电流响应催化剂及其强化典型反应的研究进展

doi:10.16085/j.issn.1000-6613.2023-1472

化工进展 ›› 2024, Vol. 43 ›› Issue (1): 49-59.DOI: 10.16085/j.issn.1000-6613.2023-1472

电流响应催化剂及其强化典型反应的研究进展

王棵旭¹^,²(), 张香平²^,³, 王红岩², 柏䶮¹(), 王慧²^,³()

^1.河南大学化学与分子科学学院，河南开封 475000
^2.离子液体清洁过程北京市重点实验室，中国科学院过程工程研究所，中国科学院绿色过程制造创新研究院，北京 100190
^3.惠州市绿色能源与新材料研究院，广东惠州 516081

收稿日期:2023-08-22 修回日期:2023-11-24 出版日期:2024-01-20 发布日期:2024-02-05
通讯作者: 柏?,王慧
作者简介:王棵旭（1997—），男，博士研究生，研究方向为电流响应催化剂的设计及催化裂解性能。E-mail：wangkexu@ipe.ac.cn。
基金资助:
国家自然科学基金委重大项目(22393953);优秀青年科学基金(22322813)

Progress on current-responsive catalysts and their applications in intensifying typical reactions

WANG Kexu¹^,²(), ZHANG Xiangping²^,³, WANG Hongyan², BAI Yan¹(), WANG Hui²^,³()

^1.College of Chemistry and Molecular Science, Henan University, Kaifeng 475000, Henan, China
^2.Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Innovation Academy for Green Manufacture, Chinese Academy of Sciences, Beijing 100190, China
^3.Huizhou Institute of Green Energy and Advanced Materials, Huizhou 516081, Guangdong, China

Received:2023-08-22 Revised:2023-11-24 Online:2024-01-20 Published:2024-02-05
Contact: BAI Yan, WANG Hui

摘要/Abstract

摘要：

电流响应催化剂是一类可在电场诱导作用下产生电流的新型催化材料，以其为介质的催化反应过程可突破热力学局限，在温和条件下即可发生，具有显著节能减碳潜力。本文综述了近年来电流响应催化剂强化合成氨、甲烷高值利用、丙烷脱氢三个典型反应的研究进展，总结了所开发系列电流响应催化剂，其中以负载型金属催化剂为主，其由载体（半导体型或钙钛矿型金属氧化物）和活性金属（单一金属或合金）组成，对比了不同催化剂的催化性能，分析了“质子跳跃”在强化上述反应过程的作用。最后，分析了电流强化技术未来发展方向及面临挑战，提出开发适于电流作用下的原位表征技术及分子模拟方法，这对从微观层面深入揭示反应机理具有重要意义，可反向指导催化剂设计，推动相关领域发展，助力化工行业低碳转型。

关键词: 电流响应, 催化剂, 载体, 质子跳跃机制, 热力学

Abstract:

Current-responsive catalysts are a novel type of catalytic materials that can generate electric current under the induced effect of electric field, and the reactions catalyzed by this kind of catalysts can break through the thermodynamic limitation and occur under mild conditions, with significant energy-saving and carbon-reducing potentials. In this article, we reviewed the research progress of current-responsive catalysts intensifying ammonia synthesis, high-value utilization of methane and propane dehydrogenation in recent years. Series of current-responsive catalysts were summarized, which were mainly loaded metal catalysts, consisting of the carrier (semiconductor-type or perovskite-type metal oxides) and active metals (single metal or alloys). The catalytic performance of various catalysts was compared, and the role of “proton hopping” in intensifying corresponding reactions was analyzed. Finally, the future development directions and challenges of current-enhanced technology were prospected. It was proposed that the development of in-situ characterization technology and molecular simulation methods is of great significance for revealing the reaction mechanism from the microscopic level, which can provide guidance for the design of more efficient catalysts, promote the development of related fields, and assist the low-carbon upgrading of the chemical industry.

