作者
Yu Han,Wenyuan Huang,Meng He,Bing An,Yinlin Chen,Xue Han,Lan An,Meredydd Kippax‐Jones,Jiangnan Li,Yuhang Yang,Mark D. Frogley,Cheng Li,Danielle Crawshaw,Pascal Manuel,Svemir Rudić,Yongqiang Cheng,Ian P. Silverwood,Luke L. Daemen,Anibal J. Ramirez‐Cuesta,Sarah J. Day,Stephen P. Thompson,Ben F. Spencer,Marek Nikiel,Daniel Lee,Martin Schröder,Sihai Yang⧫
摘要
Abstract Capture of trace benzene is an important and challenging task. Metal–organic framework materials are promising sorbents for a variety of gases, but their limited capacity towards benzene at low concentration remains unresolved. Here we report the adsorption of trace benzene by decorating a structural defect in MIL-125-defect with single-atom metal centres to afford MIL-125-X (X = Mn, Fe, Co, Ni, Cu, Zn; MIL-125, Ti 8 O 8 (OH) 4 (BDC) 6 where H 2 BDC is 1,4-benzenedicarboxylic acid). At 298 K, MIL-125-Zn exhibits a benzene uptake of 7.63 mmol g −1 at 1.2 mbar and 5.33 mmol g −1 at 0.12 mbar, and breakthrough experiments confirm the removal of trace benzene (from 5 to <0.5 ppm) from air (up to 111,000 min g −1 of metal–organic framework), even after exposure to moisture. The binding of benzene to the defect and open Zn(II) sites at low pressure has been visualized by diffraction, scattering and spectroscopy. This work highlights the importance of fine-tuning pore chemistry for designing adsorbents for the removal of air pollutants.