邱宇烜,李平,邵历强,苗垚

• 1:华东理工大学化工学院化学工程联合国家重点实验室

摘要(Abstract)：

针对吸附法捕集烟道气CO_2成本和能耗较高问题，研究采用六水氯化镁和碳酸氢钠通过沉淀法制备碱式碳酸镁并煅烧制得氧化镁粉体，再通过硝酸钠和碳酸钠浸渍改性并成型为(Na NO_3)_(0.1)-Mg O和(Na NO_3)_(0.1)(Na_2CO_3)_(0.05)-Mg O颗粒状吸附剂。采用X射线衍射等表征手段对两种吸附剂颗粒微观结构进行分析，并结合热重实验评估了CO_2吸附/解吸动力学和循环稳定性。进行了硝酸钠/碳酸钠改性氧化镁吸附剂颗粒填充床低浓度CO_2气体的吸附解吸实验研究，分析了氧化镁表面负载的硝酸盐和碳酸盐对低浓度CO_2条件下捕集的强化作用。结果表明，在300℃左右，硝酸钠能够在氧化镁表面形成熔盐层，显著强化了CO_2吸附性能；硝酸钠熔盐层内存在CO_2扩散阻力，需要一定的CO_2分压作为通过熔盐层所需的传质推动力，进而降低了低浓度CO_2吸附量；碳酸钠的添加可降低CO_2通过熔盐层所需的传质推动力，提高低浓度CO_2吸附量。

关键词(KeyWords)： CO_2吸附;氧化镁吸附剂;固定床;CO_2捕集;熔盐改性氧化镁吸附剂

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金(21978090,22178115)

