化学链制化学品工艺及循环材料研究进展

doi:10.11949/0438-1157.20230739

摘要/Abstract

摘要：

化学链技术在化学品生产过程强化方面表现出极大潜力，相较于传统工艺可提高㶲效率并降低碳排放。综述了目前常见的化学链制化学品工艺，主要包括化学链重整/部分氧化制合成气和氢气、低碳烷烃化学链氧化脱氢/选择性氢燃烧制烯烃、甲烷化学链氧化偶联制乙烯、甲烷化学链脱氢芳构化制苯、化学链选择性氧化制含氧有机化合物（如甲醇、环氧乙烷和甲酸等）。深入理解载氧体理化性质与化学链反应性能间的构效关系有助于实现载氧体理性设计。目前在载氧体设计方面已具备坚实的理论基础，从利用氧化物的热力学平衡氧分压筛选载氧体活性组分，到基于表面工程策略调控晶格氧释放动力学，再到通过合理构建结构和电子描述符，深入剖析载氧体性能强化策略。实验和密度泛函理论（DFT）计算数据驱动的可解释机器学习可实现载氧体的高通量筛选，极大拓宽了载氧体筛选范围，并降低试错成本。随着化学链技术的发展，载氧体这一概念可被进一步拓展至循环材料，如载氮体和载氯体等。光/电驱动的化学链过程为在低温或室温下实现高附加值产物的合成提供了新思路，拓宽了化学链技术的应用范围。此外，化学链技术还可用于共沸有机物分离过程强化，对低成本、低污染和低排放分离过程的开发具有重要意义。

关键词: 化学链, 重整, 载氧体, 循环材料, 选择性氧化

Abstract:

Chemical looping technology demonstrates significant potential for enhancing chemical production processes compared to traditional processes, resulting in increased exergy efficiency and reduced carbon emissions. This review focuses on common chemical looping processes for chemical production, including chemical looping reforming/partial oxidation (CLR/CLPO) of methane for syngas and hydrogen production, light alkanes chemical looping oxidative dehydrogenation (CL-ODH) or chemical looping selective hydrogen combustion (CL-SHC) for olefin production, chemical looping oxidation coupling of methane (CL-OCM) for ethylene production, chemical looping dehydrogenation aromatization (CL-DHA) of methane for benzene production, and chemical looping selective oxidation (CL-SO) for oxygen-containing organic compound production (such as methanol, ethylene oxide, and formic acid). A fundamental understanding of the structure-activity relationship between the textual properties of oxygen carriers and chemical looping reaction performance is paramount for achieving the rational design of oxygen carriers. At present, we have a solid theoretical foundation in the design of oxygen carriers. We use the thermodynamic equilibrium oxygen partial pressure of oxides to screen the active components of oxygen carriers, and from controlling the lattice oxygen release kinetics based on surface engineering strategies to in-depth analysis of oxygen carrier performance enhancement strategies through the rational construction of structural and electronic descriptors. Experimental and density functional theory (DFT) computational data-driven interpretable machine learning (ML) can enable high-throughput screening of oxygen carriers, which greatly broadens the screening range and reduces the cost of experiment time. With the development of chemical looping technology, the concept of oxygen carrier can be further extended to looping material (LM), such as nitrogen and chloride carriers. Photo/electro-driven chemical looping processes provide new routes to synthesize high-value-added products at low temperatures or even room temperatures, thereby broadening the application scope of chemical looping technology. Additionally, chemical looping technology can be applied to enhance the separation process of binary azeotropic organic mixtures, which is of great significance for developing low-cost, low-pollution, and low-emission separation processes.

Key words: chemical looping, reforming, oxygen carriers, looping materials, selective oxidation

中图分类号:

TQ 519

张榕江, 张博, 刘根, 杨伯伦, 吴志强. 化学链制化学品工艺及循环材料研究进展[J]. 化工学报, 2023, 74(10): 3979-3994.

Rongjiang ZHANG, Bo ZHANG, Gen LIU, Bolun YANG, Zhiqiang WU. Progress in chemical looping process for chemical production and looping materials research[J]. CIESC Journal, 2023, 74(10): 3979-3994.

图/表 17

图1 常见化学链过程示意图

Fig.1 Schematic diagram of common chemical looping processes

表1 甲烷化学链重整载氧体反应性能对比

Table 1 Comparison of reaction performance of oxygen carriers for methane chemical looping reforming

载氧体	原料组成	再生气氛	温度/℃	空速或流速/(ml/min)	转化率/%	合成气产量/(mmol/g)	文献
Ni-(α-MoC)/Al₂O₃	5% CH₄/Ar	5% CO₂/Ar	500	100	62	4.2	[19]
Rh-LaCeO_4-_x	10% CH₄/Ar	2% CO₂/Ar	650	50	88	0.5	[20]
La_0.8Ce_0.1Ni_0.4Ti_0.6O₃	5% CH₄/He	5% O₂/He	650	50	45	3.5	[21]
Fe₂O₃@SBA-16	20% CH₄/N₂	10% O₂/N₂	800	200	28	3.3	[18]
Ni_0.5WO _x /Al₂O₃	16.7% CH₄/Ar	10% O₂/He	800	30	58	3.8	[22]
10% CeO₂/LaFeO₃	5% CH₄/Ar	H₂O/N₂	800	200	67	9.9	[23]
La_1.6Sr_0.4FeCoO₆	40% CH₄/N₂	H₂O/N₂	850	50	45	7.0	[24]
La_0.5Ce_0.5FeO₃	10% CH₄/N₂	10% CO₂/N₂	850	80	80	4.2	[25]
BaFe₃Al₉O₁₉	5% CH₄/He	5% O₂/He	850	15	86	4.2	[13]
La_0.85Sr_0.15Fe_0.95Al_0.05O₃	5% CH₄/N₂	5% CO₂/N₂	900	700	79	10.6	[26]
NiFe₂O₄@SBA-15	10% CH₄/Ar	10% O_2/Ar	900	100	47	5.2	[17]
Y₃Fe₂Al₃O₁₂	5% CH₄/He	—	900	30	94	4.7	[12]
FeWO₃/SiO₂	10% CH₄/N₂	21% O₂/N₂	900	60	62	4.1	[27]

