氢诱导Pt/TiO2中Ptσ+-O-Ti4+-(H-氧空位)界面位点增强低温CO氧化

doi:10.1016/S1872-2067(26)65204-7

催化学报 ›› 2026, Vol. 90: 117-129.DOI: 10.1016/S1872-2067(26)65204-7

氢诱导Pt/TiO₂中Pt^σ+-O-Ti⁴⁺-(H-氧空位)界面位点增强低温CO氧化

田郡博^a^,^b^,^d^,^j^,¹, 郑鹏^c^,¹, 邓双^d^,^*(), 纪永军^e^,^*(), 张腾飞^f, 孙志一^g, 陈文星^g^,^*(), 王祎驰^h, 谷林^h, 苏东ⁱ, 许光文^c, 钟子宜^j^,^*(), 苏发兵^a^,^c^,^*()

^a 中国科学院过程工程研究所, 介科学与过程工程全国重点实验室, 北京 100190
^b 中国科学院大学化学工程学院, 北京 100049
^c 沈阳化工大学特色资源化工与材料教育部重点实验室, 辽宁沈阳 110142
^d 中国环境科学研究院, 基准标准与风险管控全国重点实验室, 北京 100012
^e 北京工商大学轻工科学与工程学院, 北京 100048
^f 山东科技大学低碳能源化工实验室, 山东青岛 266590
^g 北京理工大学材料科学与工程学院, 能源催化研究中心, 北京 100081
^h 清华大学材料学院, 北京电子显微镜中心和先进材料教育部重点实验室, 北京 100084
ⁱ 中国科学院物理研究所, 北京凝聚态物理国家实验室, 北京新能源材料与器件重点实验室, 清洁能源重点实验室, 北京 100190
^j 广东以色列理工学院化学工程系, 广东省能量转换材料与技术重点实验室, 广东汕头 515063

收稿日期:2026-03-23 接受日期:2026-06-05 出版日期:2026-11-18 发布日期:2026-09-09
通讯作者: *电子信箱: dengshuang@craes.org.cn (邓双),
yjji@btbu.edu.cn (纪永军),
wxchen@bit.edu.cn (陈文星),
ziyi.zhong@gtiit.edu.cn (钟子宜),
fbsu@ipe.ac.cn (苏发兵).
作者简介:
¹共同第一作者.
基金资助:
京津冀环境综合治理国家科技重大专项(2024ZD1200400);国家重点研发计划(2023YFC3707001);国家自然科学基金(52025025);国家自然科学基金(52250402);国家自然科学基金(22305138);国家自然科学基金创新研究群体科学基金(52421001);中国博士后科学基金(2024M761649);中国博士后科学基金(GZC20231203);清华大学水木学者

Hydrogen-induced Pt^σ⁺-O-Ti⁴⁺-(H-oxygen vacancy) interfacial sites in Pt/TiO₂ for enhanced low-temperature CO oxidation

Junbo Tian^a^,^b^,^d^,^j^,¹, Peng Zheng^c^,¹, Shuang Deng^d^,^*(), Yongjun Ji^e^,^*(), Tengfei Zhang^f, Zhiyi Sun^g, Wenxing Chen^g^,^*(), Yi-Chi Wang^h, Lin Gu^h, Dong Suⁱ, Guangwen Xu^c, Ziyi Zhong^j^,^*(), Fabing Su^a^,^c^,^*()

^a State Key Laboratory of Mesoscience and Process Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
^b School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100190, China
^c Key Laboratory on Resources Chemicals and Materials of Ministry of Education, Shenyang University of Chemical Technology, Shenyang 110142, Liaoning, China
^d State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
^e School of Light Industry Science and Engineering, Beijing Technology and Business University, Beijing 100048, China
^f Key Laboratory of Low Carbon Energy and Chemical Engineering, Shandong University of Science and Technology, Qingdao 266590, Shandong, China
^g Energy & Catalysis Centre, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
^h Beijing National Center for Electron Microscopy and Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
ⁱ Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
^j Department of Chemical Engineering, and Guangdong Provincial Key Laboratory of Materials and Technologies for Energy Conversion (MATEC), Guangdong Technion Israel Institute of Technology (GTIIT), Shantou 515063, Guangdong, China

Received:2026-03-23 Accepted:2026-06-05 Online:2026-11-18 Published:2026-09-09
Contact: *E-mail:dengshuang@craes.org.cn(S. Deng),yjji@btbu.edu.cn(Y. Ji),wxchen@bit.edu.cn(W. Chen),ziyi.zhong@gtiit.edu.cn(Z. Zhong),fbsu@ipe.ac.cn(F. Su).
About author:
¹These authors contributed equally to this work.
Supported by:
Jing-Jin-Ji Regional Integrated Environmental Improvement-National Science and Technology Major Project(2024ZD1200400);National Key R&D Program of China(2023YFC3707001);National Natural Science Foundation of China(52025025);National Natural Science Foundation of China(52250402);National Natural Science Foundation of China(22305138);Science Fund for Creative Research Groups of the National Natural Science Foundation of China(52421001);China Postdoctoral Science Foundation(2024M761649);China Postdoctoral Science Foundation(GZC20231203);Shuimu Scholar from Tsinghua University

