氧化锆介导界面催化在CO2加氢反应中的研究进展

doi:10.1016/S1872-2067(26)64996-0

催化学报 ›› 2026, Vol. 84: 1-24.DOI: 10.1016/S1872-2067(26)64996-0

• 综述 • 下一篇

氧化锆介导界面催化在CO₂加氢反应中的研究进展

刘芷瑶^a^,^b, 刘唐康^a^,^b(), 秦川^a^,^b, 刘国亮^a^,^b(), 郑安民^a^,^b()

^a 武汉科技大学核磁共振与分子科学交叉研究院, 湖北武汉 430081
^b 武汉科技大学化学与化工学院, 湖北省煤转化与新型碳材料耐火材料与冶金国家重点实验室, 湖北武汉 430081

收稿日期:2025-08-20 接受日期:2025-11-12 出版日期:2026-05-18 发布日期:2026-04-16
通讯作者: *电子信箱: liutk@wust.edu.cn (刘唐康),
liugl@whu.edu.cn (刘国亮),
zam@wust.edu.cn (郑安民).
基金资助:
国家重点研发计划(2023YFA1507700);国家自然科学基金(22172113);国家自然科学基金(22472126);国家自然科学基金(22402154);湖北省自然科学基金(2025AFA008);湖北省自然科学基金(2025AFA065);国家自然科学基金委员会博士后科学基金(GZC20232002);国家自然科学基金委员会博士后科学基金(GZC20232003);中国博士后科学基金(2024M752497);湖北省博士后项目(2004HBBHCXA075);湖北省教育厅研究项目(D20241104)

Zirconia-mediated interfacial catalysis for CO₂ hydrogenation

Zhiyao Liu^a^,^b, Tangkang Liu^a^,^b(), Chuan Qin^a^,^b, Guoliang Liu^a^,^b(), Anmin Zheng^a^,^b()

^a Interdisciplinary Institute of NMR and Molecular Sciences, Wuhan University of Science and Technology, Wuhan 430081, Hubei, China
^b Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, Hubei, China

Received:2025-08-20 Accepted:2025-11-12 Online:2026-05-18 Published:2026-04-16
Contact: *E-mail: liutk@wust.edu.cn (T. Liu),
liugl@whu.edu.cn (G. Liu),
zam@wust.edu.cn (A. Zheng).
About author:Tangkang Liu (Interdisciplinary Institute of NMR and Molecular Sciences, Wuhan University of Science and Technology) received his B.S. in chemistry from Guangxi University in 2016 and his Ph.D. in physical chemistry from Wuhan University in 2023. After that, he worked as a postdoctoral researcher at Wuhan University of Science and Technology (2023 to date). His research interests focus on the design and structure-performance relationships of heterogeneous catalytic materials for CO2 hydrogenation.
Guoliang Liu (Interdisciplinary Institute of NMR and Molecular Sciences, Wuhan University of Science and Technology) obtained his bachelor’s degree in Chemistry in 2010 and graduated as a Doctor of Science in 2015 from Wuhan University. He had a visiting period as a joint PhD program under the supervision of Prof. S. C. E. Tsang at University of Oxford (UK) in 2013‒2015. From 2017 to 2023, he joined Wuhan University as an Associate Researcher to start an independent academic career. He is now a full professor at Wuhan University of Science and Technology. His research interest focuses on heterogeneous catalysis of CO₂ utilization and biomass conversion.
Anmin Zheng (Interdisciplinary Institute of NMR and Molecular Sciences, Wuhan University of Science and Technology) holds the position of Professor at the Interdisciplinary Institute of NMR and Molecular Sciences (NMR-X) and Dean of the School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology. Following his PhD (2005, Wuhan Institute of Physics and Mathematics, CAS), he was appointed Full Professor in 2012. His group is dedicated to understanding the mechanisms of heterogeneous catalysis, employing a synergistic approach that bridges advanced spectroscopic experiments and multiscale theoretical modeling.
First author contact:Author contributions
Zhiyao Liu: investigation, software, data curation, formal analysis, methodology, writing - original draft. Chuan Qin: validation, formal analysis, writing review & editing. Tangkang Liu: investigation, formal analysis, methodology, writing review & editing. Guoliang Liu: conceptualization, writing - review & editing, project administration, resources, supervision, validation, funding acquisition. Anmin Zheng: project administration, resources, supervision, validation, and funding acquisition.
Supported by:
National Key R&D Program of China(2023YFA1507700);National Natural Science Foundation of China(22172113);National Natural Science Foundation of China(22472126);National Natural Science Foundation of China(22402154);Hubei Provincial Natural Science Foundation of China(2025AFA008);Hubei Provincial Natural Science Foundation of China(2025AFA065);Postdoctoral Fellowship Program of CPSF(GZC20232002);Postdoctoral Fellowship Program of CPSF(GZC20232003);China Postdoctoral Science Foundation(2024M752497);Postdoctor Project of Hubei Province(2004HBBHCXA075);Research Project of Hubei Provincial Department of Education(D20241104)

