ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Wenya Chen,Qingyun He,Ziyao He,Qin Wang,Jing Ding,Qiao Huang,Xiaojuan Liang,Zhaoping Chen,Weidong Xiang
In recent years, all-inorganic metal lead halide cesium perovskites (CsPbX3, X = Cl, Br, and I) have shown excellent luminescence performance in the field of wide color gamut backlight displays. However, Pb2+ in CsPbX3 easily leaks because of the unstable structure of CsPbX3, which seriously threatens human health. However, Mn-based metal halides (MHs) have unique environmentally friendly characteristics. In this work, Zn2+-doped Cs3MnBr5 MHs were successfully prepared, which exhibited highly efficient green emissions at 520–522 nm. Moreover, Cs3MnxZn(1–x)Br5 shows excellent stability at room temperature (25 °C) compared with Cs3MnBr5. More excitingly, when Cs3MnxZn(1–x)Br5 was encapsulated in a polystyrene (PS) polymer, Cs3MnxZn(1–x)Br5@PS showed better water, acid, daylight, and blue light stabilities. In addition, the backlight display device was designed based on different green–red ratios and thicknesses of Cs3MnxZn(1–x)Br5@K2SiF6:Mn4+@PS light conversion films, and the color gamut was over 109% of the NTSC 1953 standard, which is better than that of the reported WLED devices based on Mn-based MHs thus far. This work undoubtedly shows that Mn-based MHs have great application potential in wide color gamut backlight displays and provide a practicable route to fabricate nontoxic, low-cost, and high-performance liquid crystal displays.
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Journal of Physical Chemistry C
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2022
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IF 4.177
Zhaoxia Yang,Wenming Tian,Fengke Sun,Shengye Jin,Dongjiang You
One-dimensional (1D) perovskites are ideal broadband-emitting phosphors for white-emitting diode applications. Doping Mn2+ in 1D perovskites provides a new idea to tune the materials’ light-emitting properties. Here, we report an excitation-power-dependent dual-band emission from both self-trapped excitons (STEs) and Mn dopants in individual 1D Mn-doped DMEDAPbBr4 single crystals. By changing the excitation intensity, we realize a broad and continuous color tuning range between blue and orange. The temperature-dependent photoluminescence (PL) and transient spectroscopy measurements demonstrate that the tunable emission color is enabled by the competitive transfers of excitons to the STE state and Mn2+ ions. The Mn-doped 1D perovskites exhibit a high photostability by showing a continuous switch between blue and orange emissions during an uninterrupted operation time of 7.5 h. The high stability and emission-color switchable properties make the Mn-doped 1D perovskites special optically tunable PL materials for potential light-emitting applications.
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ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
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2022
·Vol. 648
·期 8
·e202100334
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IF 1.414
Yue-Yu Ma,Hong-Mei Pan,Dong-Yang Li,Shuang Wu,Zhihong Jing
Herein, by using different size of organic molecules as cation templates, we prepared four new two-dimensional (2D) lead halide perovskites, [PrPipz]PbBr 4 ( 1 ), [DMEDA]PbBr 4 ( 2 ), [TMEDA] 0.5 [DMA]PbCl 4 ( 3 ) and [TMA] 4 Pb 3 Cl 10 ( 4 ). Under the distinct structural directing effects of organic cations, compounds 1–4 present four different types of 2D inorganic layers. Remarkably, compounds 1 , 3 and 4 exhibit broadband blue emissions, while compound 2 exhibits broadband yellow emission upon the excitation of UV light at room temperature. This work paves a way to modulate the crystal structure and photoluminescent property of low-dimensional halide perovskite via structural modulation strategy from the molecular level.
