核壳结构Pd@CeO2/γ-Al2O3催化剂: 提升化学计量比天然气车辆废气处理的效率与耐久性

doi:10.1016/S1872-2067(25)64926-6

催化学报 ›› 2026, Vol. 82: 348-362.DOI: 10.1016/S1872-2067(25)64926-6

核壳结构Pd@CeO₂/γ-Al₂O₃催化剂: 提升化学计量比天然气车辆废气处理的效率与耐久性

潘润^a^,^g^,¹, Abubakar Yusuf^a^,¹, 王成俊^b^,^*(), 李建荣^c, 肖旨育^a, 刘帅^d, 钟易东^a, 任勇^e, 王筝^a, 杜海南^a, 周俊良^a^,^*(), 陈政^f, 何俊^a^,^g^,^*()

^a宁波诺丁汉大学化学与环境工程系, 浙江宁波 315000, 中国
^b湖南工学院化学与环境工程学院, 湖南衡阳 421000, 中国
^c宁波(北仑)中科海西产业技术创新中心, 城市环境过程与污染控制重点实验室, 浙江宁波 315000, 中国
^d浙大宁波理工学院机电与能源工程学院, 浙江宁波 315000, 中国
^e宁波诺丁汉大学机械、材料及制造工程系, 浙江宁波 315000, 中国
^f诺丁汉大学化学与环境工程系, 英国
^g诺丁汉大学卓越灯塔计划(宁波)创新研究院, 浙江宁波 315000, 中国

收稿日期:2025-07-23 接受日期:2025-10-21 出版日期:2026-03-18 发布日期:2026-03-05
通讯作者: * 电子信箱: cjwang@hnit.edu.cn (王成俊),john.zhou@nottingham.edu.cn (周俊良),jun.he@nottingham.edu.cn (何俊).
作者简介:¹共同第一作者.
基金资助:
宁波市自然科学基金(2023J024);宁波市公益类重点研发计划(2023S038);宁波市“科创甬江2035”重点研发计划(2024Z237);宁波市“科创甬江2035”重点研发计划(2024Z251);湖南省自然科学基金(2025JJ50204)

Core-shell Pd@CeO₂/γ‐Al₂O₃ catalysts: Boosting efficiency and durability in stoichiometric natural gas vehicle exhaust treatment

Run Pan^a^,^g^,¹, Abubakar Yusuf^a^,¹, Chengjun Wang^b^,^*(), Jianrong Li^c, Zhiyu Xiao^a, Shuai Liu^d, Yidong Zhong^a, Yong Ren^e, Zheng Wang^a, Hainam Do^a, John L. Zhou^a^,^*(), George Zheng Chen^f, Jun He^a^,^g^,^*()

^aDepartment of Chemical and Environmental Engineering, University of Nottingham Ningbo China, Ningbo 315000, Zhejiang, China
^bSchool of Chemical and Environmental Engineering, Hunan Institute of Technology, Hengyang 421000, Hunan, China
^cNingbo Key Laboratory of Urban Environmental Pollution and Control, Ningbo (Beilun) Zhongke Haixi Industrial Technology Innovation Center, Ningbo 315000, Zhejiang, China
^dSchool of Mechatronics and Energy Engineering, NingboTech University, Ningbo 315000, Zhejiang, China
^eDepartment of Mechanical, Materials and Manufacturing Engineering, University of Nottingham Ningbo China, Ningbo 315000, Zhejiang, China
^fDepartment of Chemical and Environmental Engineering, Faculty of Engineering, University of Nottingham, Nottingham, UK
^gNottingham Ningbo China Beacons of Excellence Research and Innovation Institute, Ningbo 315000, Zhejiang, China

Received:2025-07-23 Accepted:2025-10-21 Online:2026-03-18 Published:2026-03-05
Contact: * E-mail: cjwang@hnit.edu.cn (C. Wang),john.zhou@nottingham.edu.cn (J. L. Zhou),jun.he@nottingham.edu.cn (J. He).
About author:¹Contributed equally to this work.
Supported by:
Ningbo Natural Science Foundation Grant(2023J024);Ningbo Commonweal Key Research Program(2023S038);Ningbo Key Technology Breakthrough Projects under Yongjiang Science and Innovation 2035 Scheme(2024Z237);Ningbo Key Technology Breakthrough Projects under Yongjiang Science and Innovation 2035 Scheme(2024Z251);Hunan Provincial Natural Science Foundation of China(2025JJ50204)

摘要/Abstract

摘要：

随着中国国六(VI)和欧盟欧七(Euro VII)等车辆排放法规的日趋严格, 天然气车辆(NGVs)因其高燃烧效率和较低污染物排放而成为一种颇具前景的清洁交通工具. 在化学计量比燃烧条件下, 三效催化(TWC)技术可同时高效净化尾气中的甲烷(CH₄)、一氧化碳(CO)和氮氧化物(NO_x). 然而, CH₄分子具有极高的化学稳定性, 其高效催化氧化是主要技术挑战; 同时, NGVs的高温排气环境(有时超过800 °C)易导致传统Pd基催化剂因烧结和水热老化而失活. 因此, 开发兼具高低温活性与优异耐久性的TWC催化剂, 是推动NGVs广泛应用、满足严格排放标准的关键之一.