摘要/Abstract

摘要：

利用源自可再生能源的绿色氢气将CO₂催化转化为高附加值化学品, 被视为降低CO₂排放和实现碳中和目标最具潜力的途径之一. 近十多年来, 各类高性能非均相催化剂被相继开发并投入应用. 其中, 含锆(Zr)催化剂因其在构建高效CO₂加氢活性界面方面的独特优势而备受关注. 目前, 多数研究已确认含Zr催化剂的性能与其结构特征密切相关, 并对不同组分在催化过程中的作用机制进行了深入探讨. 然而, 关于ZrO_x在CO₂加氢过程中所调控的界面催化本质, 以及反应物分子在活性位点/界面上的活化机制与转化路径, 仍存在诸多未解之谜. 因此, 系统揭示氧化锆介导的界面在CO₂加氢领域中的作用机制具有重要的研究意义.

本文系统综述了含锆催化剂在CO₂加氢领域的最新研究进展, 重点介绍了四类用于CO₂加氢制甲醇的含锆催化剂, 并深入剖析了其结构-性能关系、反应机理及真实活性位点的识别. 此外, 为阐明ZrO_x介导活性界面在甲醇合成中的催化作用, 进一步比较了不同类型含Zr催化体系的优势与不足, 通过揭示其内部复杂的作用机制, 凸显了ZrO_x介导的活性中心在提升甲醇合成效率中的关键作用. 针对ZrO_x诱导界面上CO₂加氢反应机制尚不明确的问题, 本文系统归纳了三种主要的反应路径: (1) 甲酸盐路径, (2)逆水煤气变换反应 + CO加氢路径, (3)氧化还原机制. 此外, 还讨论了副产物水或者表面羟基物种对甲醇合成反应活性的影响机制. 尽管在识别不同含Zr催化剂上的反应路径方面已取得重要进展, 但先进表征技术的局限性仍制约着对复杂反应网络的深入解析. 无论是反应路径的探索还是活性位点的识别, 本文旨在对氧化锆介导活性界面在CO₂加氢制甲醇过程中的具体机理进行系统剖析. 最后, 探讨了含Zr催化剂在CO₂加氢制备低碳醇和烯烃等C₂₊产物中的研究进展, 并提出了未来催化剂设计的研究范围. ZrO₂在构建C-C偶联的关键活性中心具有显著优势, 不仅能促进丰富活性界面的形成, 还可加速CO₂向高附加值C₂₊产物的高效转化. 因此, 开发高效的含Zr催化剂以优化CO₂加氢反应路径并实现高附加值化学品的定向合成, 是未来值得深入探索的研究方向, 这有待于更精准的催化剂结构表征与系统化的反应网络研究, 从而推动热催化CO₂加氢技术的进一步发展.

综上, 本文系统阐述了氧化锆介导界面催化在CO₂加氢反应中的研究进展, 并深入探讨了其催化作用机制, 为理解催化活性的本征来源、提升含Zr催化剂性能提供了重要理论支撑. 基于此, 本文为高性能CO₂加氢催化剂的可控设计与开发提供理论依据, 这对推动CO₂资源化利用与绿色化学发展也具有重要科学意义.

关键词: CO₂加氢, 氧化锆, 活性位, 反应机理, 甲醇合成

Abstract:

Catalytic CO₂ hydrogenation to high-value chemicals/fuels by using green hydrogen, stemming from renewable energy, is regarded as one of the most promising approaches to alleviate the emissions of CO₂ and to build a carbon neutral society in the future. This requires the development of advanced catalyst design strategy. Zirconia has been widely used as a good catalyst support/promoter for the CO₂ hydrogenation reactions, because of its significant advantages in high thermal stability, tunable surface acidity/basicity, oxygen vacancy-mediated activation, and strong metal-support interactions. In the past few years, there has been an increasing number of advanced Zr-containing catalysts, mainly for methanol synthesis reaction. Despite some reviews involving Zr-containing catalyst systems, there is still lacking of a specific review to comprehensively address the role of Zr-induced synergistic sites/interfaces as well as their activation mechanism in CO₂ hydrogenation to methanol. Herein, this review will systematically summarize the representative four types of Zr-containing catalysts, including metal/ZrO₂ catalysts, oxide catalysts, multi-component catalysts, and MOF-derived catalysts in recent years, and deeply explore the nature of active sites/interfaces and reaction mechanisms in multiple dimensions. In addition, we will discuss the influence of surface hydroxyl groups on Zr-containing catalysts and water on the activity of methanol synthesis. Finally, we expand the research to CO₂ hydrogenation to higher alcohols/olefins and propose future research scopes for catalyst design. This review aims to provide fundamental insights into the rational design and optimization of high-performance Zr-containing catalysts for CO₂ hydrogenation reactions.

Key words: CO₂ hydrogenation, Zirconia, Active sites, Reaction mechanisms, Methanol synthesis

刘芷瑶, 刘唐康, 秦川, 刘国亮, 郑安民. 氧化锆介导界面催化在CO₂加氢反应中的研究进展[J]. 催化学报, 2026, 84: 1-24.

Zhiyao Liu, Tangkang Liu, Chuan Qin, Guoliang Liu, Anmin Zheng. Zirconia-mediated interfacial catalysis for CO₂ hydrogenation[J]. Chinese Journal of Catalysis, 2026, 84: 1-24.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)64996-0

https://www.cjcatal.com/CN/Y2026/V84/I5/1

图/表 11

Fig. 1. Schematic representation of the key factors for boosting CO2-to-methanol hydrogenation activity and the reaction mechanism on Zr-containing catalysts discussed in this review.

Table 1 Catalytic performance of different types of Zr-containing catalysts for CO2 hydrogenation to methanol.