Key words: current-responsive, catalyst, support, proton hopping mechanism, thermodynamics

中图分类号:

TM924

王棵旭, 张香平, 王红岩, 柏䶮, 王慧. 电流响应催化剂及其强化典型反应的研究进展[J]. 化工进展, 2024, 43(1): 49-59.

WANG Kexu, ZHANG Xiangping, WANG Hongyan, BAI Yan, WANG Hui. Progress on current-responsive catalysts and their applications in intensifying typical reactions[J]. Chemical Industry and Engineering Progress, 2024, 43(1): 49-59.

图/表 8

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催化剂	制备方法	电场参数			压力 /MPa	温度 /K	原料组成 /sccm	氨生成速率 /μmol·g^-1·h^-1	文献
催化剂	制备方法	电流 /mA	电压 /kV	功率 /W	压力 /MPa	温度 /K	原料组成 /sccm	氨生成速率 /μmol·g^-1·h^-1	文献
Cs/Ru/SrZrO₃	柠檬酸络合-浸渍法	6	0.47	2.82	0.9	623	N₂=60 H₂=180	30099	[34-36]
Co/Ce_0.5Zr_0.5O₂	柠檬酸络合-浸渍法	6	0.19	1.14	0.1	721.7	N₂=60 H₂=180	2128.4	[37]
Fe/CeO₂	浸渍法	6	0.2	1.2	0.1	373	N₂=60 H₂=180	150	[38]
Fe/Ce_0.4Al_0.1Zr_0.5O_2-_δ	柠檬酸络合-液相还原法	6	0.41	2.46	0.1	476.2	N₂=60 H₂=180	1045.5	[39]
Ru/CeO₂	浸渍法	6	0.28	1.68	0.1	378	N₂=60 H₂=180	266.4	[40]
Ru/Sr_1-_x Ba _x ZrO₃(0≤x≤0.50)	柠檬酸络合-浸渍法	6	0.284	1.704	0.1	646.4	N₂=60 H₂=180	3937.7	[41]

催化剂	制备方法	电场参数			压力 /MPa	温度 /K	原料组成 /sccm	氨生成速率 /μmol·g^-1·h^-1	文献
催化剂	制备方法	电流 /mA	电压 /kV	功率 /W	压力 /MPa	温度 /K	原料组成 /sccm	氨生成速率 /μmol·g^-1·h^-1	文献
Cs/Ru/SrZrO₃	柠檬酸络合-浸渍法	6	0.47	2.82	0.9	623	N₂=60 H₂=180	30099	[34-36]
Co/Ce_0.5Zr_0.5O₂	柠檬酸络合-浸渍法	6	0.19	1.14	0.1	721.7	N₂=60 H₂=180	2128.4	[37]
Fe/CeO₂	浸渍法	6	0.2	1.2	0.1	373	N₂=60 H₂=180	150	[38]
Fe/Ce_0.4Al_0.1Zr_0.5O_2-_δ	柠檬酸络合-液相还原法	6	0.41	2.46	0.1	476.2	N₂=60 H₂=180	1045.5	[39]
Ru/CeO₂	浸渍法	6	0.28	1.68	0.1	378	N₂=60 H₂=180	266.4	[40]
Ru/Sr_1-_x Ba _x ZrO₃(0≤x≤0.50)	柠檬酸络合-浸渍法	6	0.284	1.704	0.1	646.4	N₂=60 H₂=180	3937.7	[41]

