期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 4, 页码 5887-5896出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c22986
关键词
hierarchy; MOFs; carbon composites; host-guest interaction; hydrogenation catalysis
资金
- National Natural Science Foundation of China [21706199, 51861135313]
- Rapid Response Bilateral Collaborative Funding of the Sino-German Centre for Research Promotion [C-0046]
- Guangdong Province International Scientific and Technological Cooperation Projects [2020A0505100036]
- International Science and Technology Cooperation Program of China [2015DFE52870]
- Young Top-notch Talent Cultivation Program of Hubei Province
This study demonstrates the synthesis of a urchin-like superstructure consisting of sulfur-doped carbon and HfO2 through a solvent-mediated strategy. The synthesized Pd@SC/HfO2 composite exhibits excellent catalytic activity and stability for water-phase hydrodeoxygenation and hydrogenation reactions.
Carbon materials with hierarchical morphologies, pores, and compositions have attracted extraordinary attention due to their unique structural advantages and widespread applications. However, their control-lable synthesis remains a grand challenge. Herein, a solvent-mediated strategy was demonstrated for the preparation of an urchin-like super-structure via modulating the hydrothermal condition (acetic acid/water ratio) of metal-organic frameworks (MOFs). The direct pyrolysis of a hierarchical NUS-6 precursor produced a well-defined carbon-based composite consisting of sulfur-doped carbon (SC) and HfO2 with an urchin-like morphology and micro-/mesoporosity, while the doped S sites and oxygen vacancies of HfO2 can help to anchor and activate Pd nanoparticles (NPs) through the strong host-guest interaction, which was further confirmed by the calculated results of the binding energy and differential charge density through density functional theory (DFT). The synthesized Pd@SC/HfO2 composite exhibited extremely high catalytic activity and stability toward the water-phase hydrodeoxygenation of vanillin (conversion >99%, selectivity >99%), as well as good universality for the hydrogenation of a series of unsaturated hydrocarbons in an aqueous system. Remarkably, the catalytic activity and structural stability of Pd@SC/HfO2 were largely maintained even after successive 10 cycles.
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