Ni-CeO2界面富电子Ni原子变化规律及其促进CO甲烷化的作用机制研究

doi:10.1016/S1872-2067(25)64688-2

催化学报 ›› 2025, Vol. 74: 177-190.DOI: 10.1016/S1872-2067(25)64688-2

Ni-CeO₂界面富电子Ni原子变化规律及其促进CO甲烷化的作用机制研究

李新立^a, 张笑楠^a, 杜臻臻^a, 韩飞雪^b, 范志辉^a, 张少康^a, 张振洲^a, 涂维峰^a^,^*(), 韩一帆^a^,^b^,^*()

^a郑州大学炼焦煤资源绿色开发全国重点实验室, 先进功能材料制造教育部工程研究中心, 河南郑州 450001
^b华东理工大学化工学院, 上海 200237

收稿日期:2025-01-18 接受日期:2025-03-14 出版日期:2025-07-18 发布日期:2025-07-20
通讯作者: *电子信箱: yifanhan@ecust.edu.cn (韩一帆),weifengtu@zzu.edu.cn (涂维峰).
基金资助:
国家自然科学基金(22278379);国家自然科学基金(22238003);国家自然科学基金(22208314);国家自然科学基金(22078307);河南省自然科学基金(232300421090);河南省自然科学基金(222301420010)

Electronic enrichment on Ni atoms at Ni-CeO₂ interfaces: Unraveling the catalytic role in CO methanation and its volcano-type relation with the CeO₂ content

Xinli Li^a, Xiaonan Zhang^a, Zhenzhen Du^a, Feixue Han^b, Zhihui Fan^a, Shaokang Zhang^a, Zhenzhou Zhang^a, Weifeng Tu^a^,^*(), Yi-Fan Han^a^,^b^,^*()

^aState Key Laboratory of Coking Coal Green Exploitation & Engineering Research Center of Advanced Functional Material Manufacturing, Ministry of Education, Zhengzhou University, Zhengzhou 450001, Henan, China
^bSchool of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2025-01-18 Accepted:2025-03-14 Online:2025-07-18 Published:2025-07-20
Contact: *E-mail: yifanhan@ecust.edu.cn (Y.-F. Han), weifengtu@zzu.edu.cn (W. Tu).
Supported by:
National Natural Science Foundation of China(22278379);National Natural Science Foundation of China(22238003);National Natural Science Foundation of China(22208314);National Natural Science Foundation of China(22078307);Natural Science Foundation of Henan(232300421090);Natural Science Foundation of Henan(222301420010)

摘要/Abstract

摘要：

CO甲烷化是一种关键的工业过程, 广泛应用于天然气生产、氨合成原料气中含氧化物的脱除以及生物质衍生气的提质. 提高CO甲烷化速率的关键在于高效活化CO中的强C≡O键. 目前, 提高CO甲烷化催化剂活性的策略之一是将可还原氧化物(如La₂O₃, ZrO₂和CeO₂等)锚定在Ni颗粒表面, 形成金属-氧化物界面. 该界面的形成可调控CO的吸附和解离行为, 从而显著提升催化剂的热稳定性和甲烷化活性. 尽管金属-氧化物相互作用对CO甲烷化催化剂的性能调控至关重要, 但界面结构如何影响表面中间体的形成及反应路径, 其微观机理仍不明确.

