Benchmark C2H2/CO2 Separation in an Ultramicroporous Metal-Organic Framework via Copper(I)-Alkynyl Chemistry.
Abstrak
Separation of acetylene from carbon dioxide remains a daunting challenge because of their very similar molecular sizes and physical properties. We herein report the first example of using copper(I)-alkynyl chemistry within an ultramicroporous MOF (CuI@UiO-66-(COOH)2) to achieve ultrahigh C2H2/CO2 separation selectivity. The anchored Cu(I) ions on the pore surfaces can specifically and strongly interact with C2H2 molecule through copper(I)-alkynyl π-complexation and thus rapidly adsorb large amount of C2H2 at low-pressure region, while effectively reduce CO2 uptake due to the small pore sizes. This material thus exhibits the record high C2H2/CO2 selectivity of 185 at ambient conditions, significantly higher than the previous benchmark ZJU-74a (36.5) and ATC-Cu (53.6). Theoretical calculations reveal that the unique π-complexation between Cu(I) and C2H2 mainly contributes to the ultrastrong C2H2 binding affinity and record selectivity. The exceptional separation performance was evidenced by breakthrough experiments for C2H2/CO2 gas mixtures. This work suggests a new perspective to functionalizing MOFs with copper(I)-alkynyl chemistry for highly selective separation of C2H2 over CO2.
Topik & Kata Kunci
Penulis (13)
Ling Zhang
Ke Jiang
Lifeng Yang
Libo Li
Enlai Hu
Ling Yang
Kai Shao
Huabin Xing
Yuanjing Cui
Yu Yang
Bin Li
Banglin Chen
G. Qian
Akses Cepat
- Tahun Terbit
- 2021
- Bahasa
- en
- Total Sitasi
- 168×
- Sumber Database
- Semantic Scholar
- DOI
- 10.1002/anie.202102810
- Akses
- Open Access ✓