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

Xiaosha Guo; Xixi Di; Tian Tang; Yixuan Shi; Dong Liu; Wei Wang; Zhifeng Liu; Xiaohui Ji; Xianzhao Shao

doi:10.1016/j.jcis.2023.12.085

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

J Colloid Interface Sci. 2024 Mar 15:658:362-372. doi: 10.1016/j.jcis.2023.12.085. Epub 2023 Dec 16.

Authors

Xiaosha Guo¹, Xixi Di¹, Tian Tang¹, Yixuan Shi¹, Dong Liu¹, Wei Wang¹, Zhifeng Liu², Xiaohui Ji¹, Xianzhao Shao³

Affiliations

¹ Shaanxi Key Laboratory of Catalysis, School of Chemistry and Environment Science, Shaanxi University of Technology, Hanzhong 723001, PR China.
² Shaanxi Key Laboratory of Catalysis, School of Chemistry and Environment Science, Shaanxi University of Technology, Hanzhong 723001, PR China; State Key Laboratory of Qinba Bio-Resource and Ecological Environment, Shaanxi University of Technology, Hanzhong 723001, PR China.
³ Shaanxi Key Laboratory of Catalysis, School of Chemistry and Environment Science, Shaanxi University of Technology, Hanzhong 723001, PR China. Electronic address: xianzhaoshao@snut.edu.cn.

PMID: 38113545
DOI: 10.1016/j.jcis.2023.12.085

Abstract

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 (E_a) 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.

Keywords: Covalent organic frameworks; Formic acid dehydrogenation; Hexavalent chromium (Cr(VI)); PdAuIr alloys.