金属氧化物半导体用于光热催化CO2加氢反应：最新进展和展望

doi:10.3866/PKU.WHXB202212042

物理化学学报 >> 2023, Vol. 39 >> Issue (11): 2212042.doi: 10.3866/PKU.WHXB202212042

所属专题：多物理场能源催化转化

金属氧化物半导体用于光热催化CO₂加氢反应：最新进展和展望

万宇彤, 方帆(), 孙瑞雪, 张杰, 常焜()

南京航空航天大学材料科学与技术学院, 南京 210016

收稿日期:2022-12-27 录用日期:2023-02-16 发布日期:2023-03-02
通讯作者: 方帆,常焜 E-mail:fangfan1990@nuaa.edu.cn;changkun@nuaa.edu.cn
基金资助:
国家自然科学基金(51888103);江苏省自然科学基金(BK20210308);中国博士后科学基金(2021M701695);中央高校基本科研业务费专项资金(NE2019103);江苏省研究生科研实践创新计划(SJCX21_0097)

Metal Oxide Semiconductors for Photothermal Catalytic CO₂ Hydrogenation Reactions: Recent Progress and Perspectives

Yutong Wan, Fan Fang(), Ruixue Sun, Jie Zhang, Kun Chang()

College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China

Received:2022-12-27 Accepted:2023-02-16 Published:2023-03-02
Contact: Fan Fang, Kun Chang E-mail:fangfan1990@nuaa.edu.cn;changkun@nuaa.edu.cn
Supported by:
the National Natural Science Foundation of China(51888103);the Natural Science Foundation of Jiangsu Province, China(BK20210308);the Postdoctoral Science Foundation of China(2021M701695);the Fundamental Research Funds for the Central Universities, China(NE2019103);the Postgraduate Research & Practice Innovation Program of Jiangsu Province, China(SJCX21_0097)

摘要/Abstract

摘要：

由于人类经济社会的快速发展，大气中二氧化碳的浓度逐年增加造成了严重的生态环境问题。为了应对气候变化带来的挑战，中国作出了“到2030年达到碳排放峰值，到2060年实现碳中和”的重大承诺。理想情况下，将二氧化碳转化为增值产品或太阳能燃料(如CH₄、CO)是一种两全其美的策略，可以同时缓解温室效应和解决能源供需不足的问题。在为上述策略提出的设想中，利用可再生的绿H₂生产化学品来减少CO₂的方案是首选，它除了实现CO₂减排，还可以激发清洁能源的潜力。为了研究这一还原过程，人们设计了许多催化反应，其中光催化是最理想的方案，因为太阳能是清洁和可持续的。在光催化中，光热催化二氧化碳加氢技术因其较高的催化效率和太阳能的广泛利用而成为一种很有前途的CO₂转化方案。对光热催化加氢原理目前主要有两种解释：(1)仅以太阳光为能量源，驱动催化剂自身产热从而实现二氧化碳的转化。在这种情况下，反应仍以热催化方式进行。(2)光能与热能相互耦合协同催化反应的发生。因此，根据催化方式的不同，光热催化剂的合理设计和成功合成非常重要。值得关注的是，金属氧化物半导体由于其独特的能带结构和化学性质，高稳定性，环境友好等优点，被广泛应用于光热催化加氢反应的研究。在本文中，我们主要从负载催化剂、微观结构工程、缺陷工程三种不同的催化剂调控策略综述了金属氧化物材料用于光热催化CO₂加氢反应的研究进展，特别是近五年的重要研究成果。同时，对这些调制策略的机理进行了总结和介绍，以供进一步理解。本文还介绍了不同类型的光热加氢反应器，以及一些重要参数对催化反应的影响。最后，对金属氧化物催化剂的设计策略提出建议，并对光热减排技术的发展提出展望。

关键词: CO₂还原, 催化加氢, 光热协同, 金属氧化物, 调控策略

Abstract:

