吸附强化蒸汽重整制氢中CO2固体吸附剂的研究进展

doi:10.16085/j.issn.1000-6613.2018-2243

摘要/Abstract

摘要：

吸附强化蒸汽重整（SESR）制氢技术是集重整反应（H₂生产）和选择性分离（CO₂吸附）于一体的新型技术。该技术的特点为采用固体吸附剂在高温下对CO₂进行原位脱除，以改变反应的正常平衡极限，提高烃类转化率，提高H₂产量，减少CO₂排放。在整个SESR制氢技术中，吸附剂的选择与反应条件至关重要。本文探讨了CaO、水滑石、Li₂ZrO₃、Li₂SiO₃以及双功能吸附剂在SESR制氢过程中的性能，总结了提高这些吸附剂吸附性能的不同方法。确定了固体吸附剂的反应条件，如温度、压力、水蒸气量等因素的影响及相关的反应机理。分析表明，CaO基吸附剂由于其低廉的价格及较高的吸附能力，被认为是最具潜力的吸附剂，然而在SESR制氢过程中，CaO基吸附剂面临着多次循环再生后吸附能力衰减的挑战。集吸附与催化双重功能的吸附催化材料由于可以克服SESR制氢中不同固体催化剂和吸附剂的匹配问题、降低所用固体材料的成本，从而使其在吸附强化蒸汽重整制氢方面具有巨大优势，并成为该领域未来研究的一个重要方向。

关键词: 二氧化碳, 吸附剂, 吸附（作用）, 蒸汽重整, 制氢

Abstract:

The sorption enhanced steam reforming (SESR) hydrogen production is an new technology consisting of reforming reaction (H₂ production) and selective separation (CO₂ sorption). The technology is characterized by in situ removal of CO₂ by solid adsorbent at high temperature to change the normal equilibrium limit of the shift reaction, increase hydrocarbons conversion and H₂ production with reduced CO₂emission. The selection of suitable sorbents and reaction conditions during sorption-enhanced steam reforming for high-purity hydrogen production is of vital importance.This study discussed the performances of CaO, hydrotalcite, Li₂ZrO₃, Li₂SiO₃and bifunctional based sorbents during sorption-enhanced steam reforming for high-purity hydrogen production, while different methods for enhancing these sorbents activities were summarized. The factors of reaction conditions such as temperature, pressure, the amount of water vapor etc. and related reaction mechanisms using these solid sorbents are identified. The results show that CaO-based adsorbents are considered to be the most potential adsorbents due to their low cost and high adsorption capacity. Nevertheless, the deactivation of CaO during multi-cycles carbonation-regeneration is challenging for continuous long-term operating conditions for hydrogen production from catalytic steam reforming. However, in the process of hydrogen production by SESR, CaO-based adsorbents are facing the challenge of attenuation of adsorption capacity after multi-cycles carbonation-regeneration. The multifunctional sorbent-catalyst materials having a dual function of catalytic steam reforming and in-situ CO₂ removal has great advantages in SESR because they can overcome the problems related with handling of different solids of catalyst and sorbent and decrease the cost of the total solid material used. What’s more, the multifunctional sorbent-catalyst materials will become an important direction for future research in this field.

Key words: carbon dioxide, adsorbents, adsorption, steam reforming, hydrogen production

中图分类号:

O643

王云珠,泮子恒,赵燚,罗永明,高晓亚. 吸附强化蒸汽重整制氢中CO₂固体吸附剂的研究进展[J]. 化工进展, 2019, 38(11): 5103-5113.

Yunzhu WANG,Ziheng PAN,Yi ZHAO,Yongming LUO,Xiaoya GAO. Research progress in CO₂ solid sorbents for hydrogen production by sorption-enhanced steam reforming: a review[J]. Chemical Industry and Engineering Progress, 2019, 38(11): 5103-5113.

