Ir/TiO2催化剂甲烷燃烧反应中TiO2晶面依赖效应

doi:10.1016/S1872-2067(24)60227-5

催化学报 ›› 2025, Vol. 70: 378-387.DOI: 10.1016/S1872-2067(24)60227-5

Ir/TiO₂催化剂甲烷燃烧反应中TiO₂晶面依赖效应

段会梅^a^,^*^,¹(), 李晓菲^a^,¹, 王传辉^a, 张丛筠^a, 余楷文^b, 陈磊^a, 张云尚^c, 纪嘉宾^a, 杨贤峰^d, 杨东江^a^,^e^,^*()

^a青岛大学环境科学与工程学院, 生物纤维与生态纺织品国家重点实验室, 山东青岛 266071, 中国
^b昆士兰大学环境学院, 昆士兰州布里斯班, 澳大利亚
^c中国科学技术大学化学物理系, 安徽省表界面化学与能源催化重点实验室, 安徽合肥 230026, 中国
^d华南理工大学分析测试中心, 广东广州 510640, 中国
^e宁波工业大学微纳材料与器件研究所, 浙江宁波 315211, 中国

收稿日期:2024-10-29 接受日期:2024-12-13 出版日期:2025-03-18 发布日期:2025-03-20
通讯作者: * 电子信箱: duanhm@qdu.edu.cn (段会梅),d.yang@qdu.edu.cn (杨东江).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22376110);山东省自然科学基金(ZR2023ME098);山东省自然科学基金(ZR2021QB083);青岛市应用基础研究项目(RZ2200001413);生物纤维与生态纺织品国家重点实验室(青岛大学)(RZ2000004399)

TiO₂-facet-dependent effect on methane combustion over Ir/TiO₂ catalysts

Huimei Duan^a^,^*^,¹(), Xiaofei Li^a^,¹, Chuanhui Wang^a, Congyun Zhang^a, Kaiwen Yu^b, Lei Chen^a, Yunshang Zhang^c, Jiabin Ji^a, Xianfeng Yang^d, Dongjiang Yang^a^,^e^,^*()

^aSchool of Environmental Science and Engineering, State Key Laboratory of Bio-fibers and Eco-textiles, Qingdao University, Qingdao 266071, Shandong, China
^bSchool of the Environment, The University of Queensland, Brisbane, QLD, 4072, Australia
^cKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, Anhui, China
^dAnalytical and Testing Centre, South China University of Technology, Guangzhou 510640, Guangdong, China
^eInstitute of Micro/Nano Materials and Devices, Ningbo University of Technology, Ningbo 315211, Zhejiang, China

Received:2024-10-29 Accepted:2024-12-13 Online:2025-03-18 Published:2025-03-20
Contact: * E-mail: duanhm@qdu.edu.cn (H. Duan),d.yang@qdu.edu.cn (D. Yang).
About author:¹Contributed equally to this work.
Supported by:
National Nature Science Foundation of China(22376110);Shandong Provincial Natural Science Foundation(ZR2023ME098);Shandong Provincial Natural Science Foundation(ZR2021QB083);Applied Basic Research of Qingdao City (Postdoctoral Project)(RZ2200001413);State Key Laboratory of Bio-Fibers and Eco-Textiles (Qingdao University)(RZ2000004399)

摘要/Abstract

摘要：

甲烷作为一种清洁能源, 也是一种强温室效应气体. 在天然气汽车尾气净化、天然气电厂尾气处理、乏风瓦斯和油田伴生气处理等过程中, 大量低浓度未燃尽甲烷的直接排放会造成严重的能量损失和温室效应. 甲烷催化燃烧是一种有效处理低浓度甲烷的净化技术. 负载型Ir催化剂, 特别是负载在TiO₂载体上的Ir基催化剂, 因其较好的低温活化甲烷能力而受到越来越多的关注. 活性金属的氧化还原性能对催化剂的甲烷燃烧性能至关重要. 载体形貌工程借助金属-载体相互作用可有效调控活性金属的氧化还原性能. 然而至今, TiO₂暴露晶面对Ir/TiO₂催化剂甲烷燃烧性能影响及其相关机制研究尚不清楚, 阐明TiO₂暴露面与Ir/TiO₂催化剂甲烷燃烧反应活性之间的结构-性能关系具有重要意义.

本文首先制备了主要暴露{100}, {101}和{001}晶面的TiO₂纳米晶, 采用湿化学法制备了均匀负载的Ir/TiO₂纳米催化剂, 并用于甲烷催化燃烧性能评估. 研究发现, TiO₂暴露晶面显著影响了Ir/TiO₂催化剂的甲烷燃烧催化性能, 活性顺序为Ir/TiO₂-{100} > Ir/TiO₂-{101} >> Ir/TiO₂-{001}. TiO₂显著的晶面依赖效应与催化剂中不同电子金属-载体相互作用(EMSI)和氧空位紧密相关. 相比于Ir-TiO₂-{101}和Ir-TiO₂-{001}界面, Ir-TiO₂-{100}界面处具有更强的电子转移TiO₂→Ir, 诱导了富电子Ir物种的形成. 原位红外漫反射结合密度泛函理论计算研究发现, 相比于Ir/TiO₂-{101}和Ir/TiO₂-{001}催化剂, Ir-TiO₂-{100}催化剂表面更易发生CH₄分子中C-H的断裂. Ir/TiO₂-{100}催化剂中富电子Ir结构和丰富的氧空位极大地增强了活性Ir物种的氧化还原性能, 加速了CH₄和O₂分子在催化剂表面的吸附和活化, 进而显著增强了甲烷氧化催化性能.