Catalyst	T (°C)	P (MPa)		GHSV (mL g^-1 h^-1)		H₂/CO₂		CO₂ Conversion (%)			MeOH selectivity (%)		MeOH STY (g kg^-1 h^-1)			TOF^e (h^-1)		Ref.
Metal/ZrO₂ catalyst
Cu/ZrO₂	280	3		10000		3		12.4			~30		—			—		[13]
Cu-ZrO₂	230	0.1		12000		9		~3.5			<30		—			—		[14]
Cu-1.0%	260	0.8		20^a		3		~1.5			~50		—			—		[10]
CuZr-1	260	3		15000		3		11			72.1		362			7.8		[15]
Pd-Cu/ZrO₂	260	1.5		6000		3		<5			~50		16			—		[16]
30%Cu/ZrO₂	240	3		9600		3		11.0			46.4		175			1.2		[18]
CAZ-1	180	3		1200		3		<2			100		—			1.4		[39]
ZrO₂/Cu	220	3		48000		3		<5			~70		524			1.2		[40]
Ni₅Ga₃/ZrO₂	270	3		8000		3		~9			26.9		273			3.2		[38]
InNi₃C_0.5/ZrO₂	325	6		36000		10		25.7			90.2		—			—		[17]
Oxide catalyst
ZnZrO_x	325	5		24000		3		5.2			72.2		273			—		[21]
ZnZrO_x-RA	290	5		24000		3		4.4			94		342			—		[22]
20%ZnO-ZrO₂	320	2		24000		3		6.4			78.5		413			—		[23]
ZnZr25	300	1		3600		3		8.1			71		61			—		[24]
25%Zr-ZnO	300	4		9000		4		~5			75		120			—		[25]
CP@PVA-ZnZrO_x	320	5		24000		3		8.2			85.9		576			—		[26]
In₂O₃/ZrO₂	280	3		12000		3		6.0			61.6		—			—		[41]
In₂O₃/5Li-ZrO₂	280	3		12000		3		12.1			84.6		—			—		[41]
Catalyst			T (°C)		P (MPa)		GHSV (mL g^-1 h^-1)		H₂/CO₂	CO₂ Conversion (%)		MeOH Selectivity (%)		MeOH STY (g kg^-1 h^-1)	TOF^e (h^-1)		Ref.
In₂O₃/ZrO₂(SG)			280		4		15000		3	16.2		94.4		950	—		[42]
InZr			250		0.1		6000		3	—		27		0.3 ^c	—		[43]
5%GaZnZrO_x			320		5		24000		3	8.8		~87		630	—		[74]
2CuGaZrO_x			300		3		6000		3	8.3		87		~160	—		[75]
0.5wt%CuZnZrO_x			290		4.5		10800		3	9.5		76		278	—		[76]
3%CuZnO-ZrO₂			250		5		12000		3	19.7		81.4		—	—		[77]
Cu-ZnZrO_x			300		5		24000		4	5		~90		550	—		[78]
0.8%Pd/ZnZrO_x			320		5		24000		4	~15		~60		~660	—		[79]
CP-Pd/ZnZr(0.1wt%)			320		5		30000		3	8.1		87		735	—		[73]
15wt%ZnO-3wt%Pd/ZrO₂			330		3		12000		3	12		~96		472	—		[80]
In_2.5/ZnZrO_x			300		5		24000		3	9.7		82.7		661	—		[81]
Ni-In₂O₃/ZrO₂			275		5		63000 ^b		3	—		73		490	—		[82]
1Pd-5In₂O₃/m-ZrO₂			280		5		24000		4	4		~90		620	—		[72]
Multi-component catalyst
ZrZnO_x/Cu			220		3		48000		3	8.4		70		990	3.6		[44]
Cu-Zn-Zr-(o)			250		3		6000		3	23.0		34		150	1.0		[45]
Cu-ZnZr			230		3		24000		3	2.5		86.0		177	1.4		[46]
30Cu-ZZ_66/34			280		5		25000 ^b		4	19.6		50		725	4.8		[47]
Cu_0.3Ce_0.3Zr_0.7			240		3		30000		3	4.1		55.2		192	2.0		[48]
CuCeZr			240		3		20000		3	6.5		64.8		271	—		[49]
CCZ-450			280		3		10000		3	13.2		71.8		325	0.5		[50]
Cu/MgOZrO₂			250		3		30000		3	—		76.7		8768	250		[56]
Cu/42Zr-SiO₂			210		3		4000		3	3.6		86.1		42	—		[12]
Cu-GaZrO_x-24			260		3.5		48000		4	7		60		630	—		[27]
CuZrIn5			225		3.3		9000		3	6.6		69.5		422	—		[28]
In-Co-Zr			310		5		10280		4	17.4		77.4		362	—		[29]
Cu₃MnZn_0.5Z_0.5			260		5		4000 ^b		3	7.1		69.7		70 ^d	—		[30]
Cu/ZnO/ZrO₂/MgO (CZZ1_0.8M_0.2)			220		3		18000		3	7.3		71.8		305	—		[31]
Zn/Cu/Zn/Zr			500		3		7500 ^b		3	3.1		79		64	—		[32]
Cu-ZnO-ZrO₂			200		3		3 ^b		3	18.2		80.2		297	35.3		[84]
Zr-MOF-derived catalyst
Cu@PCN222			250		3		31200 ^b		3	7.7		54.8		437	—		[33]
CZ-0.5-400			280		4.5		21600		3	11.1		68.4		588	13.4		[51]
12%Cu-ZrO₂-1-3			220		3		15000		3	~7		~80		288	16.2		[34]
CM-300			220		3		15600		3	5.0		85		144	8.1		[53]
Cu/ZrO₂-DM			200		2		4000		3	13.95		90.80		724	—		[54]
CU-0.5-300			260		4.5		21600		3	13.1		78.8		796	12.7		[35]
MOF-808-Zn-4			250		4		4500 ^b		3	2.1		>99%		182.9	—		[52]
ZnO/Zr₁₂-bpdc			250		4		4800 ^b		3	7.5		>95		110	—		[36]
In₂O₃@ZrO₂			290		3		12000		3	10.4		84.6		290	—		[37]
Cu/ZnO_x/ZrO₂			260		4		12000 ^b		3	17.8		52		217	0.9		[55]