图/表 6

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稳定吸附剂	稳定剂含量/％	吸附条件	再生条件	循环次数 /次	CO₂吸附 /gCO₂?g^-1	参考文献
Ca₁₂Al₁₄O₃₃	7.7	650℃，15% CO₂，30min	900℃，100% N₂，10min	30	0.600	[36]
Ca₁₂Al₁₄O₃₃	—	690℃，15% CO₂，60min	950℃，100% N₂，15min	7	0.660	[37]
Al₂O₃	19	750℃，40% CO₂，20min	750℃，100% N₂，20min	30	0.360	[38]
Ca₉Al₆O₁₈	20	650℃，15% CO₂，30min	800℃，100% N₂， 10min	35	0.520	[39]
Ca₃Al₂O₆	34	690℃，15% CO₂，30min	800℃，100% N₂，5min	45	0.450	[40]
CaN₄₀Al₁	—	690℃，15% CO₂，45min	900℃，100% N₂，20min	60	0.400	[41]
MgO	25	700℃，20%CO₂，10min	730℃，100% N₂，10min	50	0.540	[42]
ZrO	34	650℃，15% CO₂/N₂，30min	850℃，100% N₂，5min	20	0.484	[43]
CaZrO₃	26.2	650℃，15% CO₂，30min	750℃，100% Ar，30min	25	0.290	[44]
Y₂O₃	20	650℃，20% CO₂，30min	850℃，100% N₂，5min	10	0.570	[45]
TiO₂	10	600℃，20% CO₂，10min	750℃，100% N₂，10min	40	0.230	[46]
Y₂O₃，MgO	40	650℃，15% CO₂/N₂，15min	900℃，100% N₂，8min	122	0.311	[47]

稳定吸附剂	稳定剂含量/％	吸附条件	再生条件	循环次数 /次	CO₂吸附 /gCO₂?g^-1	参考文献
Ca₁₂Al₁₄O₃₃	7.7	650℃，15% CO₂，30min	900℃，100% N₂，10min	30	0.600	[36]
Ca₁₂Al₁₄O₃₃	—	690℃，15% CO₂，60min	950℃，100% N₂，15min	7	0.660	[37]
Al₂O₃	19	750℃，40% CO₂，20min	750℃，100% N₂，20min	30	0.360	[38]
Ca₉Al₆O₁₈	20	650℃，15% CO₂，30min	800℃，100% N₂， 10min	35	0.520	[39]
Ca₃Al₂O₆	34	690℃，15% CO₂，30min	800℃，100% N₂，5min	45	0.450	[40]
CaN₄₀Al₁	—	690℃，15% CO₂，45min	900℃，100% N₂，20min	60	0.400	[41]
MgO	25	700℃，20%CO₂，10min	730℃，100% N₂，10min	50	0.540	[42]
ZrO	34	650℃，15% CO₂/N₂，30min	850℃，100% N₂，5min	20	0.484	[43]
CaZrO₃	26.2	650℃，15% CO₂，30min	750℃，100% Ar，30min	25	0.290	[44]
Y₂O₃	20	650℃，20% CO₂，30min	850℃，100% N₂，5min	10	0.570	[45]
TiO₂	10	600℃，20% CO₂，10min	750℃，100% N₂，10min	40	0.230	[46]
Y₂O₃，MgO	40	650℃，15% CO₂/N₂，15min	900℃，100% N₂，8min	122	0.311	[47]

吸附剂	吸附温度/℃	吸附压力/MPa	再生温度/℃	循环次数/次	吸附能力/gCO₂·g^-1	参考文献
K₂CO₃-HTlc	500	0.15	—	30	0.036	[51]
K₂CO₃-HTlc	200～500	0.10	500	8	0.050	[58]
HTlc-10Ga	300	0.10	300	5	0.080	[59]
cK-HTCGa MW	300	0.31	673	4	0.084	[60]
Na-HTlc	200	0.10	—	—	0.046	[61]

吸附剂	吸附温度/℃	吸附压力/MPa	再生温度/℃	循环次数/次	吸附能力/gCO₂·g^-1	参考文献
K₂CO₃-HTlc	500	0.15	—	30	0.036	[51]
K₂CO₃-HTlc	200～500	0.10	500	8	0.050	[58]
HTlc-10Ga	300	0.10	300	5	0.080	[59]
cK-HTCGa MW	300	0.31	673	4	0.084	[60]
Na-HTlc	200	0.10	—	—	0.046	[61]

催化剂	比表面积 /m²·g^-1	最佳吸附能力 /gCO₂·g^-1	最佳反应温度 /℃	氢气选择性（吸附饱和前）/％	参考文献
CeO₂-Ca₉Al₆O₁₈-CaO/NiO	15.40	0.420	550	98.0	[74]
Ni-CaO-Al₂O₃	29.00	0.248	500	99.4	[73]
Ni-CaO-MMT	58.80	0.250	600	100.0	[8]
Ni/(CaO/Al₂O₃)	45.23	0.042	550	99.9	[76]
K-Ni-Cu-HTlc	38.00	0.030	500	99.8	[77]
Ni/CaO-MgO-Al₂O₃	123.00	—	600	99.0	[78]
Fe/CaO-Ca₁₂Al₁₄O₃₃	7.60	0.660	700	98.0	[37]

吸附强化蒸汽重整制氢中CO₂固体吸附剂的研究进展

Research progress in CO₂ solid sorbents for hydrogen production by sorption-enhanced steam reforming: a review

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