3D printing of poly(ethyleneimine)-functionalized Mg-Al mixed metal oxide monoliths for direct air capture of CO_(2)

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.

CO2 residual concentration of potassium-promoted hydrotalcite for deep CO/CO2 purification in H2-rich gas

Elevated-temperature pressure swing adsorption is a promising technique for producing high purity hydrogen and controlling greenhouse gas emissions. Thermodynamic analysis indicated that the CO in H-rich gas could be controlled to trace levels of below 10 ppm by in situ reduction of the COconcentration to less than 100 ppm via the aforementioned process. The COadsorption capacity of potassiumpromoted hydrotalcite at elevated temperatures under different adsorption（mole fraction, working pressure） and desorption（flow rate, desorption time, steam effects） conditions was systematically investigated using a fixed bed reactor. It was found that the COresidual concentration before the breakthrough of COmainly depended on the total amount of purge gas and the COmole fraction in the inlet syngas.The residual COconcentration and uptake achieved for the inlet gas comprising CO（9.7 mL/min） and He（277.6 mL/min） at a working pressure of 3 MPa after 1 h of Ar purging at 300 mL/min were 12.3 ppm and0.341 mmol/g, respectively. Steam purge could greatly improve the cyclic adsorption working capacity, but had no obvious benefit for the recovery of the residual COconcentration compared to purging with an inert gas. The residual COconcentration obtained with the adsorbent could be reduced to 3.2 ppm after 12 h of temperature swing at 450 °C. A new concept based on an adsorption/desorption process, comprising adsorption, steam rinse, depressurization, steam purge, pressurization, and high-temperature steam purge, was proposed for reducing the steam consumption during CO/COpurification.

Frontier science and challenges on offshore carbon storage

Carbon capture and storage(CCS)technology is an imperative,strategic,and constitutive method to considerably reduce anthropogenic CO_(2)emissions and alleviate climate change issues.The ocean is the largest active carbon bank and an essential energy source on the Earth's surface.Compared to oceanic nature-based carbon dioxide removal(CDR),carbon capture from point sources with ocean storage is more appropriate for solving short-term climate change problems.This review focuses on the recent state-of-the-art developments in offshore carbon storage.It first discusses the current status and development prospects of CCS,associated with the chailenges and uncertainties of oceanic nature-based CDR.The second section outlines the mechanisms,sites,advantages,and ecologic hazards of direct offshore CO_(2)injection.The third section emphasizes the mechanisms,schemes,influencing factors,and recovery efficiency of ocean-based CO-CH_(4)replacement and CO_(2)-enhanced oil recovery are reviewed.In addition,this review discusses the economic aspects of offshore CCS and the preponderance of offshore CCs hubs.Finally,the upsides,limitations,and prospects for further investigation of offshore CO_(2)storage are presented.

Additives enhancing supported amines performance in CO_(2)capture fromair

The utilization of supported amines as adsorbents in direct air capture(DAC)has been demonstrated to be a promising strategy for the reduction of CO_(2)emissions.To improve the performance of amine-based adsorbents,the incorporation of additives has been widely adopted.In the present study,we conduct a comprehensive comparison of seven additives on tetraethylenepentamine-impregnated mesoporous silica as a representative amine-based adsorbent.The results indicate thatminor molecularweight additiveswith hydroxyl groups show improved adsorption-desorption performance and increase oxidative stability.A proposed mechanism for these improvements is the combined physical and chemical promotion effects of hydroxyl groups.Through a comprehensive review of existing literature,it is found that the effects of additives on amine-based adsorbents are dependent on factors,such as additive type,pristine adsorbent properties,incorporation method,and testing conditions.Based on these findings,it is recommended that future DAC systems prioritize the use of hydroxyl-containing additives,whereas higher CO_(2)concentration and temperature capture may benefit from the incorporation of additives without hydroxyl groups.These conclusions are expected to contribute to the design of efficient adsorbents for CO_(2)capture.

吸附法碳捕集技术的规模化应用和挑战

实现2030年碳达峰和2060年碳中和是能源领域的当前决策和长远愿景,为此必须更加紧密结合全球能源发展趋势及国家能源策略,在碳捕集与封存领域投入研发力量.近几十年来,吸附法作为一种极具应用潜力的碳捕集技术得到了快速发展.例如,对高性能吸附剂的开发进行了大量探索;适用于碳捕集的吸附循环过程得到了显著的发展;先进的吸附剂结构和装置不断被提出;将吸附过程与其他分离和/或反应过程进行耦合的复合吸附技术得到了广泛关注;吸附法碳捕集技术的应用领域也得到了拓展.为此,本文介绍了各种吸附法碳捕集循环过程,归纳总结了目前超出实验室级别装置(技术成熟度TRL5~7)的技术特点、分离性能、运行能耗和成本,应用场合包括了燃烧后碳捕集、燃烧前碳捕集和直接空气碳捕集.对吸附法碳捕集技术作了评述,指出了其在未来发展中面临的机遇和挑战.