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

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

Chinese Journal of Catalysis ›› 2026, Vol. 90: 117-129.DOI: 10.1016/S1872-2067(26)65204-7

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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:2026-11-05 Published:2026-09-09
About author:First author contact:
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

Abstract

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

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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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65204-7

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

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