催化剂	制备方法	电场参数			温度/K	原料组成/sccm	转化率/%	产物生成速率 /μmol·min^-1			文献
催化剂	制备方法	电流/mA	电压/kV	功率/W	温度/K	原料组成/sccm	转化率/%	CO₂	CO	H₂	文献
Pd/CeO₂	浸渍法	3	0.44	1.32	523	CH₄/H₂O/Ar=12/24/18； GHSV: 22500h^-1	20.3	81.4	18.0	375.3	[50-53]
Ru/CeO₂			0.92	2.78			27.5	97.4	32.4	509.3	[50-51]
Pt/CeO₂			0.93	2.80			13.9	62.5	4.8	263.6	[54]
Ni/CeO₂			0.55	1.66	487		14.5	67.9	5.1	281.4	[51]
Pd/Ce_0.25Zr_0.75O₂	尿素沉积沉淀法、浸渍法	3	1.16	3.47	536		41.0	147.8	62.2	761.9	[51]
Ru/Ce_0.25Zr_0.75O₂			1.15	3.46	544		42.3	140.4	71.0	756.9	[51]
Pt/Ce_0.25Zr_0.75O₂			0.94	2.83	526		39.1	139.6	62.8	725.2	[51,54]
Ni/Ce_0.25Zr_0.75O₂			1.18	3.54	535		41.6	126.2	84.6	708.8	[51]
Pd/SrTiO₃	柠檬酸络合-浸渍法	3	0.64	1.93	466		13.1	30.1	31.4	225.0	[51]
Ru/SrTiO₃			0.77	2.32	496		22.4	88.4	23.2	431.8
Pt/SrTiO₃			0.66	1.97	457		4.9	19.1	4.3	95.9
Ni/SrTiO₃			0.89	2.67	499		2.9	12.2	0.6	49.0
Pt/CeO₂(200mg)+ ZrO₂(50mg)	行星式球磨机混合	3	0.55	1.65	475.2	CH₄/H₂O/Ar=12/24/18	14.0	62.8	2.3	243.3	[54]
Pt/CeO₂(200mg)+ Al₂O₃(50mg)	行星式球磨机混合	3	0.76	2.28	484.3		20.4	82.7	3.7	358.9
Pt/CeO₂(200mg)+ ZrO₂(50mg)	研钵研磨混合（355~500μm）	3	0.47	1.41	474.7		11.4	51.4	1.8	202.5
Pt/CeO₂(200mg)+ ZrO₂(100mg)			0.66	1.98	482.8		14.6	62.3	5.2	262.9
Pt/CeO₂ (200mg) + Al₂O₃ (50mg)			0.64	1.92	489.5		15.6	69.9	1.9	294.2
Pt/CeO₂(200mg)+ Al₂O₃(100mg)			0.70	2.10	484.0		15.1	72.0	6.5	282.5
Pt/CeO₂(200mg)+ SiO₂(50mg)			0.59	1.77	478.8		15.2	69.4	3.8	282.2
Pd_0.9Zn_0.1/Ce_0.5Zr_0.5O₂	浸渍法	3~7	—	1.5	423	CH₄/H₂O/Ar=10/20/70	19.6	TOF-p=31.9s^-1			[55]
Pd/Nb₂O₅		9	0.144	1.30	457		7.5	—	—	—	[56]
Pd/Ta₂O₅		9	0.132	1.16	454		6.1	—	—	—	[56]
Pd/Al-CeO₂	柠檬酸络合-浸渍法	3~9	—	0.8	473	CH₄/H₂O/Ar=12/24/84	—	r(CO+CO₂)= 0.042 mmol/min			[57]
Zr_0.65Y_0.05Ni_0.3O₂	柠檬酸络合法	3~9	—	1.5	473	CH₄/H₂O/Ar=12/24/84	16.3	r(CO+CO₂)=0.113mmol/min			[58]