本文通过浸渍法合成了一系列CeO₂修饰的xCeNi/Al₂O₃催化剂, 探讨了金属-氧化物界面调控对CO甲烷化反应催化性能的优化机制, 并揭示了CeO₂团簇修饰Ni/Al₂O₃催化剂中Ni-CeO₂界面的关键作用. 催化剂性能测试表明, 当xCeNi/Al₂O₃催化剂中的Ce含量(Ce/(Ce+Ni))为0.05时(0.05CeNi/Al₂O₃), 0.05CeNi/Al₂O₃催化剂展现出最优的催化活性, 其甲烷生成速率较Ni/Al₂O₃催化剂提升4倍. X射线衍射与高分辨透射电镜表征结果表明, 小尺寸CeO₂团簇(< 6 nm)牢固锚定于Ni颗粒表面, 形成Ni-CeO₂界面, 同时不改变Ni颗粒尺寸. 结合原位X射线光电子谱及红外表征结果表明, 在Ni-CeO₂界面处经由Ni⁰与Ce⁴⁺的氧化还原反应生成部分还原的Ce³⁺原子, 并将电子转移至Ni-CeO₂界面处Ni原子, 从而形成富电子Ni活性位点. 这些富电子Ni位点显著增强了对CO和H₂的吸附与活化能力. 进一步的动力学研究表明, CO甲烷化遵循H辅助解离路径: CO* + H* → HCO* → CH* → CH₄. 富电子Ni位点通过增强电子反馈效应, 促进HCO*中间体的形成与快速转化, 大幅降低CH₄生成的表观能垒(从90 kJ mol^-1下降至66 kJ mol^-1). 然而, CeO₂的修饰并未改变CO甲烷化的基元反应步骤、速控步骤以及表面中间体的演变路径. 高精度化学反应滴定、程序升温脱附及原位红外光谱表征结果表明, 随着xCeNi/Al₂O₃催化剂中CeO₂含量的增加, 富电子Ni位点的数量在Ce/(Ce + Ni) = 0.05时达到峰值, 随后逐渐减少, 导致CH₄生成速率与CeO₂含量呈现出火山型关系. 催化剂结构-性能构效关系表明, CeO₂团簇的修饰通过调控Ni-CeO₂界面的电子结构, 显著提升了Ni催化剂的整体性能.

综上, 本文通过精确调控Ni-CeO₂界面的电子结构, 实现了对CO甲烷化反应性能的显著提升, 阐明了Ni-CeO₂界面的结构特性及其对催化性能的影响机制, 为合理设计具有定制界面电子结构的氧化物负载型多相催化剂提供一种潜在的策略.

关键词: CO甲烷化, Ni催化剂, 界面位点, 活性位点, 动态现场原位表征

Abstract:

Tuning the metal-oxide interface to achieve optimal catalytic performance represents a classic yet fast-growing area in catalysis research. This work demonstrated that the decoration of CeO₂ clusters onto Ni particles creates electron-enriched Ni sites at the Ni-CeO₂ interface with highly efficient CO methanation, by kinetics, chemical titration, and a series of in situ/operando spectroscopic characterizations. These electron-enriched Ni atoms facilitate the back-donation of electrons into the orbital of CO and thus reduce the reaction barrier of CH₄ formation, but do not alter the catalytic steps and their kinetic relevance as well as the evolution of surface intermediates during CO methanation. The amount of electron-enriched Ni atoms increases significantly to a maximum value and then decreases as the content of CeO₂ increases, leading the formation rates of CH₄ to increase in a volcano-type relation with CeO₂ contents in xCeNi/Al₂O₃ catalysts. These insights provide a comprehensive understanding of the nature and the role of the metal-oxide interface and could potentially guide the rational design of highly efficient oxide-supported catalysts for CO methanation.

Key words: CO methanation, Ni catalyst, Interfacial sites, Active sites, In-situ and operando spectroscopy

李新立, 张笑楠, 杜臻臻, 韩飞雪, 范志辉, 张少康, 张振洲, 涂维峰, 韩一帆. Ni-CeO₂界面富电子Ni原子变化规律及其促进CO甲烷化的作用机制研究[J]. 催化学报, 2025, 74: 177-190.

Xinli Li, Xiaonan Zhang, Zhenzhen Du, Feixue Han, Zhihui Fan, Shaokang Zhang, Zhenzhou Zhang, Weifeng Tu, Yi-Fan Han. Electronic enrichment on Ni atoms at Ni-CeO₂ interfaces: Unraveling the catalytic role in CO methanation and its volcano-type relation with the CeO₂ content[J]. Chinese Journal of Catalysis, 2025, 74: 177-190.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64688-2

https://www.cjcatal.com/CN/Y2025/V74/I7/177

图/表 12

Table 1 Physical properties of Ni/Al2O3 and xCeNi/Al2O3 catalysts.

Sample	Mole ratio^a Ce/(Ce+Ni)	BET surface areas^b (m² g^-1)	Mean Ni crystalline size ^c (nm)	Mean Ni particle size^d (nm)	Mean CeO₂ particle^d size (nm)	Dispersion of Ni^e (%)
Ni/Al₂O₃	—	203.7	13.1	13.2	—	7.6
0.01CeNi/Al₂O₃	0.013	244.9	14.1	—	—	7.1
0.02CeNi/Al₂O₃	0.022	225.4	15.4	—	—	6.5
0.05CeNi/Al₂O₃	0.038	229.7	15.1	14.9	3.1	6.6
0.07CeNi/Al₂O₃	0.071	224.1	15.2	—	—	6.6
0.10CeNi/Al₂O₃	0.091	205.3	14.1	15.5	4.4	7.1
0.13CeNi/Al₂O₃	0.123	189.0	14.2	15.8	5.2	7.0

Fig. 1. XRD patterns of xCeNi/Al2O3 catalysts (x = 0.00-0.13) after treated in H2/Ar (10 kPa H2 and 90 kPa Ar) at 873 K for 4 h.

