能的相变CO_(2)吸收剂体系开发

二氧化碳(CO_(2))捕集工程应用的吸收剂存在再生能耗高、传质速率低、运行损耗大等问题,严重制约了CO_(2)捕集技术的大规模推广应用。为解决这些问题,该文开发适用于低分压CO_(2)捕集的相变吸收剂。该相变吸收体系以亲水性胺N-氨乙基哌嗪(N-aminoethyl piperazine,AEP)为主吸收体系,添加亲脂性分相剂二正丁胺(Di-n-butylamine,DPA)和活化剂(activator,ACT)。通过核磁共振波谱(nuclear magnetic resonance,NMR)和捕集CO_(2)连续测试实验研究该相变吸收剂的性能。实验结果表明,吸收负载达1.082 mol CO_(2)/mol溶液,再生温度降至98.5℃,具有优异的吸收性能和解吸性能。NMR分析表明,反应产物具有氨基甲酸盐分子结构,捕集CO_(2)连续测试实验研究与同浓度3 mol/L一乙醇胺(Monoethanolamine,MEA)溶液进行对比分析可知,相同再生能耗下,单位体积同浓度相变体系相比MEA吸收容量提高33%以上;相同再生能耗下相变体系的再生率比MEA提高15%,相同再生率下相变体系的再生能耗比MEA降低31%以上。结果表明,该相变吸收剂对于低分压CO_(2)捕集具有良好的应用前景。

烟道气CO_(2)捕集用醇胺溶液降解研究进展

目前在多种CO_(2)吸收捕集技术中,醇胺法是吸收量最大、经济效益最好和研究最广泛的方法。然而,醇胺法中使用的醇胺溶液吸收剂面临的降解问题是该方法的主要缺陷。针对醇胺溶液吸收剂的降解问题,首先综述了热降解和氧化降解的产物、机理和控制研究进展,然后综述了金属离子催化降解的降解机理、规律和控制研究进展,最后对醇胺溶液吸收剂的降解问题进行了总结,并对未来的抗降解研究方向进行了展望。