Table 1 Catalytic performance of different types of Zr-containing catalysts for CO2 hydrogenation to methanol.

Catalyst	T (°C)	P (MPa)		GHSV (mL g^-1 h^-1)		H₂/CO₂		CO₂ Conversion (%)			MeOH selectivity (%)		MeOH STY (g kg^-1 h^-1)			TOF^e (h^-1)		Ref.
Metal/ZrO₂ catalyst
Cu/ZrO₂	280	3		10000		3		12.4			~30		—			—		[13]
Cu-ZrO₂	230	0.1		12000		9		~3.5			<30		—			—		[14]
Cu-1.0%	260	0.8		20^a		3		~1.5			~50		—			—		[10]
CuZr-1	260	3		15000		3		11			72.1		362			7.8		[15]
Pd-Cu/ZrO₂	260	1.5		6000		3		<5			~50		16			—		[16]
30%Cu/ZrO₂	240	3		9600		3		11.0			46.4		175			1.2		[18]
CAZ-1	180	3		1200		3		<2			100		—			1.4		[39]
ZrO₂/Cu	220	3		48000		3		<5			~70		524			1.2		[40]
Ni₅Ga₃/ZrO₂	270	3		8000		3		~9			26.9		273			3.2		[38]
InNi₃C_0.5/ZrO₂	325	6		36000		10		25.7			90.2		—			—		[17]
Oxide catalyst
ZnZrO_x	325	5		24000		3		5.2			72.2		273			—		[21]
ZnZrO_x-RA	290	5		24000		3		4.4			94		342			—		[22]
20%ZnO-ZrO₂	320	2		24000		3		6.4			78.5		413			—		[23]
ZnZr25	300	1		3600		3		8.1			71		61			—		[24]
25%Zr-ZnO	300	4		9000		4		~5			75		120			—		[25]
CP@PVA-ZnZrO_x	320	5		24000		3		8.2			85.9		576			—		[26]
In₂O₃/ZrO₂	280	3		12000		3		6.0			61.6		—			—		[41]
In₂O₃/5Li-ZrO₂	280	3		12000		3		12.1			84.6		—			—		[41]
Catalyst			T (°C)		P (MPa)		GHSV (mL g^-1 h^-1)		H₂/CO₂	CO₂ Conversion (%)		MeOH Selectivity (%)		MeOH STY (g kg^-1 h^-1)	TOF^e (h^-1)		Ref.
In₂O₃/ZrO₂(SG)			280		4		15000		3	16.2		94.4		950	—		[42]
InZr			250		0.1		6000		3	—		27		0.3 ^c	—		[43]
5%GaZnZrO_x			320		5		24000		3	8.8		~87		630	—		[74]
2CuGaZrO_x			300		3		6000		3	8.3		87		~160	—		[75]
0.5wt%CuZnZrO_x			290		4.5		10800		3	9.5		76		278	—		[76]
3%CuZnO-ZrO₂			250		5		12000		3	19.7		81.4		—	—		[77]
Cu-ZnZrO_x			300		5		24000		4	5		~90		550	—		[78]
0.8%Pd/ZnZrO_x			320		5		24000		4	~15		~60		~660	—		[79]