Fig. 2. HRTEM images and particle size distribution of the reduced Ni/Al2O3 (a1,a2), 0.05CeNi/Al2O3 (b1,b2), 0.1CeNi/Al2O3 (c1,c2) and 0.13CeNi/Al2O3 (d1,d2) catalysts.

Fig. 3. Effect of Ce content on the rate (rCH?, per total weight of Ni atoms) and TOF (per surface Ni atoms) of CH4 formation (a, 50 kPa CO, 700 kPa H2, Ar balance, 753 K) and the turnover frequencies of CH4 formation on CO pressure (b, 753 K), H2 pressure (c, 753 K), and temperature (d, 50 kPa CO, 700 kPa H2, Ar balance, 733-773 K) during CO-H2 reactions over Ni/Al2O3 and xCeNi/Al2O3 catalysts (weight hourly space velocity (WHSV) of 2.9×107 cm3 g-1 h-1, 1 MPa).

Fig. 4. H2-TPR profiles (a), Ni 2p XPS spectra (b), and Ce 3d XPS spectra (c) of Ni/Al2O3 and xCeNiAl2O3 catalysts with different Ce contents (Ce/(Ce + Ni) = 0.01, 0.02, 0.05, 0.07, 0.1 and 0.13).

Fig. 5. The fraction of Ni0 in Ni species (a), the fraction of Ce3+ in Ce species (b), CO-TPD profiles (c) of Ni/Al2O3 and xCeNiAl2O3 catalysts with different Ce contents (Ce/(Ce + Ni) = 0.01, 0.02, 0.05, 0.07, 0.1 and 0.13), and the apparent barriers of CH4 formation versus the downshift of Ni0 binding energy (d) and the desorption temperature of CO (e) over these catalysts.

Fig. 6. H2-TPD profiles (a), the fraction of surface Ni atoms and interfacial Ce atoms (b), and the amounts (normalized by the total weight of Ni atoms) of surface Ni atoms and interfacial Ce atoms (c) on Ni/Al2O3 and xCeNi/Al2O3 catalysts with different Ce contents (Ce/(Ce + Ni) = 0.01, 0.02, 0.05, 0.07, 0.1, and 0.13).

Fig. 7. The adsorption of CO (determined from the CO-TPD profiles in Fig. 5(c), normalized by total weight of Ni atoms) (a), the in-situ CO-DRIFTS spectra (b), and the fraction of interfacial CO (c) on Ni/Al2O3 and xCeNi/Al2O3 catalysts with different Ce contents (Ce/(Ce + Ni) = 0.01, 0.02, 0.05, 0.07, 0.1, and 0.13).

Fig. 8. Rates of CH4 formation (per total weight of Ni atoms) versus the amount of the H2 adsorption on interfacial Ni-CeO2 sites (a) and the amount of the CO adsorption on the interfacial Ni-CeO2 sites (b).

Fig. 9. Operando DRIFTS spectra of Ni/Al2O3 (a) and 0.05CeNi/Al2O3 (b) catalysts during CO-H2 (5 vol% CO, 70 vol% H2 and Ar balance) reaction at different temperatures (548-673 K).

Fig. 10. Transient DRIFTS spectra of Ni/Al2O3 and 0.05CeNi/Al2O3 catalysts in 5 vol% CO/Ar for 15 min (a,d), followed by Ar flow (b,e) and 70 vol% H2/Ar (c,f) at 573 K.

Scheme 1. Plausible mechanisms of CO methanation over Ni/Al2O3 and CeNi/Al2O3 catalysts.

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Ni-CeO₂界面富电子Ni原子变化规律及其促进CO甲烷化的作用机制研究

Electronic enrichment on Ni atoms at Ni-CeO₂ interfaces: Unraveling the catalytic role in CO methanation and its volcano-type relation with the CeO₂ content

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