Pd nanoparticles on a dual acid-functionalized porous polymer for direct synthesis of H2O2: Contribution by enhanced H2 storage capacity

被引:15
|
作者
Puthiaraj, Pillaiyar [1 ]
Yu, Kwangsun [1 ]
Ahn, Wha-Seung [1 ]
Chung, Young-Min [2 ]
机构
[1] Inha Univ, Dept Chem & Chem Engn, Incheon 402751, South Korea
[2] Kunsan Natl Univ, Dept Nano & Chem Engn, 558 Daehak Ro, Kunsan 54150, Jeollabuk Do, South Korea
基金
新加坡国家研究基金会;
关键词
Direct synthesis of H2O2; Hyper-crosslinked porous polymer; Hydrogen storage; Oxygen storage; Solid acid support; MICROPOROUS ORGANIC POLYMERS; HYDROGEN-PEROXIDE SYNTHESIS; PALLADIUM CATALYSTS; GAS-STORAGE; OXYGEN; O-2; NANOCRYSTALS; ORIGIN; PHASE; FILMS;
D O I
10.1016/j.jiec.2019.09.028
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Direct synthesis of H2O2 from H-2 and O-2 can avoid the energy and environmental problems of current multi-step anthraquinone oxidation process by enabling high atom utilization and generating only a water by-product. However, the direct process suffers a low H2O2 yield, and it is challenging to suppress the unfavorable side-reactions in the absence of corrosive additives under the restriction of explosion limits. In this study, an efficient new catalyst was prepared by immobilizing Pd nanoparticles (NPs) on an acidic hyper-crosslinked porous polymer (HCPP). The Pd catalyst supported on HCPP functionalized with both carboxylic and sulfonic acids (Pd/c-s-HCPP) achieved as high as 3130 mmol H2O2/g Pd.h with 82% selectivity to H2O2, which corresponded to one of the best catalysts reported so far. Pd/c-s-HCPP showed superior catalytic performance when compared with ones by Pd NPs supported on unfunctionalized HCPP (Pd/HCPP), or sulfonated resin (Pd/SO3H-resin). Extensive characterizations and H-2 adsorption measurements indicated that the c-s-HCPP provided (i) selective adsorption sites for Pd precursors, (ii) acted as an efficient H-2 reservoir in the proximity of the small Pd NPs formed, and (iii) imparts solid acidity to enhance H2O2 selectivity, which offered a new direction in the catalyst design for the direct synthesis of H2O2. (C) 2019 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.
引用
收藏
页码:375 / 384
页数:10
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