TY - JOUR
T1 - Generalized water-processed metal chalcogenide complexes: Synthesis and applications
AU - Xia, Zhe
AU - Zhong, Jie
AU - Leng, Meiying
AU - Hu, Long
AU - Xue, Ding-Jiang
AU - Yang, Bo
AU - Zhou, Ying
AU - Liu, Xinsheng
AU - Qin, Sikai
AU - Cheng, Yibing
AU - Tang, Jiang
PY - 2015
Y1 - 2015
N2 - Metal chalcogenide complexes (MCCs) have attracted considerable attention recently due to their high solubility in polar solvents, low-temperature decomposition to metal chalcogenide films, and service as ligands for colloidal nanocrystals (NCs). However, most of the MCCs were typically synthesized in the highly toxic and explosive hydrazine (denoted as hydrazine-MCCs), severely restricting the wide applications of MCCs. Here we present a versatile and environmentally benign water-based solution method for the preparation of various MCCs (denoted as water- MCCs) through directly dissolving a series of bulk V2VI3 chalcogenides (V = Sb, As and VI = S, Se, Te) in water with the presence of (NH4)2S at room temperature and ambient atmosphere. We further show that such water-MCCs can be readily processed into corresponding semiconducting thin films upon mild thermal treatment and then be extended to fabricate compositionally controlled semiconductor alloys with tunable band gaps (i.e., Sb2(S1−x,Sex)3, 0 ≤ x ≤ 1) through simple control of substrate temperature. Furthermore, we present that our water-MCCs, especially for Sb4S7 2−, can be utilized to serve as ligands for in-situ-synthesized water-based PbS quantum dots (QDs), achieving a homogeneous and stable aqueous QDs solution without needing further conventional secondary ligand exchange. Our study provides a general strategy for the synthesis of various MCCs using water as safer and more environmentally friendly solvent alternative to hydrazine, thus greatly enhancingthe wide applications of MCCs in solution-processed inorganic semiconductors.
AB - Metal chalcogenide complexes (MCCs) have attracted considerable attention recently due to their high solubility in polar solvents, low-temperature decomposition to metal chalcogenide films, and service as ligands for colloidal nanocrystals (NCs). However, most of the MCCs were typically synthesized in the highly toxic and explosive hydrazine (denoted as hydrazine-MCCs), severely restricting the wide applications of MCCs. Here we present a versatile and environmentally benign water-based solution method for the preparation of various MCCs (denoted as water- MCCs) through directly dissolving a series of bulk V2VI3 chalcogenides (V = Sb, As and VI = S, Se, Te) in water with the presence of (NH4)2S at room temperature and ambient atmosphere. We further show that such water-MCCs can be readily processed into corresponding semiconducting thin films upon mild thermal treatment and then be extended to fabricate compositionally controlled semiconductor alloys with tunable band gaps (i.e., Sb2(S1−x,Sex)3, 0 ≤ x ≤ 1) through simple control of substrate temperature. Furthermore, we present that our water-MCCs, especially for Sb4S7 2−, can be utilized to serve as ligands for in-situ-synthesized water-based PbS quantum dots (QDs), achieving a homogeneous and stable aqueous QDs solution without needing further conventional secondary ligand exchange. Our study provides a general strategy for the synthesis of various MCCs using water as safer and more environmentally friendly solvent alternative to hydrazine, thus greatly enhancingthe wide applications of MCCs in solution-processed inorganic semiconductors.
UR - http://pubs.acs.org.ezproxy.lib.monash.edu.au/doi/pdf/10.1021/acs.chemmater.5b03614
U2 - 10.1021/acs.chemmater.5b03614
DO - 10.1021/acs.chemmater.5b03614
M3 - Article
SN - 0897-4756
VL - 27
SP - 8048
EP - 8057
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 23
ER -