Intra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes

Honggen Peng; Tao Dong; Shenyou Yang; Hao Chen; Zhenzhen Yang; Wenming Liu; Chi He; Peng Wu; Jinshu Tian; Yue Peng; Xuefeng Chu; Daishe Wu; Taicheng An; Yong Wang; Sheng Dai

doi:10.1038/s41467-021-27828-x

Intra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes

Nat Commun. 2022 Jan 13;13(1):295. doi: 10.1038/s41467-021-27828-x.

Authors

Honggen Peng^#¹, Tao Dong^#², Shenyou Yang², Hao Chen^{3

4}, Zhenzhen Yang^{3

4}, Wenming Liu², Chi He⁵, Peng Wu⁶, Jinshu Tian⁷, Yue Peng⁸, Xuefeng Chu⁸, Daishe Wu², Taicheng An⁹, Yong Wang¹⁰, Sheng Dai^{11

12}

Affiliations

¹ Key Laboratory of Poyang Lake Environment and Resource Utilization, Ministry of Education, School of Resources Environmental and Chemical Engineering, College of Chemistry, Nanchang University, 999 Xuefu Road, Nanchang, Jiangxi, 330031, China. penghonggen@ncu.edu.cn.
² Key Laboratory of Poyang Lake Environment and Resource Utilization, Ministry of Education, School of Resources Environmental and Chemical Engineering, College of Chemistry, Nanchang University, 999 Xuefu Road, Nanchang, Jiangxi, 330031, China.
³ Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37830, USA.
⁴ Department of Chemistry, University of Tennessee, Knoxville, TN, 37996, USA.
⁵ State Key Laboratory of Multiphase Flow in Power Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, 710049, Shaanxi, China. chi_he@xjtu.edu.cn.
⁶ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry and Molecular Engineering, East China Normal University, North Zhongshan Road 3663, Shanghai, 200062, China.
⁷ Technology and College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014, China.
⁸ State Key Joint Laboratory of Environment Simulation and Pollution Control, National Engineering Laboratory for Multi Flue Gas Pollution Control Technology and Equipment, School of Environment, Tsinghua University, Beijing, 100084, China.
⁹ Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou, 510006, China. antc99@gdut.edu.cn.
¹⁰ The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA.
¹¹ Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37830, USA. dais@ornl.gov.
¹² Department of Chemistry, University of Tennessee, Knoxville, TN, 37996, USA. dais@ornl.gov.

^# Contributed equally.

Abstract

Zeolite-confined metal nanoparticles (NPs) have attracted much attention owing to their superior sintering resistance and broad applications for thermal and environmental catalytic reactions. However, the pore size of the conventional zeolites is usually below 2 nm, and reactants are easily blocked to access the active sites. Herein, a facile in situ mesoporogen-free strategy is developed to design and synthesize palladium (Pd) NPs enveloped in a single-crystalline zeolite (silicalite-1, S-1) with intra-mesopores (termed Pd@IM-S-1). Pd@IM-S-1 exhibited remarkable light alkanes deep oxidation performances, and it should be attributed to the confinement and guarding effect of the zeolite shell and the improvement in mass-transfer efficiency and active metal sites accessibility. The Pd-PdO interfaces as a new active site can provide active oxygen species to the first C-H cleavage of light alkanes. This work exemplifies a promising strategy to design other high-performance intra-crystalline mesoporous zeolite-confined metal/metal oxide catalysts for high-temperature industrial thermal catalysis.