Nitrogen activation and surface charge regulation for enhancing the visible-light-driven N2 fixation over MoS2/UiO-66(SH)2

Qingqing Li; Yingzhang Shi; Zhiwen Wang; Cheng Liu; Jinhong Bi; Jimmy C Yu; Ling Wu

doi:10.1016/j.jcis.2023.08.178

Nitrogen activation and surface charge regulation for enhancing the visible-light-driven N₂ fixation over MoS₂/UiO-66(SH)₂

J Colloid Interface Sci. 2023 Dec 15;652(Pt B):1568-1577. doi: 10.1016/j.jcis.2023.08.178. Epub 2023 Aug 30.

Authors

Qingqing Li¹, Yingzhang Shi¹, Zhiwen Wang¹, Cheng Liu¹, Jinhong Bi², Jimmy C Yu³, Ling Wu⁴

Affiliations

¹ State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian 350116, Fuzhou, China.
² State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian 350116, Fuzhou, China; Department of Environmental Science and Engineering, Fuzhou University, Minhou, Fujian 350108, China. Electronic address: bijinhong@fzu.edu.cn.
³ State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian 350116, Fuzhou, China; Department of Chemistry, The Chinese University of Hong Kong, Shatin, New Territories, Hong Kong (China).
⁴ State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian 350116, Fuzhou, China. Electronic address: wuling@fzu.edu.cn.

PMID: 37660613
DOI: 10.1016/j.jcis.2023.08.178

Abstract

A series of dehydrated MoS₂/UiO-66(SH)₂ (MS/UiS) composites has been prepared as photocatalysts for N₂ fixation. Typically, 10% MS/UiS exhibits the best performance with an NH₄⁺ yield rate of 54.08 μmol∙g^-1∙h^-1. ¹⁵N isotope test confirmed that the sample 10% MS/UiS was most effective for reducing N₂ to ammonia. Such enhanced activity was due to the presence of abundant unsaturated Zr and Mo sites which would synergistically promote the adsorption and activation of N₂. The photogenerated electrons would transfer to the unsaturated Zr-O clusters while part of photogenerated electrons at the interface migrate to MS via Mo^VI-O interactions between MS and UiS. These two electron transfer pathways effectively promote the separation of photogenerated carriers. The activated N₂ is reduced to ammonia by the synergistic effect of protonated hydrogen and photogenerated electrons. Finally, a possible N₂ fixation mechanism is proposed which emphasizes the significant roles of nitrogen activation and interface interaction in composites photocatalyst for improving photocatalytic performance.

Keywords: Interface interaction; MoS(2) ultrathin nanosheets; Nitrogen activation; Photocatalytic nitrogen fixation; UiO-66(SH)(2).