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Gels
·
2022
·Vol. 8
·期 1
·52
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IF 4.432
Che Zhao,Chengju Sheng,Chao Zhou
Traditional antibacterial hydrogels have a broad-spectrum bactericidal effect and are widely used as wound dressings. However, the biological toxicity and drug resistance of these antibacterial hydrogels cannot meet the requirements of long-term clinical application. Imidazolium poly(ionic liquids) (PILs) are polymeric antibacterial agents exhibiting strong antibacterial properties, as they contain a strong positive charge. In this study, two imidazolium PILs, namely poly(N-butylimidazolium propiolic acid sodium) (PBP) and poly(N-(3,6-dioxaoctane) imidazolium propiolic acid sodium) (PDP), as high efficiency antibacterial agents, were synthesized by polycondensation reaction. Then, the PILs were compounded with polyethylene glycol (PEG) by a thiol-yne click reaction to prepare injectable antibacterial hydrogels. An in vitro assay showed that the injectable antibacterial hydrogels could not only quickly killEscherichia coli(E. coli) andStaphylococcus aureus(S. aureus), but also had low toxicity for human skin fibroblasts cells (HSFs) and human umbilical vein endothelial cells (HUVECs), respectively. Additionally, the lipopolysaccharide (LPS) inflammation model revealed that the injectable antibacterial hydrogels also had anti-inflammatory effects, which would be advantageous to accelerate wound healing.Keywords:antibacterial agents;imidazolium poly(ionic liquids);injectable hydrogels;anti-inflammatory
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PubMed
高影响因子
CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Chuang Ma,Lili Gao,Zhuo Xu,Xiaotong Li,Xin Song,Yucheng Liu,Tinghuan Yang,Haojin Li,Yachao Du,Guangtao Zhao,Xinmei Liu,Mercouri G. Kanatzidis,Shengzhong Frank Liu,Kui Zhao
Metal-halide perovskitoids with corner-, edge-, and face-sharing octahedra provide a fertile “playground” for structure modulation. With low defect density, low ion migration, and high intrinsic stability, two-dimensional (2D) perovskitoid single crystals are expected to be ideal materials for room-temperature semiconductor detectors (RTSDs) as high-energy radiation. However, there is no report yet on the use of 2D perovskitoid single crystals for X-ray detection, as well as on how the halide-modulated molecular assembly would affect their structure and properties. Herein, based on an amidino-based organic spacer, we successfully synthesized a novel family of centimeter-sized 2D perovskitoid single crystals, (3AP)PbX4 (3AP = 3-amidinopyridine, X = Cl, Br, and I). This is the first time that centimeter-sized 2D perovskitoid single crystals are demonstrated for X-ray photoresponse. Detailed investigations reveal a unique crystal packing with corner-sharing and edge-sharing octahedra of inorganic frameworks and 3AP cations lying between adjacent inorganic layers in a parallel and antisymmetric manner. Changing the halide from I to Br and Cl results in greater Pb–X–Pb angles and stronger hydrogen bonding in perovskitoids and therefore consequently a better elastic recovery under stress, a more efficient charge transport in the inorganic layer, and a lower ionic migration. By varying halide substitution, an efficient X-ray photoresponse is achieved with a sensitivity up to 791.8 μC Gyair–1 cm–2 for (3AP)PbCl4 and a low detection limit of 1.54 μGyair s–1. These results reveal that the large 2D perovskitoid single crystals provide a promising platform for high performance optoelectronics.
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ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Dong Li,Xiaoying Shang,Wentao Wu,Xiaoqi Li,Zhijin Xu,Lina Li,Maochun Hong,Xueyuan Chen,Junhua Luo
Visible–infrared dual-modal light harvesting is crucial for various optoelectronic devices, particularly for solar cells and photodetectors. Hybrid metal-halide perovskites are recently emerging for visible–infrared dual-modal photodetection owing to their prominent multiphoton absorption and carrier transport performances. However, they work relying on an applied external power source or complicated heterostructures. It is still a difficult task to realize visible–infrared dual-modal self-powered photoresponse induced by a bulk photovoltaic effect (BPVE) in a single material. In this work, we constructed a polar multilayered perovskite, (Br-BA)2(EA)2Pb3Br10 (BEP; EA+ = ethylammonium, and Br-BA+ = 4-brombutylammonium). Notably, the polar feature endows BEP with a BPVE. In addition, BEP presents a distinctive two-photon activity arising from the layered quantum-well structure. Benefitting from these striking characteristics, self-powered visible–infrared dual-modal photodetection is realized, and a direct self-powered detection of 800 nm light with a photocurrent of 2.1 nA cm–2 is achieved. This work will inspire the design of desired photoelectric materials with a BPVE for high-performance self-powered visible–infrared dual-modal photodetection.
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高影响因子
RSC Advances
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2022
·Vol. 12
·期 10
·6083-6092
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IF 4.036
Xia Chen,Yongjie Li,Qiang Fu,Hongyun Qin,Junnan Lv,Kun Yang,Qicheng Zhang,Hui Zhang,Ming Wang
The use of large amounts of deleterious solvents in the synthesis of metal–organic frameworks (MOFs) is one of the important factors limiting their application in industry. Herein, we present a detailed study of the synthesis of UiO-66, which was conducted with hydrobromic (HBr) acid as a modulator for the first time, at a high concentration of precursor solution (ZrCl4 and H2BDC, both 0.2 mol L−1). Powder crystals with atypical cuboctahedron structure were obtained which indicated that the HBr acid modulator played roles by competitive coordination and deprotonation modulation, thereby controlling the processes of nucleation and crystal growth. The properties of the obtained materials were systematically characterized and compared with those of materials synthesized with hydrofluoric (HF) acid and hydrochloric (HCl) acid modulators. Despite the high concentration of defectivity, the UiO-66 material synthesized with the HBr acid additive has the characteristics of larger specific surface area, excellent thermal stability and higher porosity in the structure. Besides that, the present protocol has the advantages of high reaction mass efficiency (RME), and feasibility of scalable synthesis, providing a facile and sustainable route to diverse Zr-based MOFs.
