Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 11, Issue 33, Pages 29950-29959Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b09149
Keywords
hierarchical porous polymers; DFT calculation; structural base sites; H2S selective capture; H2S oxidation
Funding
- National Key Research and Development Program of China [2018YFA0209304]
- National Natural Science Foundation of China [21825801, 21573150]
- Natural Science Foundation of Zhejiang Province [LY15B030002]
- Program for Qishan Scholar of Fuzhou University [GXRC-18043]
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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 m(2)/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 degrees C, 1.0 bar) and display satisfactory LAST H2S/N-2 and H2S/CH4 selectivity (88.3 and 119.6, respectively, at 0 degrees 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.
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