1. Construction of novel Cu-based bimetal polycrystal@carbon catalyst prepared from bimetal HKUST-1 type MOFs (MOF-199s) for ultrafast reduction of 4-nitrophenol via interfacial synergistic catalysis.
- Author
-
Li, Junjie, Sun, Xiaodan, Subhan, Sidra, Gong, Wenxue, Li, Wenyuan, Sun, Wenqing, Zhang, Yuming, Lu, Mengting, Ji, Hongbing, Zhao, Zhongxing, and Zhao, Zhenxia
- Subjects
- *
LAMINATED metals , *ORBITAL hybridization , *CATALYSIS , *CATALYTIC activity , *METAL catalysts , *DIFFUSION - Abstract
[Display omitted] • Polycrystal C-HK(Cu/Ni) catalyst is derived from bimetal HKUST-1 via partial reduction. • Dispersed NiO/Cu/CuO on graphitic porous C engineers interfacial catalytic synergy. • Mesoporous C-HK(Cu/Ni) quickens adsorption and promotes catalytic activity for 4-NP. • C-HK(Cu/Ni) exhibits 3 ∼ 16 times higher catalytic activity for 4-NP reduction than current catalysts. • C-HK(Cu/Ni) possesses high stability and durability after six consecutive cycles. The novel Cu-based bimetal polycrystal@carbon (C-HK(Cu/M)) composites derived from metal (Ni, Zn and Co) in-situ substituted Cu-based HKUST-1 were successfully fabricated by partial reduction strategy and employed for the reduction of 4-nitrophenol (4-NP). Systematic characterization demonstrated that Ni showed stronger orbital hybridization with Cu than Zn and Co, thereby significantly improving the catalytic properties of the C-HK(Cu/Ni) composite. The presence of Ni in HKUST-1 efficiently inhibited the reduction of adjacent Cu clusters, leading to the generation of unique polycrystal NiO/Cu/CuO nanohybrids (2.4–8.0 nm) with high dispersion (Cu exposure reaching 88.5%). While, the MOF ligands were catalyzed by doping Ni into the conductive and porous carbons, and finally engineered interfacial synergistic catalysis for enhancing the kinetics and stability for the reduction of 4-NP. The porous support accelerated 4-NP diffusion and adsorption in the composite, and as a consequence, the surrounding polycrystal nanohybrids on conductive carbon were responsible for producing hydrogen reducing species for 4-NP reduction. Therefore, C-HK(Cu/Ni) exhibited ultrafast kinetics and turnover frequency (TOF) for 4-NP reduction, which were up to 179 and 14 times higher than parent C-HK(Cu), surpassing the current state-of-the-art noble metal catalysts. Moreover, the activity of C-HK(Cu/Ni) was evaluated for six consecutive runs with minimal loss, demonstrating the high reusability and practicability of the catalyst on an industrial scale. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF