Current advances and development of bio-butanol separation techniques

doi:10.16085/j.issn.1000-6613.2020-2001

Abstract

Abstract:

Biobutanol (n-butanol) is an important bulk chemical and biofuel candidate, which can be obtained via acetone-butanol-ethanol (ABE) fermentation from biomass. Because of the low concentration of solvents products, the conventional biobutanol separation is costly and energy-intensive. To overcome the above limitation, recently, alternative separation techniques are emerged. In this review, the current advances of the potential alternative separation techniques, including the vapor-liquid equilibrium, solvents polarity-based techniques and membrane-based separation for biobutanol recovery are summarized, followed by discussing the multi-stage cascade separations. Facing the generation of commercial guide biobutanol production, the trends for ABE distillation is also included. With the improvement of separation technology and the development of biorefinery process, the overall cost of biobutanol production can be decreased, which would further improve the competitiveness of biobutanol process in terms of commercialization.

Key words: bio-butanol, ABE fermentation, in situ product recovery, membrane separation, distillation, biorefinery

摘要：

生物基（正）丁醇是一种重要的化学品和替代燃料，其主要制备途径为糖质底物的丙酮-丁醇-乙醇（ABE）发酵。受制于发酵副产物多、溶剂浓度低、产物共沸等因素，传统的生物丁醇分离过程存在分离能耗大、成本高等问题，制约其产业化制备。为解决生物丁醇分离的技术瓶颈，近年来，应用新型分离技术实现与ABE发酵过程的耦合成为研究的热点。本文综述了生物丁醇分离技术的最新研究进展，讨论了基于汽液平衡、相转移、膜分离技术等新型分离方式的技术特点；并针对多级分离级联系统开发、面向终产物的精馏技术的新趋势、新特点进行剖析和讨论。随着分离技术的发展和进步、生物炼制工艺开发和集成，生物丁醇的制备成本可望进一步降低，提升市场竞争力。

关键词: 生物丁醇, 丙酮-丁醇-乙醇发酵, 原位分离, 膜分离, 精馏, 生物炼制

CLC Number:

TQ028

CAI Di, LI Shufeng, SI Zhihao, QIN Peiyong, TAN Tianwei. Current advances and development of bio-butanol separation techniques[J]. Chemical Industry and Engineering Progress, 2021, 40(3): 1161-1177.

蔡的, 李树峰, 司志豪, 秦培勇, 谭天伟. 生物丁醇分离技术的研究进展及发展趋势[J]. 化工进展, 2021, 40(3): 1161-1177.

Figures/Tables 9

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项目	汽油	正丁醇	乙醇
化学式	H，C₄～C₁₂	C₄H₁₀O	C₂H₆O
分子量/g·mol^-1	114.23	74.12	46.07
密度（20℃）/g·m^-3	0.7	0.81	0.789
酸度，pK_a	—	16.1	15.9
黏度（25℃）/mPa·s	0.6	2.573	1.074
闪点（25℃）/℃	-43	35	17.2
自燃点/℃	280	343	365
热值/MJ·L^-1	32.5	29.2	21.2
空燃比	14.7	11.2	9
研究辛烷值（马达辛烷值）	91～99 (81～89)	96 (78)	129 (102)
蒸发热/MJ·kg^-1	0.36	0.43	0.92
相对密度（15℃）	0.72～0.78	0.81	0.79
沸点/℃	125	117.4	78.4
熔点/℃	-56.6	-89.8	-114
低热值/MJ·kg^-1	43.4	34.3	26.9
高热值/MJ·kg^-1	46.5	37.3	29.8
瑞德蒸气压/psi^①	8～15	0.3	2.3
水溶性（25℃）/%	—	7.3	100
含氧量/%	0	22	35

项目	汽油	正丁醇	乙醇
化学式	H，C₄～C₁₂	C₄H₁₀O	C₂H₆O
分子量/g·mol^-1	114.23	74.12	46.07
密度（20℃）/g·m^-3	0.7	0.81	0.789
酸度，pK_a	—	16.1	15.9
黏度（25℃）/mPa·s	0.6	2.573	1.074
闪点（25℃）/℃	-43	35	17.2
自燃点/℃	280	343	365
热值/MJ·L^-1	32.5	29.2	21.2
空燃比	14.7	11.2	9
研究辛烷值（马达辛烷值）	91～99 (81～89)	96 (78)	129 (102)
蒸发热/MJ·kg^-1	0.36	0.43	0.92
相对密度（15℃）	0.72～0.78	0.81	0.79
沸点/℃	125	117.4	78.4
熔点/℃	-56.6	-89.8	-114
低热值/MJ·kg^-1	43.4	34.3	26.9
高热值/MJ·kg^-1	46.5	37.3	29.8
瑞德蒸气压/psi^①	8～15	0.3	2.3
水溶性（25℃）/%	—	7.3	100
含氧量/%	0	22	35

技术	原理	优势	劣势
基于汽液平衡
精馏	在精馏塔中进行,气液两相通过逆流接触,进行相际传热传质。溶剂随挥发度差异逐一分离	可逐一分离得到单一脱水溶剂产物	不能与发酵过程耦合，能耗高
汽提	醪液罐或发酵罐底部持续通入载气，溶剂经载气气泡带出，进入冷却塔冷却获得高浓度ABE溶剂	操作简单，无细胞毒性，稳定性强，无污染	效率较低，对溶剂中丁醇主产物的选择性差
闪蒸	将发酵液泵入闪蒸罐，在低压下维持发酵液沸腾状态，气相抽出冷凝收集	无细胞毒性，对发酵系统影响小	效率较低，对溶剂中丁醇主产物的选择性差
真空分离	将发酵罐减压以改变气液分压，富含溶剂气相抽出后冷凝获得高浓度ABE溶剂	操作简单，无细胞毒性	效率较低，对溶剂中丁醇主产物的选择性差，溶剂产率低，易染菌，能耗较高
基于相转移
吸附	滤去细胞的发酵液泵入吸附柱与固相吸附介质充分接触，ABE溶剂附着在非极性介质表面，之后通过溶剂脱附或热脱附获得溶剂产物	吸附介质可回用，对溶剂选择性较高	吸附介质易污染，需要高温或溶剂介入脱附，能耗较高
液液萃取	疏水萃取剂直接接触发酵液，ABE溶剂因分配系数差异溶解于萃取剂中实现分离	操作简单，选择性高，能耗较低	高细胞毒性导致连续性差，萃取剂损失及形成乳液
浊点萃取	表面活性剂在低温下溶解于ABE发酵液中，随温度升高表面活性剂分子形成胶团，随温度升高胶团聚集实现溶剂分离	操作简单，分离效率高	不能与发酵过程耦合，表面活性剂用量大，成本高，分离能耗较高
盐析	利用盐析效应，在发酵液中加入盐析剂，低极性ABE溶剂水中溶解度降低，形成有机相	操作简单，分离效率高	不能与发酵过程耦合，连续性差，盐析剂用量大，回收工艺复杂
膜分离技术
渗透汽化	在膜两侧蒸汽分压差推动下，发酵液中的挥发性有机物选择性透过膜，在透过侧进行收集	无细胞毒性，可进行原位发酵分离耦合，能耗低	设备投资高，存在膜污染问题
渗透萃取	发酵液中的有机物渗透通过膜，为透过侧萃取剂所萃取	操作简单，无细胞毒性	传质效率低，产物收率低，存在膜污染问题
膜蒸馏	由于表面张力作用，液体无法通过疏水微孔膜，而蒸汽可以通过，在膜透过侧得以富集	无细胞毒性，对发酵体系无影响	存在膜污染问题，液体浸润疏水微孔膜后可导致性能下降
反渗透	在发酵液侧施加一定压力，水分子沿自然渗透方向相反的方向扩散进入膜另一侧，实现有机物的富集浓缩	可用于发酵废水回收	发酵液中的丙酮易破坏膜结构，膜寿命短

