Amine-functionalized Schiff base covalent organic frameworks supported PdAuIr nanoparticles as high-performance catalysts for formic acid dehydrogenation and hexavalent chromium reduction

脱氢 催化作用 甲酸 化学 六价铬 纳米颗粒 胺气处理 共价键 席夫碱 催化效率 金属有机骨架 无机化学 高分子化学 有机化学 材料科学 纳米技术 吸附
作者
Xiaosha Guo,Xixi Di,Tian Tang,Yixuan Shi,Dong Liu,Wei Wang,Zhifeng Liu,Xiaohui Ji,Xianzhao Shao
出处
期刊:Journal of Colloid and Interface Science [Elsevier BV]
卷期号:658: 362-372 被引量:12
标识
DOI:10.1016/j.jcis.2023.12.085
摘要

Formic acid (FA) holds significant potential as a liquid hydrogen storage medium. However, it is important to improve the reaction rates and extend the practical applications of FA dehydrogenation and Cr(VI) reduction through the development of efficient heterogeneous catalysts. This study reports the synthesis of a uniformly dispersed PdAuIr nanoparticles (NPs) catalyst loaded with amine groups covalent organic frameworks (COFs). The alloyed NPs demonstrated exceptional effectiveness in FA dehydrogenation rate and Cr(VI) reduction. The initial turnover of frequency (TOF) value for FA dehydrogenation without additives was 9970 h−1 at 298 K, the apparent activation energy (Ea) was 30.3 kJ/mol and the rate constant (k) for Cr(VI) reduction was 0.742 min−1. Additionally, it showcased the ability to undergo recycling up to six times with minimal degradation in performance. The results indicate that its remarkable catalytic performance can be attributed primarily to the favorable mass transfer attributes of the aminated COFs supports, the strong metal-support interaction (SMSI), and the synergistic effects among the metals. This study offers a novel perspective on the advancement of efficient and durable heterogeneous catalysts with diverse capabilities, thereby making significant contributions to the fields of energy and environmental preservation.
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