硼基催化剂丙烷氧化脱氢制丙烯

doi:10.16085/j.issn.1000-6613.2021-2203

摘要/Abstract

摘要：

自2016年Hermans课题组发现六方氮化硼（h-BN）在丙烷氧化脱氢制丙烯（ODHP）反应中优异的烯烃选择性，各类硼基材料引起了研究者强烈的研究兴趣并广泛地用于ODHP反应。与传统金属与金属氧化物基催化剂不同，非金属硼基催化体系能够有效抑制CO _x 等过度氧化产物，提高烯烃产率，具有较广阔的工业应用前景。本综述对硼基丙烷氧化脱氢催化剂从催化剂的设计、合成策略和反应性能等方面进行了系统地讨论，阐明了催化剂的构效关系；总结了反应路线、关键中间体、决速步以及催化动力学行为，加深了硼基催化剂催化丙烷氧化脱氢活性位点和机理的理解。指出三配位B—O/B—OH活性位点的有效构建及实现表面与气相自由基反应的协同催化是提高硼基催化剂丙烷脱氢性能的关键。基于目前的研究现状和存在的问题，对硼基催化剂体系研发前景和未来工业化应用进行了展望。

关键词: 丙烷, 氧化脱氢, 硼基催化剂, 丙烯

Abstract:

Since the discovery of highly selective and efficient hexagonal boron nitride(h-BN) in 2016 as the catalyst for oxidative dehydrogenation of propane(ODHP) to propene, the boron-based materials have aroused significant research interests. Unlike traditional metal and transition metal oxide-based ODHP catalysts, the metal-free boron-based materials exhibit high industrial prospects due to their low overoxidation, high olefin productivity and environmental friendliness. In this review, the characteristics of different boron-based catalysts have been systematically discussed from the aspects of catalyst design, synthesis strategy and ODHP performance. Meanwhile, the reaction mechanisms are elaborated based on the potential reaction routes, key intermediates, rate-determining step as well as the catalytic kinetics behaviors, which could provide a comprehensive and insightful understanding of the active sites and structure-activity relationship of boron-based catalysts. It is recognized that the effective construction of the tri-coordination B-O/B-OH active sites and the realization of the synergistic catalysis of the surface and gas radical reactions are the key to improve the performance of propane dehydrogenation over boron-based catalysts. Based on the current researches and existing problems, the future development and industrial application of boron-based catalyst systems are prospected.

Key words: propane, oxidative dehydrogenation, boron-based catalyst, propene

中图分类号:

TQ051

高晓峰, 黄永康, 徐文豪, 周娴, 姚思宇, 马丁. 硼基催化剂丙烷氧化脱氢制丙烯[J]. 化工进展, 2022, 41(3): 1409-1429.

GAO Xiaofeng, HUANG Yongkang, XU Wenhao, ZHOU Xian, YAO Siyu, MA Ding. Oxidative dehydrogenation of propane to propene over boron-based catalysts[J]. Chemical Industry and Engineering Progress, 2022, 41(3): 1409-1429.

图/表 21

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分类	催化剂	温度/℃	转化率/%	选择性/%					产率/g_olefin·g_cat^-1·h^-1	参考文献
分类	催化剂	温度/℃	转化率/%	C₄⁼	C₃⁼	C₂⁼	CO	CO₂	产率/g_olefin·g_cat^-1·h^-1	参考文献
BN基催化剂	h-BN	490	14	—	79	12	9	—	0.5	［14］
	BNNTs	490	16.5	—	72	—	—	—	3.7	［14］
	高比表面积BN	525	24	—	69	—	—	—	0.04	［32］
	羟化BN	530	20.6	—	80.6	10.7	7.9	0.5	7.74	［51］
	SS-BNNSs	490	20	—	78	10	—	—	—	［80］
	介孔B _x CN	350	6.7	—	89.4	—	—	—	0.05	［79］
	h-BN/堇青石	535	17	—	82.1	14.2	3.7	—	18.6	［38］
B₂O₃基催化剂	B₂O₃@BPO₄-800	550	24.7	—	66.4	18.4	5.2	0.2	0.8	［64］
	B₂O₃/SBA-15	450	14.8	—	73.3	14.1	10.8	1.8	1.0	［60］
	B₂O₃/Al₂O₃	550	24.1	—	42.6	12.5	22.1	22.5	0.4	［56］
	B₂O_3-OCNTs	400	4.6	—	70	—	—	—	0.003	［6］
	B-CNTs	400	0.6	—	83	—	—	—	0.16	［6］
	B-AnnealedND	450	1.8	—	65	2	12	9	0.01	［31］
	B-mww	530	15	—	80.4	11.2	—	—	0.52	［68］
	BS-1	560	41.4	—	54.9	26.3	—	—	—	［69］
	BPO₄（OM）	515	14.3	—	8.25	9	7.9	0.6	16	［68］
其他B基催化剂	B₄C	500	7	—	84.2	9.3	3.4	0.7	0.6	［75］
	SiB₆	535	19.2	—	82.2	12.2	5.2	—	1.49	［32］
	B	490	16.4	—	77.9	10	6.6	3.6	11	［65］
	Ti₂B	500	5.8	—	85.4	9.1	2.1	0.4	0.5	［75］
	NiB	500	6.1	—	85.4	9.3	2.2	0.3	0.4	［75］
	CO₂B/CO₃B	500	3.2	—	87.9	7.9	1.5	0.2	0.2	［75］
	HfB₂	500	4.2	—	87.5	7.6	2	0.2	0.2	［75］
	WB	500	2.5	—	87.9	7.3	1.7	0.5	0.1	［75］

分类	催化剂	温度/℃	转化率/%	选择性/%					产率/g_olefin·g_cat^-1·h^-1	参考文献
分类	催化剂	温度/℃	转化率/%	C₄⁼	C₃⁼	C₂⁼	CO	CO₂	产率/g_olefin·g_cat^-1·h^-1	参考文献
BN基催化剂	h-BN	490	14	—	79	12	9	—	0.5	［14］
	BNNTs	490	16.5	—	72	—	—	—	3.7	［14］
	高比表面积BN	525	24	—	69	—	—	—	0.04	［32］
	羟化BN	530	20.6	—	80.6	10.7	7.9	0.5	7.74	［51］
	SS-BNNSs	490	20	—	78	10	—	—	—	［80］
	介孔B _x CN	350	6.7	—	89.4	—	—	—	0.05	［79］
	h-BN/堇青石	535	17	—	82.1	14.2	3.7	—	18.6	［38］
B₂O₃基催化剂	B₂O₃@BPO₄-800	550	24.7	—	66.4	18.4	5.2	0.2	0.8	［64］
	B₂O₃/SBA-15	450	14.8	—	73.3	14.1	10.8	1.8	1.0	［60］
	B₂O₃/Al₂O₃	550	24.1	—	42.6	12.5	22.1	22.5	0.4	［56］
	B₂O_3-OCNTs	400	4.6	—	70	—	—	—	0.003	［6］
	B-CNTs	400	0.6	—	83	—	—	—	0.16	［6］
	B-AnnealedND	450	1.8	—	65	2	12	9	0.01	［31］
	B-mww	530	15	—	80.4	11.2	—	—	0.52	［68］
	BS-1	560	41.4	—	54.9	26.3	—	—	—	［69］
	BPO₄（OM）	515	14.3	—	8.25	9	7.9	0.6	16	［68］
其他B基催化剂	B₄C	500	7	—	84.2	9.3	3.4	0.7	0.6	［75］
	SiB₆	535	19.2	—	82.2	12.2	5.2	—	1.49	［32］
	B	490	16.4	—	77.9	10	6.6	3.6	11	［65］
	Ti₂B	500	5.8	—	85.4	9.1	2.1	0.4	0.5	［75］
	NiB	500	6.1	—	85.4	9.3	2.2	0.3	0.4	［75］
	CO₂B/CO₃B	500	3.2	—	87.9	7.9	1.5	0.2	0.2	［75］
	HfB₂	500	4.2	—	87.5	7.6	2	0.2	0.2	［75］
	WB	500	2.5	—	87.9	7.3	1.7	0.5	0.1	［75］

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