CP-Pd/ZnZr(0.1wt%)			320		5		30000		3	8.1		87		735	—		[73]
15wt%ZnO-3wt%Pd/ZrO₂			330		3		12000		3	12		~96		472	—		[80]
In_2.5/ZnZrO_x			300		5		24000		3	9.7		82.7		661	—		[81]
Ni-In₂O₃/ZrO₂			275		5		63000 ^b		3	—		73		490	—		[82]
1Pd-5In₂O₃/m-ZrO₂			280		5		24000		4	4		~90		620	—		[72]
Multi-component catalyst
ZrZnO_x/Cu			220		3		48000		3	8.4		70		990	3.6		[44]
Cu-Zn-Zr-(o)			250		3		6000		3	23.0		34		150	1.0		[45]
Cu-ZnZr			230		3		24000		3	2.5		86.0		177	1.4		[46]
30Cu-ZZ_66/34			280		5		25000 ^b		4	19.6		50		725	4.8		[47]
Cu_0.3Ce_0.3Zr_0.7			240		3		30000		3	4.1		55.2		192	2.0		[48]
CuCeZr			240		3		20000		3	6.5		64.8		271	—		[49]
CCZ-450			280		3		10000		3	13.2		71.8		325	0.5		[50]
Cu/MgOZrO₂			250		3		30000		3	—		76.7		8768	250		[56]
Cu/42Zr-SiO₂			210		3		4000		3	3.6		86.1		42	—		[12]
Cu-GaZrO_x-24			260		3.5		48000		4	7		60		630	—		[27]
CuZrIn5			225		3.3		9000		3	6.6		69.5		422	—		[28]
In-Co-Zr			310		5		10280		4	17.4		77.4		362	—		[29]
Cu₃MnZn_0.5Z_0.5			260		5		4000 ^b		3	7.1		69.7		70 ^d	—		[30]
Cu/ZnO/ZrO₂/MgO (CZZ1_0.8M_0.2)			220		3		18000		3	7.3		71.8		305	—		[31]
Zn/Cu/Zn/Zr			500		3		7500 ^b		3	3.1		79		64	—		[32]
Cu-ZnO-ZrO₂			200		3		3 ^b		3	18.2		80.2		297	35.3		[84]
Zr-MOF-derived catalyst
Cu@PCN222			250		3		31200 ^b		3	7.7		54.8		437	—		[33]
CZ-0.5-400			280		4.5		21600		3	11.1		68.4		588	13.4		[51]
12%Cu-ZrO₂-1-3			220		3		15000		3	~7		~80		288	16.2		[34]
CM-300			220		3		15600		3	5.0		85		144	8.1		[53]
Cu/ZrO₂-DM			200		2		4000		3	13.95		90.80		724	—		[54]
CU-0.5-300			260		4.5		21600		3	13.1		78.8		796	12.7		[35]
MOF-808-Zn-4			250		4		4500 ^b		3	2.1		>99%		182.9	—		[52]
ZnO/Zr₁₂-bpdc			250		4		4800 ^b		3	7.5		>95		110	—		[36]
In₂O₃@ZrO₂			290		3		12000		3	10.4		84.6		290	—		[37]
Cu/ZnO_x/ZrO₂			260		4		12000 ^b		3	17.8		52		217	0.9		[55]

