钙基催化剂的设计合成及应用研究进展

doi:10.11949/0438-1157.20230193

摘要/Abstract

摘要：

钙基催化剂是以钙氧化物为金属活性位点的固体碱催化剂，具有绿色高效、廉价易得等优点，有较好的催化性能，可广泛应用于生物柴油制备、废水处理和焦油裂解重整等领域，已受到国内外研究者们越来越广泛的关注。主要介绍了钙基催化剂类型、应用研究现状及作用机理，概述了其在各个领域的研究进展，分析归纳了钙基催化剂设计合成思路的历程和趋势：从CaO、Ca(OH)₂等天然钙基催化剂到主动设计合成的负载型含Ca催化剂，指出了稳定高效钙基催化剂的设计合成是其实现进一步发展的关键。最后对钙基催化剂研究进展进行归纳总结，并对其未来发展及应用前景进行了展望。

关键词: 钙, 催化剂, 催化氧化, 催化裂解, 生物柴油合成

Abstract:

Calcium-based catalyst are solid base catalyst with calcium oxides as metal active sites. It has the advantages of being green and efficient, cheap and easy to obtain, and has good catalytic performance. It can be widely used in the fields of biodiesel preparation, wastewater treatment, and tar cracking and reforming. They have received more and more attention from researchers all over the world. This article introduces the types of calcium-based catalysts, their application research status and mechanism of action, outlines their research progress in various applications, and analyzes and summarizes the history and trends of calcium-based catalyst design and synthesis ideas. From natural calcium-based catalysts such as CaO and Ca(OH)₂ to actively designed and synthesized loaded Ca-containing catalyst, it is pointed out that the synthesis of stable and efficient calcium-based catalysts is the key to realize their further development. Finally, the research progress of calcium-based catalysts is summarized and its future development and application prospects are prospected.

Key words: calcium, catalyst, catalytic oxidation, catalytic cracking, biodiesel synthesis

中图分类号:

O 641.3

涂玉明, 邵高燕, 陈健杰, 刘凤, 田世超, 周智勇, 任钟旗. 钙基催化剂的设计合成及应用研究进展[J]. 化工学报, 2023, 74(7): 2717-2734.

Yuming TU, Gaoyan SHAO, Jianjie CHEN, Feng LIU, Shichao TIAN, Zhiyong ZHOU, Zhongqi REN. Advances in the design, synthesis and application of calcium-based catalysts[J]. CIESC Journal, 2023, 74(7): 2717-2734.

图/表 20

图1 A-SBC、30Ca/A-SBC- 600、30Ca/A-SBC-700、30Ca/A-SBC-800、20Ca/A-SBC-700、40Ca/A-SBC-700的XRD谱图[28]

Fig.1 XRD patterns of A-SBC, 30Ca/A-SBC- 600, 30Ca/A-SBC-700, 30Ca/A-SBC-800, 20Ca/A-SBC-700 and 40Ca/A-SBC-700[28]

图2 SBC、A-SBC、30Ca/A-SBC-700的SEM图[28]

Fig.2 SEM images of SBC, A-SBC, and 30Ca/A-SBC-700[28]

图3 乙酸钙、UCN前体、UCA前体、UCA700和UCN650（UCN、UCA分别代表在氮气和空气气氛中活化）(CaZrO3, Ca x Zr y O x+2y )[29], CaO-Al2O3和0.4-SrO-CaO-Al2O3催化剂的XRD谱图[31]

Fig.3 XRD patterns of calcium acetate, UCN precursor, UCA precursor, UCA700 and UCN650 (UCN, UCA represent activation in nitrogen and air atmosphere, respectively) (CaZrO3, Ca x Zr y O x+2y )[29], CaO-Al2O3 and 0.4-SrO-CaO-Al2O3 catalysts[31]

图4 催化剂的重复使用性能(a); 新鲜和回收催化剂的XRD谱图(b)[32]

Fig.4 Reuse performance of catalysts (a); XRD patterns of fresh and recycled catalysts (b)[32]

图5 果胶与Ca2+的相互作用[33]

Fig.5 Interaction of pectin with Ca2+[33]

表1 不同催化剂在生物柴油合成过程中的效果对比

Table 1 Comparison of the effects of different catalysts in the biodiesel synthesis process

催化剂	转化率/%	稳定性
CaO^[28]（焙烧法）	87	多次使用后下降了30%
CaO/SBC^[28]（浸渍法）	93.4	多次使用后下降了9%
CaO-ZrO₂^[29]（掺杂改性）	97	使用3次后保持在93%以上
CaO-MgO^[30]（水热法）	98.4	使用5次后保持在93%以上
Ca/APB^[32] (Si改性)	81.6	使用10次后基本保持稳定
CaP-600^[33]（化学交联）	99	微量浸出