Owing to the accelerated growth of the human economy and society, the increasing concentration of CO₂ in the atmosphere has caused serious ecological and environmental problems because of the greenhouse effect. In response to the challenges posed by climate change, China has made a significant commitment to "peak carbon emissions by 2030 and achieve carbon neutrality by 2060". Ideally, converting CO₂ into carbon-based energy and chemicals is supposed to be the best strategy of both worlds, mitigating the greenhouse effect while also addressing the shortage of energy supply. Among the proposed concepts for the above strategy, the scheme of reducing CO₂ using renewable green H₂ to produce chemicals is preferred, because it can stimulate the potential of clean energy while also reducing CO₂ emission. To accelerate this reduction process, many catalytic reactions, including photocatalysis, have been designed and investigated. Owing to its high catalytic efficiency and extensive use of solar energy, photothermal catalytic CO₂ hydrogenation in photocatalysis is desirable for increasing sun-to-fuel efficiency. There are two main interpretations of photothermal catalytic hydrogenation: (1) only sunlight is used as the energy source to drive the catalyst, which generates heat to promote CO₂ conversion. In this case, the reaction still proceeds in the form of thermocatalysis, whereas photocatalysis has a limited effect. (2) Solar and heat energy are coupled to participate in the catalytic reaction, which has a synergistic effect. Therefore, according to the catalytic mode, the rational design and successful synthesis of photothermal catalysts are very important. Metal oxide semiconductors, owing to their unique energy band structure and chemical properties, high stability, and environmental friendliness, are widely used in the research of photothermal catalytic hydrogenation reactions. This paper reviews the research progress on metal oxide materials used in the CO₂ hydrogenation reaction by photothermal catalysis. In particular, the most significant results of research in the last five years have been performed mainly from three different catalyst modulation strategies, such as supporting catalysts, applying microstructure engineering, and defect engineering. The mechanisms of these modulation strategies are summarized and presented for further understanding. In addition, this study introduces different types of photothermal hydrogenation reactors, accompanied by the effects of some key parameters on the reactions. Finally, design strategies for metal oxide catalysts are suggested, and an outlook of photothermal abatement technology is presented.

Key words: CO₂ reduction, Catalytic hydrogenation, Photothermal synergy, Metal oxide, Modulation strategy

万宇彤, 方帆, 孙瑞雪, 张杰, 常焜. 金属氧化物半导体用于光热催化CO₂加氢反应：最新进展和展望[J]. 物理化学学报, 2023, 39(11), 2212042. doi: 10.3866/PKU.WHXB202212042

Yutong Wan, Fan Fang, Ruixue Sun, Jie Zhang, Kun Chang. Metal Oxide Semiconductors for Photothermal Catalytic CO₂ Hydrogenation Reactions: Recent Progress and Perspectives[J]. Acta Phys. -Chim. Sin. 2023, 39(11), 2212042. doi: 10.3866/PKU.WHXB202212042

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202212042

https://www.whxb.pku.edu.cn/CN/Y2023/V39/I11/2212042

图/表 18

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Table 2

Reported metal oxide semiconductors for photothermal catalytic CO2 hydrogenation."

