Water-resistant organic-inorganic hybrid perovskite quantum dots activated by the electron-deficient d-orbital of platinum atoms for nitrogen fixation

Due to their special physicochemical properties, organic-inorganic hybrid perovskite quantum dots (OIP QDs) are ideal and potential catalysts for the nitrogen reduction reaction (NRR). However, the OIP QD-based NRR is limited by poor water resistance, competitive suppression by the hydrogen evolutio...

Full description

Saved in:
Bibliographic Details
Published in:Nanoscale 2022-08, Vol.14 (3), p.178-1792
Main Authors: Gao, Yixuan, Su, Xiao, Wei, Juanjuan, Sun, Jianghui, Zhang, Min, Tan, Hongwei, Zhang, Jiangwei, Ouyang, Jin, Na, Na
Format: Article
Language:English
Subjects:
Ammonia
Aqueous solutions
Catalysts
Chemical reduction
Doping
Electron transfer
Encapsulation
Heterojunctions
Hydrogen evolution reactions
Lead oxides
Nitrogenation
Perovskites
Quantum dots
Water resistance
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:Due to their special physicochemical properties, organic-inorganic hybrid perovskite quantum dots (OIP QDs) are ideal and potential catalysts for the nitrogen reduction reaction (NRR). However, the OIP QD-based NRR is limited by poor water resistance, competitive suppression by the hydrogen evolution reaction, and inefficient active sites on the catalyst surfaces. Herein, to ensure an efficient NRR in aqueous solution, a water-resistant polycarbonate-part-encapsulated heterojunction of Zn,Pt IV co-doped PbO-MAPbBr 3 (Pt IV /Zn/PbO/PC-Zn/MAPbBr 3 ) is prepared through one-step electrospray-based microdroplet synthesis. Confirmed by both experimental and theoretical examinations, PbO is exposed on the PC-part-encapsulated surface to construct a Type I heterojunction. This heterojunction is further improved by synergistic co-doping with Pt IV to facilitate efficient electron transfer for efficient photocatalysis of the NRR. Due to the active sites of the d-orbital electron-deficient Pt atoms (exhibiting a lower reaction energy barrier and highly selective N 2 adsorption), the ammonia yield rate is 40 times higher than that without doping. This work initiates and develops on the application of OIP QDs in the NRR. Water-resistant polycarbonate-part-encapsulated heterojunction of Zn,Pt IV co-doped PbO-MAPbBr 3 was prepared by ESI-microdroplet synthesis. Electron deficient sites of Pt IV lowered d-band center to inhibit H adsorption, enhancing N 2 affinity for NRR.
ISSN:2040-3364
2040-3372
DOI:10.1039/d2nr02662g