催化剂	制备方法	电场参数			温度/K	原料组成/sccm	转化率/%	产物生成速率 /μmol·min^-1			文献
催化剂	制备方法	电流/mA	电压/kV	功率/W	温度/K	原料组成/sccm	转化率/%	CO₂	CO	H₂	文献
Pd/CeO₂	浸渍法	3	0.44	1.32	523	CH₄/H₂O/Ar=12/24/18； GHSV: 22500h^-1	20.3	81.4	18.0	375.3	[50-53]
Ru/CeO₂			0.92	2.78			27.5	97.4	32.4	509.3	[50-51]
Pt/CeO₂			0.93	2.80			13.9	62.5	4.8	263.6	[54]
Ni/CeO₂			0.55	1.66	487		14.5	67.9	5.1	281.4	[51]
Pd/Ce_0.25Zr_0.75O₂	尿素沉积沉淀法、浸渍法	3	1.16	3.47	536		41.0	147.8	62.2	761.9	[51]
Ru/Ce_0.25Zr_0.75O₂			1.15	3.46	544		42.3	140.4	71.0	756.9	[51]
Pt/Ce_0.25Zr_0.75O₂			0.94	2.83	526		39.1	139.6	62.8	725.2	[51,54]
Ni/Ce_0.25Zr_0.75O₂			1.18	3.54	535		41.6	126.2	84.6	708.8	[51]
Pd/SrTiO₃	柠檬酸络合-浸渍法	3	0.64	1.93	466		13.1	30.1	31.4	225.0	[51]
Ru/SrTiO₃			0.77	2.32	496		22.4	88.4	23.2	431.8
Pt/SrTiO₃			0.66	1.97	457		4.9	19.1	4.3	95.9
Ni/SrTiO₃			0.89	2.67	499		2.9	12.2	0.6	49.0
Pt/CeO₂(200mg)+ ZrO₂(50mg)	行星式球磨机混合	3	0.55	1.65	475.2	CH₄/H₂O/Ar=12/24/18	14.0	62.8	2.3	243.3	[54]
Pt/CeO₂(200mg)+ Al₂O₃(50mg)	行星式球磨机混合	3	0.76	2.28	484.3		20.4	82.7	3.7	358.9
Pt/CeO₂(200mg)+ ZrO₂(50mg)	研钵研磨混合（355~500μm）	3	0.47	1.41	474.7		11.4	51.4	1.8	202.5
Pt/CeO₂(200mg)+ ZrO₂(100mg)			0.66	1.98	482.8		14.6	62.3	5.2	262.9
Pt/CeO₂ (200mg) + Al₂O₃ (50mg)			0.64	1.92	489.5		15.6	69.9	1.9	294.2
Pt/CeO₂(200mg)+ Al₂O₃(100mg)			0.70	2.10	484.0		15.1	72.0	6.5	282.5
Pt/CeO₂(200mg)+ SiO₂(50mg)			0.59	1.77	478.8		15.2	69.4	3.8	282.2
Pd_0.9Zn_0.1/Ce_0.5Zr_0.5O₂	浸渍法	3~7	—	1.5	423	CH₄/H₂O/Ar=10/20/70	19.6	TOF-p=31.9s^-1			[55]
Pd/Nb₂O₅		9	0.144	1.30	457		7.5	—	—	—	[56]
Pd/Ta₂O₅		9	0.132	1.16	454		6.1	—	—	—	[56]
Pd/Al-CeO₂	柠檬酸络合-浸渍法	3~9	—	0.8	473	CH₄/H₂O/Ar=12/24/84	—	r(CO+CO₂)= 0.042 mmol/min			[57]
Zr_0.65Y_0.05Ni_0.3O₂	柠檬酸络合法	3~9	—	1.5	473	CH₄/H₂O/Ar=12/24/84	16.3	r(CO+CO₂)=0.113mmol/min			[58]