Fig. 2. (A) The CO2 hydrogenation activity of Cu-based catalysts with various Cu loadings at 453 K. (B) The proposed Cu1-O3 configuration. (C) The wavelet transform spectroscopy of CAZ-1. Reprinted with permission from Ref. [39]. Copyright 2022, Springer Nature. (D) The methanol synthesis activity of ZrO2/Cu catalysts with varying ZrO2 contents. (E) Theoretical Zr12O23/Cu147 model presenting the inverse ZrO2/Cu-0.1 catalyst. (F) HAADF-STEM images. Reprinted with permission from Ref. [40]. Copyright 2020, Springer Nature. (G) CO2 hydrogenation activity of as-prepared Cu/MgOZrO2 catalysts. Reprinted with permission from Ref. [56]. Copyright 2024, Springer Nature. (H) Methanol selectivity and intrinsic activity measured at 210 °C as a function of ZrO2 contents, the inset showing the atomic dispersion of ZrOx species in the Cu/5Zr-SiO2 catalysts. Reprinted with permission from Ref. [12]. Copyright 2023, John Wiley and Sons.

Fig. 3. (A) Catalytic performance of different oxide catalysts. (B) In-situ DRIFTS spectra taken on different oxides under 0.1 MPa CO2 at 320 °C. Reprinted with permission from Ref. [20]. Copyright 2023, American Chemical Society. (C) Methanol yield in CO2 hydrogenation over different catalysts at various temperatures. (D) DFT simulations of charge transfer in the In2O3 stripe/m-ZrO2 and In2O3 stripe/t-ZrO2 catalyst models. In: light brown, Zr: mint green, O atoms in ZrO2: red, and O atoms in In4O6: blue. The black numbers in the image are the total number of valence electrons on In atoms. Reprinted with permission from Ref. [41]. Copyright 2020, American Chemical Society. (E) CH3OH synthesis activity (conversion, selectivity, and yield) in CO2 hydrogenation over a series of CuZnZr catalysts with varied Cu loading. (F) Schematics of hydrogen spillover effect boosting methanol production at Cu-ZnZrOx interfaces. Reprinted with permission from Ref. [76]. Copyright 2021, Elsevier.

Fig. 4. (A) Methanol selectivity and STY in CO2 hydrogenation over different Cu-Zn-Zr ternary catalysts. (B) DFT calculations of H2 dissociation at different models. Models 1 and 2 represent the interface between Cu and atomically dispersed Zn on ZrO2 support in the Cu-ZnZr sample and the Cu-ZnO interface in the Zr-CuZn sample, respectively. Reprinted with permission from Ref. [46]. Copyright 2023, John Wiley and Sons. (C) STY of methanol in CO2 hydrogenation over various inverse catalysts. ‘*’ refers to physical mixing. (D) EPR spectra of CuO, ZrO2, ZnO, ZnO/Cu, ZrO2/Cu, and ZrZnOx/Cu catalysts. Reprinted with permission from Ref. [44]. Copyright 2024, Elsevier.

Fig. 5. (A) TEM image and structure schematic of UiO-67-Pt. Reprinted with permission from Ref. [96]. Copyright 2020, American Chemical Society. (B) Scheme showing the synthesis of MOF-808-Zn and the active site of Zr4+-O-Zn2+. Reprinted with permission from Ref. [52]. Copyright 2021, American Chemical Society. (C) The CO2 hydrogenation activity over various catalysts. Reprinted with permission from Ref. [54]. Copyright 2024, Elsevier. (D) Illustration for Cu species deposition using defective nodes. Reprinted with permission from Ref. [90]. Copyright 2020, Springer Nature. (E) Schematic illustration for the synthesis of Cu/ZnOx/ZrO2 catalyst from MOF precursor. Reprinted with permission from Ref. [55]. Copyright 2022, Elsevier.