Type	Photothermal catalysts and materials	Reaction conditions	Catalytic performance	Ref.
Supported catalysts	Ru/Al₂O₃	300 W Xe lamp	CH₄: 18.16 mol∙h⁻¹∙g⁻¹	27
	Rod-shaped Ru/Al₂O₃	1 sunsolar intensity, 250 ℃	CH₄: 135 mmol∙g_Ru⁻¹	61
	Ru/TiO₂	1 sun solar intensity, 150 ℃	CH₄: 1.72 mmol∙g_cat⁻¹∙h⁻¹	62
	Small Pd/Nb₂O₅ nanorods	300 W Xe lamp (4.2 W∙cm⁻²)	CO: 18.8 mol∙h⁻¹∙g_Pd⁻¹	28
	Pd/ZnO	Two high-pressure mercury lamps, 12 bar	CH₃OH: 4.0 mmol∙g⁻¹∙h⁻¹ CO: 8.3 mmol∙g⁻¹∙h⁻¹	67
	Au/TiO₂	Green light irradiation, 200 ℃	CO: 0.70 μmol∙g_cat⁻¹∙ s⁻¹	70
	Ni/Al₂O₃	300 W Xe lamp	CH₄: 2.30 mol∙h⁻¹∙g⁻¹	27
	Ni-Al₂O₃/SiO₂	LED lamp	CH₄: 35 mmol g⁻¹ h⁻¹	71
	Cu/ZnO	Visible light, 1 bar	CH₃OH: 2.13 μmol∙g⁻¹∙min⁻¹	75
	(Cu⁺, Pd)/H_yWO_3−x	2 W∙cm² illumination	CO: 0.073 mmol∙g⁻¹∙h⁻¹	82
	CoFeAl layered-double-hydroxide (LDH)	UV-Vis irradiation	C₂₊: 36.3%	29
	Co₇Cu₁Mn₁O_x	300 W Xe lamp, 200 ℃ +	C₂₊: 7.5 mmol∙g⁻¹∙h⁻¹	83
Micro-structure modulation	Ru/SiNW	Xe lamp with 3.2 suns intensity	CH₄: 0.99 mmol∙g⁻¹∙h⁻¹	85
	Nanostructured RuO₂ on Si Photonic Crystal	High-intensity solar simulated irradiation	CH₄: 4.4 mmol∙g_cat⁻¹∙h⁻¹	88
	In₂O_3−x(OH)_y/SiNW	300 W Xe lamp, 150 ℃	CO: 22.0 μmol∙g_cat⁻¹∙h⁻¹	86
	Core-shell structured Ni₁₂P₅@SiO₂	300 W Xe lamp	100% CO: 135mmol∙g⁻¹∙h⁻¹	89
	Core-satellite structured Co@SiO₂	300 W Xe lamp (1.7 W∙cm⁻²)	CO: 80 mmol∙g_Co⁻¹∙h⁻¹	90
	Nanoporous-silica-encapsulated nickel nanocrystal (Ni@p-SiO₂)	300 W Xe lamp (2.8 W∙cm⁻²)	CO: 0.344 mol∙g_Ni⁻¹ min⁻¹	31
	Rod-like nanocrystal superstructure In₂O_3−x(OH)_y	130 W Xe lamp, 1 bar	50%CH₃OH: 0.06mmol∙g⁻¹∙h⁻¹	91
	ZIF-67 derived Co/Al₂O₃	PLS-SXE300UV, PerfectLight	97.7%CH4: 6036 μmol∙g⁻¹ ∙h⁻¹	94
	Metal-organic framework-derived Ga-Cu/CeO₂	300 W Xe lamp	100%CO: 112 mmol∙g⁻¹∙h⁻¹	95
	MIL-125(Ti)-derived defective Ni/TiO₂	Infrared (IR) light	100%CH₄: 271.9 mmol∙g _Ni⁻¹∙h⁻¹	32
Defect modulation	In₂O_3−x/In₂O₃	Light intensity = ~20 suns	100%CO: 1874.62 μmol∙m⁻²∙h⁻¹	58
	2D Black In₂O_3−x nanosheets	300 W Xe lamp	100% CO: 103.21 mmol∙g⁻¹∙h⁻¹	30
	H_zIn₂O_3−x(OH)_y	Light intensity of 6 suns, 1 bar	CH₃OH : 33.24%−49.23%	22
	Ru/H_xMoO_3−y	Vis-NIR light irradiation, 140 ℃	CH₄: 20.8 mmol∙g⁻¹∙h⁻¹	98
	Bi₂O_3−x	Infrared (IR) light	100%CO: 4.6 μmol∙g⁻¹∙h⁻¹	101

Table 2

Fig 16

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Equation	Reaction	∆G_{298 K}^Ө/(kJ∙mol⁻¹)	∆H_{298 K}^Ө/(kJ∙mol⁻¹)
1	CO₂(g) + H₂(g) ↔ CO(g) + H₂O(g)	28.6	41.2
2	CO₂(g) + 3H₂(g) ↔ CH₃OH(g) + H₂O(g)	3.5	−49.1
3	CO₂(g) + 4H₂(g) ↔ CH₄(g) + 2H₂O(g)	−113.6	165
4	CO₂(g) + xH₂(g) ↔ C₂H_x(g) + xH₂O(g)	–	–

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金属氧化物半导体用于光热催化CO₂加氢反应：最新进展和展望

Metal Oxide Semiconductors for Photothermal Catalytic CO₂ Hydrogenation Reactions: Recent Progress and Perspectives

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