Design of Efficient, Hierarchical Porous Polymers Endowed with Tunable Structural Base Sites for Direct Catalytic Elimination of COS and H2S

Jinxing Mi; Fujian Liu; Wei Chen; Xiaoping Chen; Lijuan Shen; Yanning Cao; Chaktong Au; Kuan Huang; Anmin Zheng; Lilong Jiang

doi:10.1021/acsami.9b09149

Design of Efficient, Hierarchical Porous Polymers Endowed with Tunable Structural Base Sites for Direct Catalytic Elimination of COS and H₂S

ACS Appl Mater Interfaces. 2019 Aug 21;11(33):29950-29959. doi: 10.1021/acsami.9b09149. Epub 2019 Aug 8.

Authors

Jinxing Mi¹, Fujian Liu¹, Wei Chen², Xiaoping Chen¹, Lijuan Shen¹, Yanning Cao¹, Chaktong Au¹, Kuan Huang³, Anmin Zheng^{2

4}, Lilong Jiang¹

Affiliations

¹ National Engineering Research Center of Chemical Fertilizer Catalyst (NERC-CFC), School of Chemical Engineering , Fuzhou University , Gongye Street 523 , Fuzhou 350002 , China.
² National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics , Chinese Academy of Sciences , Wuhan 430071 , China.
³ Key Laboratory of Poyang Lake Environment and Resource Utilization of Ministry of Education, School of Resources Environmental and Chemical Engineering , Nanchang University , Nanchang 330031 , China.
⁴ School of Materials Science and Engineering , Zhengzhou University , Zhengzhou , Henan 450001 , P. R. China.

PMID: 31352779
DOI: 10.1021/acsami.9b09149

Abstract

Hydrogen sulfide (H₂S) is malodorous and highly toxic, and its selective removal from industrial feedstock is highly recommended for safety and environment protection. We report here a class of nitrogen-functionalized, hierarchical porous polymers (N-HPPs) synthesized from one-step alkylation-induced cross-linking without any involvement of templates. The as-engineered N-HPPs are large in BET surface area (792-1397 m²/g) and endowed with hierarchical porosity. The incorporated nitrogen species of N-HPPs act as structural base sites with properties that can be precisely controlled. By molecular simulation, the enhanced interactions between N-HPPs and H₂S were verified. The synthesized N-HPPs show superb capacities for H₂S adsorption (9.2 mmol/g at 0 °C, 1.0 bar) and display satisfactory IAST H₂S/N₂ and H₂S/CH₄ selectivity (88.3 and 119.6, respectively, at 0 °C). Catalyzed by the structural base sites located in the N-HPPs, the COS together with its derived H₂S can be effectively eliminated under mild conditions.

Keywords: DFT calculation; HS oxidation; HS selective capture; hierarchical porous polymers; structural base sites.