Fig. 6. Reaction pathway of CO2 hydrogenation to methanol.

Fig. 7. In-situ DRIFTS spectra of Cu-ZnZr catalysts during CO2 hydrogenation reaction (A), followed by He sweep after reaction (B), and the dynamic evolution (C) of normalized peak area of formate HCOO* (2878 cm-1, orange) and methoxy OCH3* (2936 cm-1, green). Reprinted with permission from Ref. [46]. Copyright 2023, John Wiley and Sons. (D) In-situ DRIFTS spectra of Cu/10Zr-SiO2, (E) The relative energy of transition states (TS) on Model 1 (Cu/Zr1-Si) and Model 2 (Cu/ZrO2-Si) during the hydrogenation process to intermediates HCOO* and HOCO*, which follow formate and RWGS + CO-hydro pathways, respectively. Cu: orange, Zr: green; Si: blue, O: red, C: black, and H: gray. Reprinted with permission from Ref. [12]. Copyright 2023, John Wiley and Sons. (F) Proposed mechanism of CO2 hydrogenation over Ni5Ga3 alloy catalyst supported on ZrO2. Reprinted with permission from Ref. [38]. Copyright 2022, Elsevier.

Fig. 8. (A) Specific initial reaction rates of formate decomposition for the three surface species observed and the rate of methanol formation at steady-state at 220 °C and 3 bar under 20% CO + 60% H2 in He. Reprinted with permission from Ref. [104]. Copyright 2023, John Wiley and Sons. (B) The scheme illustrates the different reaction behaviors of the HCOO-Cu and HCOO-Zr intermediates on inverse ZrO2/Cu and Cu/ZrO2 catalysts. Reprinted with permission from Ref. [40]. Copyright 2020, Springer Nature. (C) The proposed interface sites for methanol synthesis on Cu-Zn-Zr ternary catalysts produced by the DFSP method. Reprinted with permission from Ref. [46]. Copyright 2023, John Wiley and Sons. (D) The adsorption modes of active species at various surface/interface models. Reprinted with permission from Ref. [72]. Copyright 2023, John Wiley and Sons.

Fig. 9. (A) An outline of potential reaction pathways to methanol from adsorbed carbon dioxide. Reprinted with permission from Ref. [14]. Copyright 2024, Elsevier. (B) XPS of Zn 2p for ZnZrOx-RA and ZnZrOx-CP catalysts. Reprinted with permission from Ref. [22]. Copyright 2023, Elsevier. (C) The comparison of intermediate species of CO2 adsorption and hydrogenation on Cu/CeO2 and Cu/ZrO2. Reprinted with permission from Ref. [13]. Copyright 2020, Elsevier. (D) Possible reaction paths of CO2 hydrogenation to methanol over CZZ catalysts. Reprinted with permission from Ref. [120]. Copyright 2020, Elsevier.

Fig. 10. (A) Proposed mechanism of methanol and ethanol synthesis from CO2 hydrogenation over Zr12-bpdC-Cu catalysts. Reprinted with permission from Ref. [126]. Copyright 2019, Springer Nature. (B) Role of the K-ZrO2 interfaces in CO2 hydrogenation over KFeCu/a-ZrO2. CO-DRIFTS spectra (left) and the corresponding higher alcohol synthesis activity (right). (C) The illustration for the contribution of K-ZrO2 interfaces to CO insertion process. Reprinted with permission from Ref. [124]. Copyright 2023, American Chemical Society. (D) Catalytic CO2 hydrogenation to C2+ products over various Fe catalysts with different supports. Reprinted with permission from Ref. [136]. Copyright 2022, Elsevier. (E) Light olefin selectivity versus CO2 conversion for various FeM/ZrO2 catalysts. Reprinted with permission from Ref. [139]. Copyright 2022, American Chemical Society.

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氧化锆介导界面催化在CO₂加氢反应中的研究进展

Zirconia-mediated interfacial catalysis for CO₂ hydrogenation

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