本文清楚阐明了Ir/TiO₂催化剂在甲烷燃烧反应中TiO₂晶面依赖效应, 加深了Ir纳米催化反应体系中EMSI和氧空位对甲烷燃烧催化性能的基本理解, 为高效Ir基甲烷燃烧催化剂的设计提供了理论依据.

关键词: Ir/TiO₂, TiO₂晶面依赖, 甲烷燃烧, 氧空位, 金属-载体相互作用

Abstract:

Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction. Herein, uniform Ir nanoparticles supported on anatase TiO₂ with different morphologies predominantly exposing {100}, {101}, and {001} planes were synthesized and tested for methane combustion. The CH₄ catalytic activity shows a remarkable TiO₂-facet-dependent effect and follows the order of Ir/TiO₂-{100} > Ir/TiO₂-{101} >> Ir/TiO₂-{001}. Detailed characterizations and DFT calculations reveal that compared with Ir-TiO₂-{101} and Ir-TiO₂-{001} interfaces, the superior Ir-TiO₂-{100} interface facilitates the generation of electron-rich Ir species through more profound charge transfer from TiO₂-{100} to Ir atoms. The electron-rich Ir structure, featuring abundant defect oxygen vacancies, significantly enhances the redox properties of active Ir species and reduces the activation energy for breaking the initial C-H bond in CH₄, resulting in the superior catalytic activity for methane combustion. These findings deepen fundamental insights into the TiO₂-facet-dependent reactivity of different Ir/TiO₂ nanomaterials in methane oxidation and pave the way for designing efficient Ir-based methane oxidation catalysts.

Key words: Ir/TiO₂, TiO₂-facet-dependent, Methane combustion, Oxygen vacancies, Metal-support interaction

段会梅, 李晓菲, 王传辉, 张丛筠, 余楷文, 陈磊, 张云尚, 纪嘉宾, 杨贤峰, 杨东江. Ir/TiO₂催化剂甲烷燃烧反应中TiO₂晶面依赖效应[J]. 催化学报, 2025, 70: 378-387.

Huimei Duan, Xiaofei Li, Chuanhui Wang, Congyun Zhang, Kaiwen Yu, Lei Chen, Yunshang Zhang, Jiabin Ji, Xianfeng Yang, Dongjiang Yang. TiO₂-facet-dependent effect on methane combustion over Ir/TiO₂ catalysts[J]. Chinese Journal of Catalysis, 2025, 70: 378-387.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(24)60227-5

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图/表 8

Fig. 1. TEM and HRTEM images of three different anatase TiO2 nanocrystals. (A1,A2) TiO2-{100}; (B1,B2) TiO2-{101}; (C1,C2) TiO2-{001}.

Fig. 2. XRD and Raman spectra of pure TiO2 (A,B) and Ir/TiO2 (C,D) samples. The standard patterns of Ir (PDF# 46-1044) and anatase TiO2 (PDF# 21-1272) were attached for comparison.

Fig. 3. TEM (Inserted: particle size distributions of Ir particles) and HRTEM images of Ir/TiO2-{100} (A1,A2), Ir/TiO2-{101} (B1,B2), and Ir/TiO2-{001} (C1,C2) catalysts.

Fig. 4. The CH4 conversion (A) and CO2 yield (B) as a function of reaction temperature over Ir/TiO2-{100}, Ir/TiO2-{101}, and Ir/TiO2-{001} samples.

Fig. 5. Ir 4f (A), O 1s (B), and Ti 2p (C) XPS spectra of three different Ir/TiO2 samples.

Fig. 6. H2-TPR (A), EPR (B), and NH3-TPD (C) spectra of three different Ir/TiO2 samples.

Fig. 7. In situ DRIFTS spectra of Ir/TiO2-{100}, Ir/TiO2-{101}, and Ir/TiO2-{001} samples under the following conditions at 350 °C: 0.2% CH4/Ar (25 mL min-1) and 2% O2/Ar (25 mL min-1).

Fig. 8. Charge density difference for Ir/TiO2-{100} (A), Ir/TiO2-{101} (B), and Ir/TiO2-{001} (C) samples: cyan and yellow areas mean charge depletion and accumulation, respectively. The optimized geometric structures (D) and activation energy (E) of the first C-H bond cracking in CH4 on the surfaces of three Ir/TiO2 catalysts. I, II, and III represent Ir/TiO2-{100}, Ir/TiO2-{101}, and Ir/TiO2-{001}, respectively.

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Ir/TiO₂催化剂甲烷燃烧反应中TiO₂晶面依赖效应

TiO₂-facet-dependent effect on methane combustion over Ir/TiO₂ catalysts

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