辐射冷却和太阳能加热驱动的CO2变温捕获

doi:10.11949/0438-1157.20221078

摘要/Abstract

摘要：

变温吸附是一种有效的二氧化碳(CO₂)捕集技术，但变温过程需要消耗大量能量，尤其是加热和降温过程。将被动辐射制冷和太阳能加热相结合并应用于聚吡咯基氮掺杂多孔碳PPy-650对CO₂的捕集过程，从而实现变温系统的低能耗。在吸附过程中，聚(偏氟乙烯-六氟丙烯)膜[P(VdF-HFP)_HP]覆盖于吸附剂层，在太阳光照射下通过辐射冷却效应将吸附剂冷却至室温以下。对于脱附过程，将具有优异光热转换能力的PPy-650暴露在太阳光下，利用光能进行加热。整个加热和冷却过程完全由太阳能驱动，不需要额外消耗能量。700 W/m²模拟光下的吸附-脱附循环测试结果表明，PPy-650在这一变温吸附系统中具有良好的CO₂工作容量(35.69 cm³/g)。经过真实太阳光下的吸附/脱附循环后，PPy-650的吸附能力未见下降。

关键词: CO₂捕集, 吸附, 太阳能, 辐射制冷, 氮掺杂多孔碳

Abstract:

Temperature-swing adsorption is an effective technique for CO₂ capture, but the temperature swing procedure is energy-intensive, especially the heating and cooling processes. The low-energy-consumption temperature-swing system is realized by using polypyrrole-based nitrogen-doped porous carbon PPy-650 which combines passive radiative cooling and solar heating. During the adsorption process, the adsorbent layer is coated with a layer of hierarchically porous poly (vinylidene fluoride-co-hexafluoropropene) [P(VdF-HFP)_HP], which can cool the adsorbents to a sub-ambient temperature under sunlight through radiative cooling. For desorption, PPy-650 with excellent photothermal conversion ability is exposed to light irradiation for heating. The heating and cooling process is driven entirely by solar energy without any energy input. The regeneration of PPy-650 was investigated by means of adsorption-desorption cycles carried out at 700 W/m². The results demonstrate that PPy-650 has a good CO₂ working capacity (35.69 cm³/g) in this temperature-swing adsorption system, the adsorption capacity of PPy-650 did not decrease.

Key words: CO₂ capture, adsorption, solar energy, radiative cooling, N-doped porous carbon

中图分类号:

TQ 028.8

党迎喜, 谈朋, 刘晓勤, 孙林兵. 辐射冷却和太阳能加热驱动的CO₂变温捕获[J]. 化工学报, 2023, 74(1): 469-478.

Yingxi DANG, Peng TAN, Xiaoqin LIU, Linbing SUN. Temperature swing for CO₂ capture driven by radiative cooling and solar heating[J]. CIESC Journal, 2023, 74(1): 469-478.

图/表 10

图1 低能耗CO2变温吸附/脱附系统

Fig.1 Low-energy-consumption CO2 temperature swing adsorption/desorption system

图2 吸附装置与材料的表征(a)吸附装置照片(光功率计和温度测试仪分别用于记录太阳光强度和周围环境温度); (b),(c)176 μm厚的聚合物P(VdF-HFP)HP膜的SEM图(插图为该膜的照片); (d)P(VdF-HFP)HP膜的反射率和发射率; (e)辐射降温性能测试[于中国南京(30o51´~32o15´N,118o21´~118o46´E)室外环境中测得],包括太阳光强度、环境和P(VdF-HFP)HP膜的温度及两者的温差;(f)PPy-650在700 W/m2连续模拟光照射下的热成像图; (g)在700 W/m2连续模拟光照射下吸附剂的膜上温度(Solar heating)和膜下温度(Radiative cooling); (h)PPy-650和商业活性炭(Commercial AC)的光吸收度对比

Fig.2 Adsorption devices and characterization of the materials

图3 PPy和PPy-T的结构表征

Fig.3 Structure characterization of PPy and PPy-T

表1 样品的理化性质

Table 1 Physicochemical properties of the samples

Sample	S_BET/ (m²/g)	V_t/ (cm³/g)	V_micro/ (cm³/g)	元素组成/%(质量)
Sample	S_BET/ (m²/g)	V_t/ (cm³/g)	V_micro/ (cm³/g)	C	H	N	吡啶氮	吡咯氮	四级型氮
PPy	35	0.13	0.05	53.38	3.68	16.03	—	—	—
PPy-450	614	0.33	0.15	55.41	3.62	11.99	3.02	8.02	0.95
PPy-550	1096	0.51	0.44	52.51	3.65	9.95	3.20	5.84	0.91
PPy-650	2134	1.08	0.89	63.27	2.45	6.71	1.36	3.20	2.15
PPy-750	3163	1.50	1.39	84.26	2.80	2.22	0.34	1.04	0.84

图4 样品的SEM图

Fig.4 SEM images of samples

图5 PPy-650的微孔及表面元素分布

Fig.5 Distribution of micropores and surface elements of PPy-650

图6 样品的FT-IR谱图

Fig.6 FT-IR spectra of samples

图7 PPy-T的XPS的N 1s拟合谱图

Fig.7 XPS peak fitting of the N 1s spectra of PPy-T

图8 CO2和N2吸附性能(a),(b)35℃和60℃, 1 bar下的样品吸附等温线; (c)样品的CO2工作容量; (d)样品的等量吸附热和再生率比较; (e)在700 W/m2模拟太阳光照射下, 吸附时装置的照片(Ⅰ)和热成像图(Ⅱ)以及脱附时装置的照片(Ⅲ)和热成像图(Ⅳ); (f)PPy-650的动态穿透曲线; (g)PPy-650的吸附-脱附循环过程; (h)真实太阳光下PPy-650的循环性能[2022年6月30日~7月9日在中国南京(30o51´~32o15´N,118o21´~118o46´E)测定, 红色虚线为700 W/m2模拟太阳光制热时PPy-650的穿透吸附量]

Fig.8 CO2 and N2 adsorption performance

图9 样品上的CO2/N2的IAST吸附选择性(a)和CO2的等量吸附热(b)

Fig.9 IAST selectivity of CO2/N2 (a) and CO2 isosteric heat of adsorption (b) on samples

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辐射冷却和太阳能加热驱动的CO₂变温捕获

Temperature swing for CO₂ capture driven by radiative cooling and solar heating

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