催化剂	制备方法	电场参数			温度/K	原料组成/sccm	转化率/%		产率/%			参考文献
催化剂	制备方法	电流/mA	电压/kV	功率/W	温度/K	原料组成/sccm	CH₄	CO₂	CO	H₂	H₂/CO	参考文献
Pt/CeO₂	浸渍法	20	0.14	2.81	453	CH₄/CO₂/Ar=20/20/40	15.1	16.4	—	—	0.76	[70]
Ni/La-ZrO₂	柠檬酸络合-浸渍法	3	1.23	3.7	555	CH₄/CO₂/Ar=25/25/50；W/F^①=1.6g·h/mol	22.8	24.8	22.8	—	0.83	[71-72]
Ni_0.8Fe_0.2/CeO₂	尿素沉积沉淀法	10	—	—	473	CH₄/CO₂/Ar=10/10/10	6.0	6.5	5.7	6.0	0.82	[73-74]
Ni-Fe/AC	浸渍法	9	1	9	673	CH₄∶CO₂∶N₂=1∶1∶2； GHSV：800h^-1	19.53	29.36	—	—	0.67	[75]

电流响应催化剂及其强化典型反应的研究进展

Progress on current-responsive catalysts and their applications in intensifying typical reactions

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催化剂	制备方法	电场参数			温度 /K	原料组成/sccm	转化率/%		C₂/%		参考文献
催化剂	制备方法	电流 /mA	电压 /kV	功率 /W	温度 /K	原料组成/sccm	CH₄	O₂	选择性	产率	参考文献
Gd₂O₃	—	3	0.8	2.4	423	CH₄/O₂/Ar=25/5/100； W/F=3.2g·h/mol	10.3	46.5	(C₂H₆+C₂H₄)：39.2； C₂H₂：0.8	—	[83]
Sr-La₂O₃(Sr/La=1/20)	柠檬酸络合法	3	0.9	2.7	423	CH₄/O₂/Ar=25/5/100； W/F=3.2g·h/mol	8.9	51.3	C₂H₆：33.5 C₂H₄：15.5 C₂H₂：0	—	[84-85]
La-ZrO₂		3	2	6	423	CH₄/CO₂/Ar=25/25/50 W/F=1.67g·h/mol； WHSV：18h^-1	3.2	CO₂：4.1	(C₂H₆+C₂H₄)：31.2	—	[86]
La_0.7Ca_0.3AlO_3-_δ		3	1.2	3.6	588	CH₄/O₂/Ar=25/5/70	17.4	77.5	C₂H₆：15.8 C₂H₄：13.3 C₂H₂：0.2	5.1	[87]
La_0.7Ca_0.3AlO_3-_δ		3	2.5	7.5	423	CH₄/CO₂/Ar=25/25/50	10.4	CO₂：14.2	19.6	2.0	[88]
Ce₂(WO₄)₃		3	0.7	2.1	659	CH₄/O₂/Ar=25/15/60； W/F(CH₄)：1.5g·h/mol	9.7	11.6	(C₂H₆+C₂H₄+C₂H₂)：41.2	4.0	[89]
Ce₂(WO₄)₃/CeO₂	浸渍法	3	0.8	2.5	649	CH₄/O₂/Ar=25/15/60； W/F(CH₄)：1.6g·h/mol	13.6	—	(C₂H₆+C₂H₄+C₂H₂)：39.0	—	[90]
(TBA)₃PW₁₂O₄₀/CeO₂	Copaux法-浸渍法	3	1.3	3.9	689	CH₄/O₂/Ar=25/15/60； W/F(CH₄)：1.6g·h/mol	14.9	20.6	C₂H₆：13.8 C₂H₄：18.4 C₂H₂：11.2	6.5	[90-91]
CePO₄	水热法	7	0.8	5.6	542	CH₄/O₂/Ar=15/12/33； W/F(CH₄)：2.49g·h/mol	62	66	(C₂H₆+C₂H₄+C₂H₂)：29	18	[92]
TiO₂/ZSM-5	水热法-机械化学法	8	2.4	19.2	432	CH₄/O₂/Ar=25/15/60； W/F(CH₄)：1.6g·h/mol	18.4	—	C₂H₆：8.5 C₂H₄：15.7 C₂H₂：6.5 C₃H₆：1.7	5.6	[93]

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