烟气脱硫
化学工程
核化学
废物管理
化学
有机化学
工程类
作者
Shengnan Lu,Yonghou Xiao,Qidong Zhao,Wenkai Zhao,Gaohong He
标识
DOI:10.1016/j.seppur.2022.122665
摘要
• A micro-mesoporous CPO-27-Ni was successfully synthesized by soft template method. • Defective CPO-27-Ni possesses a uniform distribution of mesopores. • Rational defects expose more active sites and facilitate adsorbates diffusion. • DMA18-C-0.5 shows excellent adsorption desulfurization and regeneration performance. Deep desulfurization from fuel has gradually become a research hotspot with enhancing requirements of environmental protection. CPO-27-Ni was considered as one of promising adsorbents towards adsorption desulfurization by virtue of its prodigious high pore volume and high specific surface area. However, the dominant microporous channels in traditional CPO-27-Ni hinder the diffusion of thiophene sulfide and its derivatives with relatively large molecular size, which limits its desulfurization efficiency. Herein, we proposed a strategy to reasonably construct defective CPO-27-Ni with micro-mesoporous structure using N, N-dimethyloctadecylamine (DMA18) as a template, aim at improving the diffusion efficiency by introducing meso-pores. Different amounts of DMA18 were introduced to synthesize defective CPO-27-Ni (DMA18-C- X ) by solvothermal method, and DMA18-C-0.5 (the mole ratio of added DMA18 to Ni 2+ was 0.5) exhibited a satisfactory desulfurization performance. The dynamic breakthrough adsorption capacities of dibenzothiophene, benzothiophene and thiophene over the DMA18-C-0.5 were remarkably promoted, which were as high 3.79, 6.45 and 9.29 times as the traditional CPO-27-Ni, respectively. The crystal structure of CPO-27-Ni was not altered after adding template agent DMA18, while a uniform distribution of mesopores appeared. The largest mesopore attained a size of 2.8 nm, which effectively promoted the full exposure of more unsaturated Ni 2+ active sites and enhanced the interaction between Ni 2+ active sites and sulfides, resulting in strengthened adsorption desulfurization performance. This method of introducing proper defects to construct mesopores in MOFs provides some useful references for preparing high-efficiency desulfurization adsorbents.
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