作者(Author): 邱宇烜,李平,邵历强,苗垚

参考文献(References)：

• [1] FERNáNDEZ J R, GARCIA S, SANZ-PéREZ E S. CO2 capture and utilization editorial[J]. Industrial&Engineering Chemistry Research, 2020, 59(15):6767-6772.
• [2] NOCITO F, DIBENEDETTO A. Atmospheric CO2 mitigation technologies:Carbon capture utilization and storage[J]. Current Opinion in Green and Sustainable Chemistry, 2020, 21:34-43.
• [3] WANG Q, LUO J Z, ZHONG Z Y, et al. CO2 capture by solid adsorbents and their applications:Current status and new trends[J].Energy Environ, 2011, 4(1):42-55.
• [4] PARDAKHTI M, JAFARI T, TOBIN Z, et al. Trends in solid adsorbent materials development for CO2 capture[J]. ACS Applied Materials&Interfaces, 2019, 11(38):34533-34559.
• [5]柳春杰,吴素芳. CaCO3改性对提高MgO基CO2吸附剂循环稳定性的影响[J].高校化学工程学报, 2020, 34(3):742-748.LIU C J, WU S F. Effect of CaCO3 modification on improving cycle stability of MgO-based CO2 adsorbents[J]. Journal of Chemical Engineering of Chinese Universities, 2020, 34(3):742-748.
• [6]元慧力,钟雯诗,郑淑娟,等.柔性碳纤维基吸附剂的制备及CO2吸附性能[J].高校化学工程学报, 2023, 37(1):61-67.YUAN H L, ZHONG W S, ZHENG S J, et al. Preparation of flexible carbon fiber based sorbents and their CO2 capture performance[J]. Journal of Chemical Engineering of Chinese Universities, 2023, 37(1):61-67.
• [7] QIAO Y Q, WANG J Y, ZHANG Y, et al. Alkali nitrates molten salt modified commercial MgO for intermediate-temperature CO2capture:Optimization of the Li/Na/K ratio[J]. Industrial&Engineering Chemistry Research, 2017, 56(6):1509-1517.
• [8] VU A T, HO K, JIN S, et al. Double sodium salt-promoted mesoporous MgO sorbent with high CO2 sorption capacity at intermediate temperatures under dry and wet conditions[J]. Chemical Engineering Journal, 2016, 291:161-173.
• [9] XIAO G K, SINGH R, CHAFFEE A, et al. Advanced adsorbents based on MgO and K2CO3 for capture of CO2 at elevated temperatures[J]. International Journal of Greenhouse Gas Control, 2011, 5(4):634-639.
• [10] DAL POZZO A, ARMUTLULU A, REKHTINA M, et al. CO2 uptake and cyclic stability of MgO-based CO2 sorbents promoted with alkali metal nitrates and their eutectic mixtures[J]. ACS Applied Energy Materials, 2019, 2(2):1295-1307.
• [11] HARADA T, SIMEON F, HAMAD E Z, et al. Alkali metal nitrate-promoted high-capacity MgO adsorbents for regenerable CO2capture at moderate temperatures[J]. Chemistry of Materials, 2015, 27(6):1943-1949.
• [12] WANG K, ZHAO Y W, CLOUGH P T, et al. Structural and kinetic analysis of CO2 sorption on NaNO2-promoted MgO at moderate temperatures[J]. Chemical Engineering Journal, 2019, 372:886-895.
• [13] PANG H, SUN A W, XU H R, et al. Regenerable MgO-based sorbents for CO2 capture at elevated temperature and pressure:Experimental and DFT study[J]. Chemical Engineering Journal, 2021, 425:130675.
• [14] WANG L, ZHOU Z M, HU Y W, et al. Nanosheet MgO-based CO2 sorbent promoted by mixed-alkali-metal nitrate and carbonate:Performance and mechanism[J]. Industrial&Engineering Chemistry Research, 2017, 56(20):5802-5812.
• [15] LEE C H, MUN S, LEE K B. Characteristics of Na–Mg double salt for high-temperature CO2 sorption[J]. Chemical Engineering Journal, 2014, 258:367-373.
• [16] VU A T, PARK Y, JEON P R, et al. Mesoporous MgO sorbent promoted with KNO3 for CO2 capture at intermediate temperatures[J].Chemical Engineering Journal, 2014, 258:254-264.
• [17] GAO W L, ZHOU T T, GAO Y S, et al. Study on MNO3/NO2(M=Li, Na, and K)/MgO composites for intermediate-temperature CO2capture[J]. Energy&Fuels, 2019, 33(3):1704-1712.
• [18] PAPALAS T, ANTZARAS A N, LEMONIDOU A A. Magnesite-derived MgO promoted with molten salts and limestone as highly-efficient CO2 sorbent[J]. Journal of CO2 Utilization, 2021, 53:101725.
• [19] GONG F C, HUANG Z, WEI X L, et al. MgO promoted by Fe2O3 and nitrate molten salt for fast and enhanced CO2 capture:Experimental and DFT investigation[J]. Separation and Purification Technology, 2023, 307:122766.
• [20] GAO W L, VASILIADES M A, DAMASKINOS C M, et al. Molten salt-promoted MgO adsorbents for CO2 capture:Transient kinetic studies[J]. Environmental Science&Technology, 2021, 55(8):4513-4521.
• [21] ZHENG Y H, WU J Y, ZHANG L J, et al. Unravelling the pore templating effect on CO2 adsorption performance of alkali metal nitrates promoted MgO pellets[J]. Chemical Engineering Journal, 2022, 450:137944.
• [22] DING Y D, ZHAO X X, CHEN L, et al. Hydration activation of MgO pellets for CO2 adsorption[J]. Industrial&Engineering Chemistry Research, 2021, 60(14):5310-5318.
• [23] HU Y C, LIU X W, ZHOU Z J, et al. Pelletization of MgO-based sorbents for intermediate temperature CO2 capture[J]. Fuel, 2017,187:328-337.
• [24] CAI Y F, LIU W, SUN Z, et al. Granulation of alkaline metal nitrate promoted MgO adsorbents and the low-concentration CO2capture performance in the fixed bed adsorber[J]. Journal of CO2 Utilization, 2022, 61:102047.
• [25] LIU W, CAI Y F, LUO M J, et al. Potential application of alkaline metal nitrate-promoted magnesium-based materials in the integrated CO2 capture and methanation process[J]. Industrial&Engineering Chemistry Research, 2022, 61(7):2882-2893.