Designing multivariate porphyrin-based metal-organic frameworks with Ni/Co dual-metal atom sites for cooperative NO2 capture and NO retention

Shanshan Shang, Chao Yang, Yuanmeng Tian, Zeyu Tao, Mallory Smith, Hongyan Zhang, Lin Zhang, Liangchun Li, Qinfen Gu, Hong Cai Zhou, Yong Sik Ok, Jin Shang

Research output: Contribution to journalArticlepeer-review

4 Citations (Scopus)

Abstract

Selective adsorption using porous materials is a promising approach to removing ambient nitrogen dioxide (NO2). However, the highly reactive nature of NO2 and the often-associated release of nitric oxide (NO) render a formidable challenge in developing effective and stable adsorbents. Here, we designed multivariate porphyrin-based metal–organic frameworks (MTV-PMOFs Al-PMOF(NixCoy)) featuring atomically dispersed Ni/Co dual-metal centers in the porphyrin ring as active adsorption sites, as robust adsorbents capable of synergistically boosting NO2 adsorption capability and retaining the evolved NO. The introduction of the Ni/Co dual-metal sites in MTV-PMOFs greatly enhanced the NOx adsorption performance. Under dry conditions, Al-PMOF(Ni1Co1) exhibited a NO2 adsorption capacity of 3.66 mmol/g (100 ppm NO2 in feed), among the highest under similar conditions, a high NO retention ability, and good regenrability (85%). Under wet conditions, its NO2 removal capacity was further elevated by more than 50% (5.65 mmol/g). Moreover, the Ni/Co ratio in MTV-PMOFs dictates a structure–property relationship between the released amount of NO and adsorbed capacity of NO2. Such a corporative NO2 and NO adsorption was for the first time established in MOFs. The material stability and potential economic value were also investigated to demonstrate the applicability of MTV-PMOFs as NO2 adsorbents. This work provides new perspectives for the development of adsorption-based technology for mitigating ambient NO2 pollution and managing other corrosive and toxic gases.

Original languageEnglish
Article number124080
JournalSeparation and Purification Technology
Volume320
DOIs
Publication statusPublished - 2023 Sept 1

Bibliographical note

Publisher Copyright:
© 2023 Elsevier B.V.

Keywords

  • Cooperative adsorption
  • Dual single-atom Ni/Co site
  • Multivariate MOFs
  • Nitrogen oxides removal
  • Synergistic effect

ASJC Scopus subject areas

  • Analytical Chemistry
  • Filtration and Separation

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