Search

Low-dimensional organic–inorganic metal halides have shown great application potential and new opportunities for use in solid-state lighting due to their excellent optical and electronic properties. However, the most studied hybrid compounds contain lead, which limits their application environments. The preparation of organic–inorganic metal halides with high luminous efficiency, long-term stability, and a lead-free composition for environmental protection has become an important goal for the design of materials. Here, novel Sb3+-doped indium-based metal halides, (CH3NH3)4InCl6·Cl, have been designed and synthesized via a simple mechanical ball milling method; in the lead-free zero-dimensional (0D) halide (CH3NH3)4InCl6·Cl, isolated [InCl6]3− octahedra are separated by methylamine cations. Under UV excitation, the bulk-phase powder exhibits broadband orange-yellow emission peaking at 607 nm with a full width at half-maximum of ∼160 nm upon incorporating Sb3+ into the (CH3NH3)4InCl6·Cl matrix. The photoluminescence quantum yield (PLQY) of Sb3+-doped (CH3NH3)4InCl6·Cl is as high as 67.72%. The effects of the Sb3+-doping concentration on the crystal structure and optical characteristic have been investigated. The indirect band gap characteristics of (CH3NH3)4InCl6·Cl were demonstrated via density functional theory (DFT) calculations, and the relatively wide band gaps of 3.83 eV and 2.99 eV of (CH3NH3)4InCl6·Cl and (CH3NH3)4ClInCl6:Sb3+ were experimentally determined. These experimental results suggest that the as-prepared Sb3+-doped (CH3NH3)4InCl6·Cl has potential applications in solid-state lighting devices. [ABSTRACT FROM AUTHOR]

Peroxymonosulfate (PMS) addition into a MnO x system is generally believed to be an effective way for expediting organics removal. Whereas in this work, we found single MnO x with a micro-current got an even better oxidation performance comparing that with PMS addition. The carbon paper electrodeposited by amorphous MnO x (AMO) was used as cathode, and the micro-current (55 µA/cm2) increased the methylene blue (MB) degradation rate by 6.1 times through enhancing the AMO oxidative ability in acidic media. At the same pH, the MB degradation rate in AMO (AMO-MC) system was close to that in AMO system with PMS addition (AMO-MC-PMS). More importantly, the MB mineralization in AMO-MC was about 1.6 times higher than that in AMO-MC-PMS. Similar phenomena were also investigated when using tetracycline (TC) as organic pollutant. The mechanisms of AMO-MC and AMO-MC-PMS for MB removal were comprehensively studied and compared. It was found that the micro-current prompted the Mn valence converting from high to low. Conversely, the PMS addition hindered this converting and impeded the direct oxidation of AMO. The GC-MS analysis indicated that the presence of PMS induced the formation of sulfoxide-containing intermediates (SCIs) which were difficult to be further degraded and resulted in the suppression of MB mineralization. Density functional theory (DFT) calculation indicated that the intermediates from AMO-MC were more facile to be attacked in an electrophilic way and adsorbed on the cathode than the SCIs. It proposed that the AMO with micro-current had the potential to remove organics efficiently, and blind PMS addition should be avoided. [Display omitted] • Amorphous MnO x (AMO) system can remove MB efficiently with the aid of a cathodic micro-current. • The micro-current can improve the activity of AMO system better than peroxymonosulfate (PMS). • Single AMO system got mineralization of 30% higher than the AMO-MC-PMS system. • Refractory intermediates were generated in the AMO-MC-PMS system. • PMS may not always play a positive role and blind addition should be avoided. [ABSTRACT FROM AUTHOR]