图2 负载与溶出颗粒的对比以及溶出颗粒促进晶格氧迁移[21]

Fig.2 Comparison of supported and exsolved particles and the promotion of lattice oxygen migration by exsolved particles[21]

图3 传统蒸汽重整工艺与化学链脱氢工艺㶲损失对比[40]

Fig.3 Comparison of exergy losses during traditional steam reforming and chemical looping dehydrogenation process[40]

图4 化学链脱氢的类型[41]

Fig.4 Types of chemical looping dehydrogenation[41]

表2 低碳烷烃化学链脱氢载氧体反应性能对比

Table 2 Comparison of reaction performance of oxygen carriers for light alkanes chemical looping dehydrogenation

反应类型	载氧体	原料组成	再生气氛	温度/℃	GHSV/h^-1	转化率/%	选择性/%	文献
CL-ODH	0.2Ce/SrFeO₃	25% C₂H₆/Ar	25% CO₂/Ar	700~750	6000	29	82	[42]
	FeCeTiO _x	20% C₂H₆/N₂	20% CO₂/Ar	600	—	13	84	[43]
	Co_0.3Mo_0.7/Fe₂O₃	10%~16.7% C₂H₆/Ar	16.7% O₂/Ar	775~825	6000	56	87	[44]
	Mg-La_1.6Sr_0.4FeCoO₆	40% C₂H₆/N₂	20% O₂/N₂	650~750	—	53	89	[45]
	NaW-LaMnO₃	40% C₂H₆/N₂	20% O₂/N₂	750~800	—	71	85	[46]
	La_0.8Sr_0.2FeO₃@Li₂CO₃	12.5%~80% C₂H₆/N₂	—	700	—	50	91	[47]
	Mo-V-O氧化物	19% C₃H₈/N₂	21% O₂/N₂	500	2500	36	89	[48]
	La_0.8Sr_0.2FeO₃@LiBr	19% C₄H₁₀/Ar	—	500	—	75	56	[49]
CL-SHC	Ni/HY	10% C₂H₆/He	5% O₂/He	600	5100	18	97	[50]
	Na₂WO₄-CaMn_0.9Fe_0.1O₃	80% C₂H₆/Ar	20% O₂/Ar	650~750	600	41	90	[51]
	Mg₆MnO₈@Na₂WO₄	80% C₂H₆/Ar	17% O₂/Ar	850	4500	81	76	[52]
	Mg₆MnO₈@Na₃PO₄	80% C₂H₆/He	17% O₂/He	800~850	4500	78	57	[53]
	Ce_0.92Pb_0.08O₂/PbO	C₃H₈∶C₃H₆∶H₂=4∶1∶1	1% O₂/Ar	550	13200	50	85	[54]
	Ce_0.9Bi_0.1O₂	C₃H₈∶C₃H₆∶H₂=4∶1∶1	1% O₂/Ar	550	13200	33	77	[55]

图5 用于比较金属氧化物的热力学平衡氧分压的改进Ellingham图[2]

Fig.5 Modified Ellingham diagram for comparing thermodynamic equilibrium oxygen partial pressures of metal oxides[2]

图6 利用碱/碱土金属表面修饰(a)以及惰性壳层包覆策略(b)降低表面氧通量[46-47,67-68]

Fig.6 Using alkali/alkaline earth metal surface-modification (a) and inert shell coating (b) to reduce surface oxygen flux[46-47,67-68]

图7 数据驱动的可解释机器学习实现载氧体的高通量筛选

Fig.7 High throughput screening of oxygen carriers using data-driven interpretable machine learning

图8 具有凹曲率结构的α-MoO3/Al2O3和凸曲率结构的H3PMo12O40/Al2O3丙烷化学链脱氢反应性能对比[71]

Fig.8 Reaction performance comparison of α-MoO3/Al2O3 with concave curvature and H3PMo12O40/Al2O3 with convex curvature for chemical looping dehydrogenation of propane[71]

图9 双活性位点及串联催化的化学链脱氢载氧体设计[50,78]

Fig.9 Design of chemical looping dehydrogenation oxygen carriers with dual active sites and tandem catalysis[50,78]

图10 以水为氧化介质的甲烷选择性氧化机理[95]（1 bar=0.1 MPa）

Fig.10 The mechanism of the selective oxidation of methane using water as oxidant[95]

图11 以生物基化学品作为还原剂在金属上的CO2水热还原制甲酸[107]

Fig.11 Hydrothermal reduction of formic acid by CO2 on metals with bio-based chemicals as reducing agents[107]

图12 光驱动的甲烷化学链氯化反应过程[109]

Fig.12 Photo-driven chemical looping chlorination of methane process[109]

图13 光驱动的基于甲烷硝化反应的化学链制甲醇反应过程[110]

Fig.13 Photo-driven chemical looping process for methanol production based on methane nitration reaction[110]

图14 由亚胺锂(Li2NH)介导的电驱动化学链合成氨过程[112]

Fig.14 Electro-driven chemical looping ammonia synthesis mediated by lithium imide (Li2NH)[112]

图15 化学链分离过程示意图[113]

Fig.15 Schematic diagram of chemical looping separation (CLS) process[113]

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