High-Throughput Screening Assisted Discovery of Robust Metal–Organic Frameworks for Efficient Ambient NO <sub>2</sub> Removal
Jianqing Wu, Shanshan Shang, Xuquan Liu, Jinpeng Zhang, Chao Yang, Fengliang Wang, Fengying Ma, Xinyu Chen, Gaozhou Liang, Haitao Zhou, Xiangwei Zou, Peirong Chen, Hongxia Xi, Qinfen Gu, ChongXiong Duan, Daiqi Ye
Abstract
Nitrogen dioxide (NO 2 ) is a hazardous air pollutant that poses severe threats to sustainable air pollution control, yet its efficient ambient capture remains a major challenge. Here, we integrate a NO 2 -specific high-throughput computational screening (HTCS) of over 15,000 metal–organic frameworks (MOFs) from the CoRE database with targeted experimental validation to identify robust aluminum-based MOFs for selective NO 2 capture. Guided by the physicochemical characteristics of NO 2 and synthetic feasibility principles, four optimized Al-MOFs, i.e., KMF-1, CAU-23, MIL-160, and MOF-303, incorporating distinct heteroatom functional sites (-NH, -S, -O, and -N-NH, respectively), were investigated to probe the structure–adsorption correlations. Among them, MOF-303 exhibited an exceptional dynamic NO 2 capacity of 5.31 mmol·g –1, surpassing most reported porous adsorbents. Spectroscopic analyses and DFT calculations revealed that synergistic dipole interactions and hydrogen bonding at unique -N-NH bifunctional sites governed adsorption behavior. Such site-specific interactions endowed MOF-303 with long-term stability and regenerability, also validating the physicochemical descriptor-guided screening rationale and confirming its reliability under realistic conditions. Together, these results connect theoretical prediction with experimental verification, establishing a transferable paradigm for targeted environmental remediation and next-generation materials screening.