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[Display omitted] • Comparisons of NO x adsorption and desorption among series of zeolites are conducted. • Effects of zeolite structures, cations, SiO 2 /Al 2 O 3 ratios on NO x sorption are shown. • H-typed 10-membered-ring straight-channel zeolite is selected as preferred sorbent. • Importance of kinetics of NO oxidation-NO 2 physisorption process is revealed. • Accessibility of Brønsted acid sites that drives NO-NO 2 catalytic cycle is discussed. Adsorption is a promising technology for deep purification of nitrogen oxides (NO x) from flue gases and simultaneously recycling NO 2 as an economically valuable chemical. Zeolite as a robust NO x adsorbent provides the key step for success in practical applications, of which the screening remains challenging regarding the NO-NO 2 oxidation and adsorption combined process. In this work, experimental evaluations on practical NO x sorption performances on series of zeolites were conducted. Effects of the zeolite typological structure, compensating cation, and SiO 2 /Al 2 O 3 ratio on deep purification efficacy, water resistance, and regenerability at varying humidity were obtained, revealing the importance of kinetics of the NO oxidation and NO 2 physisorption consecutive process. The H-typed 10-membered-ring straight-channel zeolites (MFI and FER) were demonstrated to be the preferred NO x adsorbents qualified for industrial needs, as compared to other caged-channel, hybrid-channel, larger-sized straight-channel, or Na-typed counterparts. Deeper insights into the key role of Brønsted acid sites (BAS) in driving the NO-NO 2 catalytic cycle and promoting the adsorption competitiveness of NO x over water vapor were revealed based on in-situ diffuse reflectance Fourier transform infrared spectroscopy characterizations. The MFI zeolite with improved performance at the low-silica version could benefit from the efficient utilization of BAS within the highly accessible medium-sized straight channel, while the FAU zeolite (representative caged-channel zeolite) requiring appropriate SiO 2 /Al 2 O 3 ratio for optimal BAS utilization may suffer from the limited site accessibility. The findings clarify the relationships between NO x oxidative adsorption performances and zeolite properties, which provides a fundamental perspective and scientific screening strategy for NO x adsorbents. [ABSTRACT FROM AUTHOR]

Adsorption is a promising technology for simultaneously capturing nitrogen oxides (NO x) from flue gases and recycling NO 2 as a profitable chemical, for which a robust and efficient adsorbent provides the key step for success in practical applications. This work reports the enhancement of NO x adsorption performances with less cost of desorption energy on Cu-ZSM-5 zeolites prepared by a facile and rapid (690 s) modification method, the incipient-wetness impregnation coupled with microwave drying (IM). In comparisons to H-ZSM-5, Na-ZSM-5 and conventionally liquid-phase ion-exchanged counterparts under sub-1000 ppm NO x feed concentrations and room temperature, the IM sample renders a record NO x adsorption capacity (q t,NOx) of 0.878 mmol/g from dry gas stream on zeolites, and an applicable q t,NOx of 0.1 mmol/g from wet gas stream with a proper copper loading (2.1 wt%). The temperature programmed desorption of NO x on the optimal IM sample saturated with NO x from wet gas stream exhibit primary peak temperature lower than reported Cu-ZSM-5 and significant NO 2 proportion (72.6 %) in desorbed NO x. Deeper insights into advantageous NO x oxidative adsorption over the properly-loaded Cu-ZSM-5 in terms of diverse adsorbate states and competitiveness towards H 2 O were gained, showing IM method a promising sorbent improvement strategy for practical use. [Display omitted] • Cu-ZSM-5 is prepared by incipient-wetness impregnation coupled with microwave drying. • A record NO x adsorption capacity at sub-1000 ppm dry gas feed on zeolites is obtained. • Applicable NO x adsorption capacity at wet feed is gained on properly-loaded Cu-ZSM-5. • Lower NO x desorption temperature and higher NO 2 proportion in desorbed gas are shown. • Advantageous NO x oxidative adsorption competing with H 2 O on Cu-ZSM-5 is revealed. [ABSTRACT FROM AUTHOR]

Adsorption is a promising technology for capturing nitrogen oxides (NO x) from humid flue gases, for which as the preferred NO x adsorbent, zeolite with an appropriate silica to alumina (Si/Al) ratio provides the key step for success in practical applications. In this work, the effects of Si/Al ratio, temperature, relative humidity (RH), and feed gas (NO x -H 2 O(g)–CO 2 –O 2 -N 2) compositions on NO x sorption behavior on HZSM-5 zeolites were systematically investigated, based on a series of characterizations, fixed-bed adsorption and temperature programmed desorption (TPD) tests. The low-silica HZSM-5(25) showed the best performance (326.6 μmol/g and 39.2 μmol/g at dry and 90%RH) as compared to others with higher Si/Al ratios at each RH, in which the roll-up effect was positively correlated with the Si/Al ratios and humidity. O 2 enhanced NO x adsorption and reached an optimal adsorption capacity at the concentration of 14%, while CO 2 had little effect on NO x adsorption. The decrease in temperature increased NO x adsorption capacity on HZSM-5(25), benefitting from NO 2 physisorption as well as satisfactory NO oxidation within the active adsorbent structure. The facile thermal desorption of NO x and significant NO–NO 2 conversion on HZSM-5(25) was exhibited by bimodal TPD peaks at 343–353K and 533–543K respective for NO and NO 2 , in contrast to those on Silicalite-1. A potential "water-resistant" strategy via the enhancement of NO x adsorption competitiveness was revealed, providing a theoretical guideline for NO x adsorbent screening in industrial applications. [Display omitted] • Influential rules of multiple factors on NO x adsorption are systematically explored. • Low-silica HZSM-5 shows the best NO x adsorption performance at each condition. • Contributions of NO oxidation and NO 2 physisorption at varying temperatures are shown. • Greater regenerability of NO x from NO x -H 2 O(g)–CO 2 –O 2 -N 2 feed on HZSM-5 is demonstrated. • A "water-resistant" strategy for enhancing NO x adsorption competitiveness is proposed. [ABSTRACT FROM AUTHOR]

[Display omitted] • Distillation separation process is proposed to recover NO 2 and SO 2 from flue gases. • The feasibility of NO 2 /SO 2 distillation separation is theoretically verified. • A distillation process with advantageous dual-column liquid-phase feeding is designed. • Process optimization based on robust sensitivity analysis are demonstrated. • Significant economic benefits from the recovered NO 2 and SO 2 products are estimated. High-purity NO 2 and SO 2 have significant economic values and are widely used in many fields. The large amounts of NO 2 and SO 2 in industrial flue gases are worthy of recovery for environmental protection and economic benefits. In this work, a dual-column distillation separation process was proposed to further separate and upgrade NO 2 and SO 2 following a flue gas adsorption capture process. The feasibility of distillation separation of NO 2 /SO 2 from the desorbed gas, and the advantage of liquid-phase feeding way over gas-phase counterpart in terms of lower energy consumption (1286.39 kW) were demonstrated. Key process parameters such as the number of total stages, the feed stage number, the mole flow rate at bottom of column, the reflux ratio and operating pressure for the two columns (15, 6, 16.66 kmol/h, 0.16, 4 bar; 21, 10, 4.43 kmol/h, 0.50, 1 bar) were determined. Heat and mass transfers along the column height as well as the process robustness against feed composition fluctuation indicate its applicability for practical operation and adaptation to industrial needs. An economic analysis shows a significant annual revenue of 14,333.52 thousand USD based on high-purity (>99.5%) SO 2 and NO 2 products recovered from a typical scale (~1000,000 m3/h) of iron-ore sintering flue gas, not only offsetting the total operating cost of the entire adsorption capture-distillation recovery process but also generating net profit. [ABSTRACT FROM AUTHOR]

Conventional flue gas nitrogen oxides (NO x) abatement technologies commonly convert NO x into harmless compounds, while less effort has been made to recycle NO 2 as a profitable chemical in many industries. Towards this end, adsorption is a promising technology for which an advanced technique for NO 2 desorption and efficient sorbent regeneration provides the key step for success in practical applications. This work reports a novel cyclic adsorption process for NO x removal with recycling of NO 2 from iron-ore sintering flue gas of a steel plant. This process using self-prepared and validated pelletized Na-ZSM-5 zeolites as low-cost sorbents involves NO x catalytic adsorption and reversible desorption using multiple hot gas circulations (GC) within the enclosed fixed bed followed by scavenging and purge at mild conditions. In comparison to conventional cyclic processes, greater amount of recyclable NO 2 was obtained, rendering the NO x recovery of >92% and the mean NO 2 concentration of >2% significantly enriched from original 20 ppm in feed gas. A robust adsorption-desorption performance with appreciable NO x working capacity was achieved for up to 16 cycles. The key role of the segmentation of GC in boosting NO x regenerability was addressed, providing an economical three-tower strategy for continuous NO 2 production for practical use. ga1 • NO x removal and with recycling of NO 2 from flue gas was studied through field tests. • Comparisons among different adsorption cycles in NO x removal and recycling were made. • A novel technique for efficient NO 2 desorption and sorbent regeneration was proposed. • NO x recovery of 92% and recyclable desorbed NO 2 concentration of >2% were obtained. • Robust cyclic performance with NO x working capacity of >0.1 mmol/g was demonstrated. [ABSTRACT FROM AUTHOR]