本研究成功设计并制备了一种核壳结构的Pd@CeO₂/Al₂O₃三效催化剂, 旨在显著提升其在化学计量比NGVs尾气处理中的催化效率与耐久性. 通过超分子自组装法构筑的Pd@CeO₂/Al₂O₃核壳结构, 其内核为金属Pd, 外壳由CeO₂纳米颗粒组成, 载体为γ-Al₂O₃. 系统表征(X射线衍射, N₂吸附-脱附, 透射电镜, X射线光电子能谱, H₂-程序升温还原, CO-红外漫反射光谱(DRIFTS))结果表明, 该核壳结构有效抑制了Pd纳米颗粒的烧结, 增大了催化剂比表面积(500 °C煅烧的Pd@Ce/Al (S-500)催化剂达186 m²/g), 增强了金属-载体相互作用, 并显著提升了表面Ce³⁺比例和氧空位浓度. 催化性能测试结果表明, 优化后的核壳催化剂Pd@Ce/Al (S-500)展现出优异的低温起燃活性, 其对CH₄和NO转化的T₅₀值分别低至336和397 °C; 与无核壳结构的参比催化剂Pd-Ce/Al (S-500)相比, 其T₉₀值分别降低了113和177 °C. 动力学测试进一步证实, Pd@Ce/Al (S-500)具有在350 °C下最高的反应速率(3312.7 µmol/(s·mol_Pd))和周转频率(0.032 s^-1), 以及最低的CH₄氧化表观活化能(102.2 kJ/mol). CO-DRIFTS分析明确将Pd-CeO₂界面识别为三效催化的关键活性位点. 密度泛函理论计算从分子层面揭示了性能提升的机理: 核壳结构优化了Pd-CeO₂界面的电子结构, 使Pd处于较低的氧化态并具有更高的d带中心, 从而显著降低了CH₄首个C-H键断裂能垒(从PdO(101)的0.64 eV降至PdCeO(111)的0.18 eV)及NO还原能垒. 值得注意的是, 在经过800 °C、16 h苛刻水热老化后, 核壳催化剂Pd@Ce/Al (S-500)在长达100 h的连续运行稳定性测试中, 对CH₄和NO的转化率仅分别下降5.5%和6.6%, 展现出较好的长期水热稳定性, 这主要归因于CeO₂壳层对Pd内核的物理屏障效应, 以及界面处更利于H₂O解离并利用其参与反应的特性.

综上, 本工作通过实验与理论计算相结合, 深入阐释了核壳Pd@CeO₂结构在提升Pd基TWC催化剂活性和稳定性中的关键作用, 特别是Pd-CeO₂界面作为核心活性位点的功能机制. 该研究为设计开发适用于下一代天然气车辆尾气净化并满足超低排放法规要求的高性能、高耐久性三效催化剂提供了新的设计思路和理论依据. 未来, 通过进一步优化核壳结构的组成与微观结构, 并探索其在实际复杂工况下的应用潜力, 有望推动此类高效催化剂在天然气车辆尾气净化领域的应用研究及推广.

关键词: 核壳催化剂, Pd@CeO₂/Al₂O₃催化剂, 天然气车辆, 化学计量比燃烧, 三效催化, 水热稳定性

Abstract:

Natural gas vehicles (NGVs) offer significant environmental advantages by reducing pollutant emissions, but effective exhaust treatment remains a challenge due to high methane emissions and catalyst deactivation over time. This study introduces a core-shell Pd@CeO₂/Al₂O₃ three-way catalyst (TWC) designed to enhance the efficiency and durability of NGV exhaust treatment. The core-shell structure significantly improves catalytic performance. The optimized Pd@Ce/Al (S-500) catalyst demonstrates excellent low-temperature activity, with T₅₀ values of 336 °C for CH₄ and 397 °C for NO. It also achieves remarkable reductions of 113 and 177 °C in the T₉₀ for CH₄ and NO conversion, respectively, compared to the non-core-shell counterpart, Pd-Ce/Al (S-500). Characterizations reveal enhanced metal-support interactions, increased oxygen vacancies, and optimized Pd-CeO₂ interfaces as key active sites. Density functional theory calculations further demonstrate that the core-shell structure facilitates electron transfer at Pd-CeO₂ interfaces and lowers energy barriers for three-way reactions, enhancing catalytic efficiency. Notably, the core-shell Pd@Ce/Al (S-500) catalyst maintains high conversion efficiency for CH₄ and NO, with only slight losses (5.5% and 6.6%, respectively) over a 100-h time-on-stream stability test, following 16 h of harsh hydrothermal aging at 800 °C, showcasing its long-term stability. These findings provide a deeper understanding of the role of the core-shell Pd@CeO₂ structure in Pd-based TWCs and offer valuable insights for designing durable and efficient catalysts to meet the stringent emission standards of NGVs.

Key words: Core-shell catalyst, Pd@CeO₂/Al₂O₃, Natural gas vehicles, Stoichiometric combustion, Three-way catalysis, Hydrothermal stability

潘润, Abubakar Yusuf, 王成俊, 李建荣, 肖旨育, 刘帅, 钟易东, 任勇, 王筝, 杜海南, 周俊良, 陈政, 何俊. 核壳结构Pd@CeO₂/γ-Al₂O₃催化剂: 提升化学计量比天然气车辆废气处理的效率与耐久性[J]. 催化学报, 2026, 82: 348-362.

Run Pan, Abubakar Yusuf, Chengjun Wang, Jianrong Li, Zhiyu Xiao, Shuai Liu, Yidong Zhong, Yong Ren, Zheng Wang, Hainam Do, John L. Zhou, George Zheng Chen, Jun He. Core-shell Pd@CeO₂/γ‐Al₂O₃ catalysts: Boosting efficiency and durability in stoichiometric natural gas vehicle exhaust treatment[J]. Chinese Journal of Catalysis, 2026, 82: 348-362.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64926-6

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图/表 6

Fig. 1. TEM images of Pd@CeO2 (A1,A2), Pd@CeO2-OA (B1, B2), Pd-CeO2 (C1,C2), Pd-CeO2-OA (D1,D2). DF-TEM images with EDS mapping analysis and EDS line profiles of Pd@CeO2 (E1-E4) and Pd@CeO2-OA (F1-F4).

Fig. 2. Heating light-off curves of all samples on catalytic CO, CH4 and NO reaction and the samples calcined at 500 °C (a-c) and 850 °C (d-f). Conditions: 5000 ppm CO, 1000 ppm CH4, 1000 ppm NO, 4000 ppm O2, 10% CO2 and N2, GHSV = 100 L/(g·h). (g-i) TOS test on catalytic CO, CH4 and NO reaction for aged Pd@Ce/Al (S-500) and aged Pd-Ce/Al (S-500) at GHSV = 100 L/(g·h) and 450 °C. Conditions: 5000 ppm CO, 1000 ppm CH4, 1000 ppm NO, 4000 ppm O2, 10% CO2, 10% H2O and N2.

Fig. 3. Arrhenius plots for CH4 over the Pd@Ce/Al-E, Pd@Ce/Al-S, Pd-Ce/Al-E and Pd-Ce/Al-S calcined at 500 °C (a) and 850 °C (b). Conditions: 5000 ppm CO, 1000 ppm CH4, 1000 ppm NO, 4000 ppm O2, 10% CO2 and N2, GHSV = 300 L/(g·h).

Fig. 4. XPS spectra of Pd 3d (a,b), O 1s (c,d) and Ce 3d (e,f) of catalysts.

Fig. 5. H2-TPR profiles (a,b) and DRIFTS spectra (c,d) of Pd@Ce/Al-E, Pd@Ce/Al-S, Pd-Ce/Al-E and Pd-Ce/Al-S calcined at 500 and 850 °C.

Fig. 6. (a) Partial density of states for PdO (101) and PdCeO (111). The energy profile on PdO (101) (red) and PdCeO (111) (black) of CH4 dissociation (b), NO + CO reaction (c), NO + CH4 reaction (d), NO dissociation (e), and H2O dissociation (f). O: red; Ce: yellow; Pd: gray; C: brown; H: pink.

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核壳结构Pd@CeO₂/γ-Al₂O₃催化剂: 提升化学计量比天然气车辆废气处理的效率与耐久性

Core-shell Pd@CeO₂/γ‐Al₂O₃ catalysts: Boosting efficiency and durability in stoichiometric natural gas vehicle exhaust treatment

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