Li Jinjian, Chen Yuting, Ke Tian, Jin Yuanyuan, Fan Rongrong, Xu Guihong, Yang Liu, Zhang Zhiguo, Bao Zongbi, Ren Qilong, Yang Qiwei
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, Zhejiang, China.
Institute of Zhejiang University-Quzhou, Quzhou, Zhejiang, China.
Nat Commun. 2025 Jan 13;16(1):632. doi: 10.1038/s41467-025-56031-5.
Physisorption presents a promising alternative to cryogenic distillation for capturing the most potent greenhouse gas, SF, but existing adsorbents face challenges in meeting diverse chemical and engineering concerns. Herein, with insights into in-pore chemistry and industrial process design, we report a systematic investigation that constructed two low-cost composites pellets (Al(fum)@2%HPC and Al(fum)@5%Kaolin) coupled with an innovative two-stage Vacuum Temperature Swing Adsorption (VTSA) process for the ultra-efficient recovery of low-concentration SF from N. Record-high selectivities (> 2×10) and SF dynamic capacities (~ 2.7 mmol/g) were achieved, while exceptional SF productivities (~ 58.7 L/kg), yields (~ 96.8%), and recyclability (~ 1000 cycles) were demonstrated in fixed-bed adsorption-desorption experiments under mild regeneration conditions. 2D solid-state NMR/in-situ FTIR, DFT-D binding/diffusion simulation analyses revealed the multi-site binding mode and the ultra-fast diffusion of SF within the channels. The proposed VTSA processes successfully met the dual stringent requirements of both environmental protection and electricity equipment operation: the SF recovery of 99.91% accompanied with a SF purity/working capacity of 99.91%/2.1 mmol/g, which significantly outperformed the industrial employed adsorbent zeolite 13X and showed only 18.7% the energy consumption of the cryogenic distillation.
物理吸附是一种很有前景的替代低温蒸馏的方法，用于捕获最具强效的温室气体六氟化硫（SF₆），但现有的吸附剂在满足各种化学和工程要求方面面临挑战。在此，通过对孔内化学和工业过程设计的深入了解，我们报告了一项系统研究，该研究构建了两种低成本复合颗粒（Al(fum)@2%HPC和Al(fum)@5%高岭土），并结合创新的两级真空变温吸附（VTSA）工艺，用于从氮气中高效回收低浓度的六氟化硫。实现了创纪录的高选择性（>2×10）和六氟化硫动态容量（2.7 mmol/g），同时在温和再生条件下的固定床吸附-解吸实验中展示了优异的六氟化硫生产率（58.7 L/kg）、产率（96.8%）和可回收性（1000次循环）。二维固态核磁共振/原位傅里叶变换红外光谱、密度泛函理论-色散（DFT-D）结合/扩散模拟分析揭示了六氟化硫在通道内的多位点结合模式和超快扩散。所提出的VTSA工艺成功满足了环境保护和电力设备运行的双重严格要求：六氟化硫回收率为99.91%，同时六氟化硫纯度/工作容量为99.91%/2.1 mmol/g，显著优于工业上使用的吸附剂13X沸石，并且仅显示出低温蒸馏能耗的18.7%。