技术	原理	优势	劣势
基于汽液平衡
精馏	在精馏塔中进行,气液两相通过逆流接触,进行相际传热传质。溶剂随挥发度差异逐一分离	可逐一分离得到单一脱水溶剂产物	不能与发酵过程耦合，能耗高
汽提	醪液罐或发酵罐底部持续通入载气，溶剂经载气气泡带出，进入冷却塔冷却获得高浓度ABE溶剂	操作简单，无细胞毒性，稳定性强，无污染	效率较低，对溶剂中丁醇主产物的选择性差
闪蒸	将发酵液泵入闪蒸罐，在低压下维持发酵液沸腾状态，气相抽出冷凝收集	无细胞毒性，对发酵系统影响小	效率较低，对溶剂中丁醇主产物的选择性差
真空分离	将发酵罐减压以改变气液分压，富含溶剂气相抽出后冷凝获得高浓度ABE溶剂	操作简单，无细胞毒性	效率较低，对溶剂中丁醇主产物的选择性差，溶剂产率低，易染菌，能耗较高
基于相转移
吸附	滤去细胞的发酵液泵入吸附柱与固相吸附介质充分接触，ABE溶剂附着在非极性介质表面，之后通过溶剂脱附或热脱附获得溶剂产物	吸附介质可回用，对溶剂选择性较高	吸附介质易污染，需要高温或溶剂介入脱附，能耗较高
液液萃取	疏水萃取剂直接接触发酵液，ABE溶剂因分配系数差异溶解于萃取剂中实现分离	操作简单，选择性高，能耗较低	高细胞毒性导致连续性差，萃取剂损失及形成乳液
浊点萃取	表面活性剂在低温下溶解于ABE发酵液中，随温度升高表面活性剂分子形成胶团，随温度升高胶团聚集实现溶剂分离	操作简单，分离效率高	不能与发酵过程耦合，表面活性剂用量大，成本高，分离能耗较高
盐析	利用盐析效应，在发酵液中加入盐析剂，低极性ABE溶剂水中溶解度降低，形成有机相	操作简单，分离效率高	不能与发酵过程耦合，连续性差，盐析剂用量大，回收工艺复杂
膜分离技术
渗透汽化	在膜两侧蒸汽分压差推动下，发酵液中的挥发性有机物选择性透过膜，在透过侧进行收集	无细胞毒性，可进行原位发酵分离耦合，能耗低	设备投资高，存在膜污染问题
渗透萃取	发酵液中的有机物渗透通过膜，为透过侧萃取剂所萃取	操作简单，无细胞毒性	传质效率低，产物收率低，存在膜污染问题
膜蒸馏	由于表面张力作用，液体无法通过疏水微孔膜，而蒸汽可以通过，在膜透过侧得以富集	无细胞毒性，对发酵体系无影响	存在膜污染问题，液体浸润疏水微孔膜后可导致性能下降
反渗透	在发酵液侧施加一定压力，水分子沿自然渗透方向相反的方向扩散进入膜另一侧，实现有机物的富集浓缩	可用于发酵废水回收	发酵液中的丙酮易破坏膜结构，膜寿命短

发酵方式	发酵类型	底物	气提方式	菌种	冷凝浓度/g·L^-1			ABE转化率 /g·g^-1	ABE产率 /g·(L·h)^-1	参考文献
发酵方式	发酵类型	底物	气提方式	菌种	丙酮	丁醇	ABE	ABE转化率 /g·g^-1	ABE产率 /g·(L·h)^-1	参考文献
批次	固定化	葡萄糖	连续	C. acetobutylicum JB 200	—	—	—	0.32	0.47	[33]
	固定化	葡萄糖	连续	C. acetobutylicum JB 200	—	175.6	227	0.4	0.66	[37]
	固定化	葡萄糖	连续	C. acetobutylicum ABE 1201	44.2~66.5	97.9~166.8	155.7~255.6	0.4	0.36	[34]
	游离	木屑+葡萄糖	连续	C. acetobutylicum CC 101	—	—	42~96	0.39	0.13	[40]
补料批次	固定化	葡萄糖	间歇	C. acetobutylicum JB 200	20~50	150.5	195.9	0.36	0.53	[37]
	固定化	葡萄糖	间歇	C. acetobutylicum B 3	40	150	200	0.36	0.61	[35]
	固定化	葡萄糖	间歇	C. acetobutylicum ABE 1201	45~55	140~175	210~255	0.34	0.38	[37]
	游离	葡萄糖	连续	Cbeijerinckii BA 101	—	—	38.3~99.6	0.36	0.59	[38]
	固定化	葡萄糖	连续	C. acetobutylicum JB 200	26~50	100~160	155~210	0.37	0.53	[39]
	固定化	葡萄糖	连续	C. acetobutylicum ABE 1201	~50	115	155~205	0.38	1.15	[37]
	固定化	木薯渣	连续	C. acetobutylicum JB 200	25.7	59.8	90.3	0.37	0.53	[41]
	游离	葡萄糖	间歇	C. acetobutylicum TSH1; B. cereus TSH2	56.49	185.65	267.15	0.33	0.93	[42]
	固定化	高粱汁	连续	C. acetobutylicum ABE 1201	44.1	112.9	166.5	0.41	0.53	[43]
	固定化	玉米秸秆	间歇	C. acetobutylicum ABE-P 1201	—	77~136	115~220	0.29	0.13	[44]
连续	固定化	乳清	连续	C. acetobutylicum P 262	—	—	53.7	0.4	5.12	[45]