Citation: Wei Yan, Rui Sun, Meng Li, Licheng Li, Zhuhong Yang, Zelin Hua, Xiaohua Lu, Chang Liu. Heterogeneous interfacial engineering of Pd/TiO₂ with controllable carbon content for improved direct synthesis efficiency of H₂O₂[J]. Chinese Journal of Catalysis, ;2020, 41(2): 312-321. doi: S1872-2067(19)63412-1 shu

Heterogeneous interfacial engineering of Pd/TiO₂ with controllable carbon content for improved direct synthesis efficiency of H₂O₂

Wei Yan ^a, ,
Rui Sun ^a ,
Meng Li ^a ,
Licheng Li ^b ,
Zhuhong Yang ^a ,
Zelin Hua ^b ,
Xiaohua Lu ^a ,
Chang Liu ^a

a State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, Jiangsu, China;
b College of Chemical Engineering, Innovation Research Center of Lignocellulosic Functional Materials, Nanjing Forestry University, Nanjing 210037, Jiangsu, China

Received Date: 28 March 2019
Revised Date: 22 May 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (21878143, 21476106, 21838004), Joint Re-search Fund for Overseas Chinese Scholars and Scholars in Hong Kong and Macao Young Scholars (21729601), the fund of State Key Laboratory of Materials-Oriented Chemical Engineering (ZK201702), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

Series of heterogeneous interfacial engineered TiO₂ (C-TiO₂) with controllable carbon content were facilely synthesized by incipient-wet impregnation using glucose and subsequent thermal carbonization. The obtained C-TiO₂ were used as catalytic supports to load Pd nanoparticles for H₂O₂ direct synthesis from H₂ and O₂. The as-prepared samples were systematically studied by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), air isothermal microcalorimeter, temperature-programmed reduction of H₂ (H₂-TPR), and so on. The catalytic results showed that H₂O₂ productivity and H₂O₂ selectivity of Pd/C-TiO₂ firstly rose with increasing carbon content and then declined. Pd/C-TiO₂ catalyst with 1.89 wt% of carbon content showed the best catalytic performance that had 61.2% of selectivity and 2192 mmol H₂O₂/g_Pd/h of productivity, which were significantly better than those of pristine Pd/TiO₂ (45.2% and 1827 mmol H₂O₂/g_Pd/h). Various characterization results displayed that the carbon species were heterogeneously dispersed on TiO₂ surface. Moreover, no obvious geometric transformation in supports and Pd nanoparticles were observed among different catalysts. The superficial hydrophobicity of Pd/C-TiO₂ was gradually promoted with increasing carbon content, which led to the corresponding decrease in adsorption energy of H₂O₂ with catalysts. According to structure-performance relationship analyses, the heterogeneous interfacial engineering of carbon could maintain the interaction of Pd nanoparticles with TiO₂ and simultaneously accelerate the H₂O₂ desorption. Both factors further determined the excellent H₂O₂ direct synthesis performance of Pd/C-TiO₂.
- Direct synthesis of H₂O₂,
- TiO₂,
- Carbon,
- Heterogeneous interfacial engineering,
- Pd
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Heterogeneous interfacial engineering of Pd/TiO₂ with controllable carbon content for improved direct synthesis efficiency of H₂O₂