摘要/Abstract

摘要：

随着工业化进程的加速, CO作为典型的大气污染物及工业尾气的重要组成部分, 其高效去除对于环境保护与工业安全具有重要意义. 负载型贵金属催化剂因其优异的低温CO氧化活性而备受关注, 在此类催化剂中金属-载体相互作用(MSI)被认为是决定催化剂活性、稳定性及抗中毒性能的关键因素. 传统MSI理论普遍认为其形成机制主要源于高温还原条件下产生的氧空位及由此引发的电子转移效应, 而氢气在界面结构重构中的作用通常仅被视为还原剂效应而未被充分重视. 近年来, 越来越多的研究表明, 氢原子可能直接参与界面结构的构建并诱导新活性位点的形成. 因此, 揭示氢诱导的界面重构机制, 阐明其对催化反应路径及MSI调控规律, 具有重要的科学价值, 有助于新型高效催化剂的开发及MSI理论的深化.

本研究以商业TiO₂为载体, 通过纯氢气处理制备TiO₂-100%H₂载体, 并采用浸渍法制备Pt/TiO₂-100%H₂催化剂, 系统探讨了氢诱导界面重构对CO氧化性能的影响. 结合表征技术与密度泛函理论(DFT)计算结果表明, 氢处理后TiO₂亚表面氧空位通过电荷补偿机制稳定了原子氢, 形成了独特的O-Ti⁴⁺-(H-OV)结构. Pt负载后, 该结构进一步诱导Pt与载体之间形成新型Pt^σ+-O-Ti⁴⁺-(H-OV)界面构型, 构建了线性的电子-质子协同传输通道. 界面重构导致Pt中心及界面氧原子电子密度增加, 使Pt-O键长由1.952 Å延长至2.014 Å, O-Ti键长由2.021 Å延长至2.054 Å. 原位表征及DFT计算进一步揭示, Pt^σ⁺-O-Ti⁴⁺-(H-OV)界面不仅促进了CO分子的吸附活化, 还增强了界面吸附氧及晶格氧的活化与迁移能力. 一方面, 电子富集的Pt中心促进了O₂的吸附及界面吸附氧的形成; 另一方面, 亚表面氢占据氧空位后与Pt中心形成的界面相互作用增强了晶格氧的迁移能力. 基于此, 提出了一种耦合Langmuir-Hinshelwood(L-H)机制与Mars-van Krevelen(MvK)机制的协同氧化路径: 其一, CO吸附并与吸附氧(O_ads)反应, 即L-H机制; 其二, CO与活化的界面晶格氧(O_latt)反应, 即MvK机制. 两种途径协同促进了CO₂的快速生成与解吸. 在Pt负载量仅为0.17 wt%的条件下, Pt/TiO₂-100%H₂催化剂即可在120 °C实现CO的完全转化, 并在含0.005% SO₂及10 vol% H₂O的复杂气氛中表现出优异的稳定性. 与传统Pt/TiO₂催化剂相比, 其在120 °C下的周转频率提升了59倍, 显示出显著增强的本征活性.

综上, 本研究突破了传统MSI主要依赖氧空位调控的既有认知框架, 揭示了氢诱导的金属-载体界面重构新机制, 进而阐明了氢介导界面重构在催化反应中的关键作用. 上述发现为高效低温CO氧化催化剂的设计提供了新的理论基础和思路. 此外, 所构建的Pt^σ⁺-O-Ti⁴⁺-(H-OV)界面结构模型有望拓展至其他可还原氧化物负载金属体系.

关键词: CO氧化, Pt/TiO₂催化剂, 氢还原, 氧空位, 界面结构

Abstract:

Understanding reconstructed interfacial sites is crucial for enhancing the catalytic conversion efficiency, as these sites can facilitate reactant adsorption, transformation, and desorption. Herein, we report an unconventional interfacial structure of Pt^σ⁺-O-Ti⁴⁺-H^δ⁺-oxygen vacancy (OV), in which atomic hydrogen binds to Ti⁴⁺ sites via a charge-compensation mechanism involving subsurface OVs. This restructuring induced by hydrogen creates electron-rich Pt centers and interfacial oxygen, resulting in spatial elongation of the Pt-O and O-Ti bonds. This Pt^σ⁺-O site, stabilized by -Ti⁴⁺-(H-OV), promotes the activation of CO adsorption/interfacially absorbed oxygen and interfacial lattice oxygen, effectively coupling the Langmuir-Hinshelwood and Mars-van Krevelen pathways. These sites facilitate the rapid CO₂ formation and desorption. Consequently, this system achieves complete CO conversion at 120 °C with an ultralow Pt loading of 0.17 wt% (even in the presence of 0.005% SO₂ and 10% vol H₂O) and a 59-fold increase in turnover frequency compared to the control sample lacking this interfacial structure.