图6 Al2O3-PDA-Ca x O y 催化剂设计合成思路示意图[16]

Fig.6 Roadmap of Al2O3-PDA-Ca x O y catalyst synthesis[16]

表2 不同催化剂处理实际废水的效果对比

Table 2 Comparison of the effectiveness of different catalysts in treating actual wastewater

催化剂	废水类型	COD/ (mg·L^-1)	COD 去除率/%
煤基活性炭^[55]	煤化工废水生化出水	283.8	32.16
AC^[56]	纺织废水	2570	50
FeO _x /AC^[57]	炼油厂废水	54.6~256	40
γ-Al₂O₃^[58]	石化废水	750	46
CuCo/CAF_Ni^[59]	煤气化废水	70~80	60~65
Mn _x Ce_1-_x /γ-Al₂O₃^[60]	焦化废水	150	45.6
Al₂O₃-PDA-Ca _x O _y^[16]	石化废水（生化出水）	140~160	62
Ca-C/Al₂O₃^[17]	化工园区废水（生化出水）	100~129	65
Al₂O₃-PDA-SA-Ca _x O _y^[18]	化工园区废水（生化出水）	100~129	66

图7 Ca-C/Al2O3催化剂制备流程示意图[17]

Fig.7 Schematic diagram of the Ca-C/Al2O3 catalyst preparation process[17]

图8 Al2O3-PDA-SA-Ca x O y 催化剂制备流程示意图[18]

Fig.8 Schematic diagram of Al2O3-PDA-SA-Ca x O y catalyst preparation process [18]

图9 生物质炭基材料催化焦油原位催化裂解示意图[69]

Fig.9 Schematic diagram of in situ catalytic cracking of tar catalyzed by biomass carbon-based materials[69]

图10 含Ca、K的生物炭催化焦油模型化合物的重整机制（a）[70]；催化剂表面焦炭沉积过程（b）[72]（碳在催化活性表面颗粒上的化学吸附（ⅰ），焦炭包裹无机分子（ⅱ），焦炭沉积阻塞多孔结构（ⅲ），焦炭沉积导致的催化剂结构退化（ⅳ））

Fig.10 Mechanism of Ca- and K-containing biochar-catalyzed reformation of tar model compounds (a)[70]; Catalyst surface coke deposition process (b)[72]: chemisorption of carbon on catalytically active surface particles (ⅰ), coke encapsulation of inorganic molecules (ⅱ), coke deposition blocking porous structures (ⅲ), and catalyst structural degradation due to coke deposition (ⅳ)

图11 Ca基催化剂效果对比（a）；Ca基催化剂的XRD谱图（b）；反应机制示意图（c）[74]

Fig.11 Comparison of the effect of Ca-based catalysts (a); XRD pattern of Ca-based catalysts (b); Schematic representation of the reaction mechanism (c)[74]

表3 不同催化剂在焦油裂解重整过程中的效果对比

Table 3 Comparison of the effects of different catalysts in tar cracking reforming process

催化剂	反应体系	反应温度/℃	转化率/%	H₂摩尔分数/%
白云石颗粒^[66]	模拟焦油(乙酸、苯)	850	99.8、18.7	—
白云石焙烧物^[67]	生物质焦油	900	95.14	—
Ca-K/生物炭^[70]	模拟焦油(甲苯、萘)	800	86~100	62
Ca/CPC^[74]	模拟焦油(甲苯)	900	94.4	68.5
Fe₆Al₄Ca₁^[75]	煤焦油	900	90	50
Ni/生物炭^[76]	生物质焦油	800	96.5	—
Fe/生物炭^[77]	生物质焦油	800	92.6	39.88
Cu/生物炭^[77]	生物质焦油	800	90.6	—

图12 Ca(OH)2吸附臭氧的DRIFTS光谱[79]

Fig.12 DRIFTS spectra of ozone adsorption by Ca(OH)2[79]

图13 臭氧在Ca(OH)2表面脱附的DRIFTS光谱[79]

Fig.13 DRIFTS spectra of ozone desorption on Ca(OH)2 surfaces[79]

图14 Ca(OH)2催化臭氧氧化肉桂醛的反应机理[79]

Fig.14 Reaction mechanism of Ca(OH)2-catalyzed ozone oxidation of cinnamaldehyde[79]

图15 Ca(OH)2催化剂降解VOCs过程反应机理[82]

Fig.15 Reaction mechanism of VOCs removal process by CaO catalyst [82]

图16 Ca-OH/(N/C)双位点协同催化机制示意图[18]

Fig.16 Schematic diagram of the Ca-OH/(N/C) dual-site synergistic catalytic mechanism[18]

图17 钙基催化剂反应机理概述

Fig.17 Overview of the reaction mechanism of calcium-based catalysts

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