Key words: CO oxidation, Pt/TiO₂ catalyst, Hydrogen reduction, Oxygen vacancy, Interfacial structure

田郡博, 郑鹏, 邓双, 纪永军, 张腾飞, 孙志一, 陈文星, 王祎驰, 谷林, 苏东, 许光文, 钟子宜, 苏发兵. 氢诱导Pt/TiO₂中Pt^σ+-O-Ti⁴⁺-(H-氧空位)界面位点增强低温CO氧化[J]. 催化学报, 2026, 90: 117-129.

Junbo Tian, Peng Zheng, Shuang Deng, Yongjun Ji, Tengfei Zhang, Zhiyi Sun, Wenxing Chen, Yi-Chi Wang, Lin Gu, Dong Su, Guangwen Xu, Ziyi Zhong, Fabing Su. Hydrogen-induced Pt^σ⁺-O-Ti⁴⁺-(H-oxygen vacancy) interfacial sites in Pt/TiO₂ for enhanced low-temperature CO oxidation[J]. Chinese Journal of Catalysis, 2026, 90: 117-129.

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https://www.cjcatal.com/CN/Y2026/V90/I11/117

图/表 5

Fig. 1. Support modification strategy and structure characterization. (a) Schematic illustration of the support preparation. EPR spectra (b) and 1H NMR spectra (c) of the TiO2 supports. (d) Crystal structure along anatase TiO2 (101) plane and the enlarged rainbow-colored ABF-STEM image of TiO2-100%H2, black and white dotted circles represent the possible occupied OVs. (e) The intensity STEM line profiles of the selected orange dotted zone.

Fig. 2. Catalyst preparation and structure characterization. (a) Schematic illustration of the catalyst preparation. TEM image (b), particle distribution (c), and AC-HAADF-STEM image (d) of Pt/TiO2-100%H2 catalyst, insert of (d): filtered image via FFT. Raman spectra (e), EPR spectra (f), H2-TPR profiles (g), Pt 4f spectra (h), and O 1s spectra (i) of Pt/TiO2, Pt/TiO2-air, and Pt/TiO2-100%H2. k2 weighted Fourier transform spectra from EXAFS (j) and normalized Pt L3 edge XANES (k) spectra of Pt foil, PtO2, Pt/TiO2, Pt/TiO2-air, and Pt/TiO2-100%H2. (l) Bader Charge analysis of Pt/TiO2-100%H2 (la) and Pt/TiO2 (lb). (m) Proposed scheme for the lengthened Ti-O and Pt-O bonds and their electron transfer on Pt-O-Ti-(H-OV) structure of Pt/TiO2-100%H2 (grey, Pt; red, O; lotus pink, H; blue, Ti).

Fig. 3. The measured catalytic performances of all the catalysts. (a) CO conversion as a function of reaction temperature over all catalysts. Reaction conditions: 0.4 g of catalyst, a gas mixture containing 1 vol% CO and 16 vol% O2 balanced with N2. (b) The cycling test of the CO oxidation activity of Pt/TiO2-100%H2 from 80 to 160 °C. Cyclic CO oxidation reaction condition: 0.4 g of catalyst, a gas mixture containing 1 vol% CO and 16 vol% O2 balanced with N2. (c) Ea over different catalysts. (d) Pt specific TOFs of the catalysts at 110 °C and 120 °C. (e) Cyclic CO conversion of Pt/TiO2-100%H2 in the presence of 0.005% SO2 and/or 10 vol%H2O. (f) CO conversion on stream reaction time over Pt/TiO2-100%H2 in the presence of 0.005% SO2 and/or 10 vol%H2O. (g) A long-term test of Pt/TiO2-100%H2. Reaction conditions: 0.4 g of catalyst, 1 vol% CO, 16 vol% O2, balanced with N2, 400 mL min−1, WHSV = 60000 mL g−1 h−1).

Fig. 4. Investigation of the reaction mechanism for CO oxidation. In-situ DRIFTS spectra recorded on Pt/TiO2-100%H2 after introducing CO, CO+O2, and removing CO (a), after introducing O2 and switching to CO (b). (c) Raman spectra under CO exposure on Pt/TiO2-100%H2. In-situ NAP XPS of O 1s spectra on Pt/TiO2-100%H2 of UHV, introducing CO, and switching to O2 (d), and UHV, introducing O2, and switching to CO (e). (f) Illustration of dual functional interfacial sites.

Fig. 5. DFT calculations conducted to investigate the CO oxidation mechanisms over Pt/TiO2 and Pt/TiO2-100%H2. The Gibbs free energy variation of intermediates in CO oxidation via MvK on Pt/TiO2-100%H2 (a) and Pt/TiO2 (b); via L-H on Pt/TiO2-100%H2 (c) and on Pt/TiO2 (d).

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氢诱导Pt/TiO₂中Pt^σ+-O-Ti⁴⁺-(H-氧空位)界面位点增强低温CO氧化

Hydrogen-induced Pt^σ⁺-O-Ti⁴⁺-(H-oxygen vacancy) interfacial sites in Pt/TiO₂ for enhanced low-temperature CO oxidation

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