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Advanced Healthcare Materials
·
2022
·Vol. 11
·期 12
·2200199
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IF 11.092
Maohua Chen,Jingjing Zhou,Pan Ran,Fangmei Lei,Jie Meng,Junwu Wei,Xiaohong Li
It is of paramount importance to develop novel approaches for combating bacterial resistance and the integration of different antibacterial mechanisms is essential to achieve synergistic bactericidal efficiency while reducing the associated side effects. Herein, amphiphilic antimicrobial copolymers derived from poly- l -lysine (PLL), black phosphorus quantum dots (BPQDs) as near-infrared (NIR) sensitizer, and S-nitrosocysteamine (SNO) as nitric oxide (NO) donor, are assembled into PELI@BPQD-SNO nanoparticles through electrostatic interactions. Amphiphilic copolymers with isopentanyl grafts on PLL at a ratio of 50% achieve an optimal balance between antibacterial activity and hemolysis rate. Photothermal effect of BPQDs leads to NIR-responsive release of NO and the combination with amphiphilic copolymers mutually enhances long-term inhibition of bacterial growth. In an S. aureus -infected subcutaneous abscess model, the bactericidal rate of PELI@BPQD-SNO/NIR treatment reaches nearly 99.6%, which is significantly higher than those without NO release (38%) or amphiphilic copolymers (24%) or NIR irradiation (17%). PELI@BPQD-SNO/NIR treatment shows full recovery of infected wounds, efficient retardation of inflammatory cells, and reconstruction of blood vessels similar to those of healthy skin. Therefore, the electrostatic assembly demonstrates a promising strategy to deliver charged therapeutic agents and the photoactivated release of NO and amphiphilic copolymers achieves synergistic antibacterial efficacy without using any antibiotics.
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高影响因子
CRYSTENGCOMM
·
2022
·Vol. 24
·期 11
·2100-2106
·
IF 3.756
Song-Tao Dong,Zhuang Fu,Miaocheng Yu,Jia-Ling Jiang,Xiaoyun Jin,Yu-Hang Guo,Lei Wang,Ya-Mei Zhang
Self-powered photoelectric devices as a new type of sensor without an external power source have a great potential advantage in the next generation of portable and wearable personal devices. The design of those devices is normally based on three kinds of strategies: a p–n junction, the Schottky junction and ferroelectric polarization. Here, a novel solution based on ion migration induced self-powered photodetectors was explored. In this work, high quality halide perovskite FAPbBr3 crystals were grown by an inverse temperature crystallization (ITC) method. An irreversible ion migration was intentionally created using a symmetrically structured Au/FAPbBr3/Au device. The resulting built-in electric field and energy band bending were proved using electrical measurements in the dark and under light. Finally, the response of the ion migration induced self-powered FAPbBr3 detector was investigated with the values of R (∼0.18 mA W−1) and EQE (∼0.055%) under light with a power density of 1 mW cm−2 and a wavelength of 397 nm. Our investigation demonstrates that ion migration, which is normally deemed a detrimental factor for device stability, can be intentionally used for self-powered photoelectric devices.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Lusheng Liang,Qiu Xiong,Zilong Zhang,Yaming Yu,Peng Gao
Defects can easily form at the surfaces and grain boundaries of solution-processed organic-inorganic halide perovskites films, leading to undesired non-radiative recombination and ion migration in the device. Consequently, this limits the performance of perovskite solar cells (PSCs). Herein, a new organic ammonium halide salt with cyano (-CN) functional group, 4-cyanobenzenaminium iodide (CNBAI), was developed to passivate the defects in the bulk of perovskite films. It was found that the CNBAI can improve the film morphology of the perovskite layer and passivate the various types of defects in the perovskite. On the one hand, the -CN group could bind with the under-coordinated Pb 2+ and form intermolecular halogen bonds with the iodide atom in perovskite, as illustrated by X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy measurements. On the other hand, CNBAI could fill the iodide vacancy with its own iodide ions. For the first time, we demonstrate experimentally that the -CN group can simultaneously interact with Pb 2+ and form CN … I halogen bond in the perovskite. In addition, the introduced CNBAI improved energy alignment between the perovskite and adjacent charge transport layers. Finally, the PSCs fabricated with CNBAI-based perovskite films achieved the best PCE of 22.4% with negligible hysteresis and displayed good long-term stability.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Xiran Lin,Tao Shen,Minghui Li,Jingwen Shaoyu,Wei Zhuang,Ming Li,Hong Xu,Chenjie Zhu,Hanjie Ying,Pingkai Ouyang
Effectively removing heavy metals from the wastewater using a green low-cost natural polymer-based adsorbent received a great deal of attention. In this study, natural γ-polyglutamic acid (γ-PGA) and ε-poly-L-lysine (ε-PL) functionalized lignin (DLGS and DLLS) were synthesized through demethylation/phenolation and amination to increase its intrinsic reactivity and adsorption sites, which were used to remove heavy metals from aqueous solutions. DLGS and DLLS were comprehensively characterized by 31 P, 2D HSQC NMR, and elemental analysis (EA). The adsorption property of DLGS and DLLS for Pb 2+ have been systematically investigated. The adsorption kinetics and isotherms were compliant with the pseudo-second-order model and Langmuir isotherm model, respectively. The maximum adsorption capacity of DLGS and DLLS for Pb 2+ was 275.9 and 231.8 mg g −1 at 298 K, respectively, which is higher than that of most of the lignin-based adsorbent reported. Furthermore, it is confirmed that DLGS and DLLS exhibit excellent selectivity for removing Pb 2+ through competitive adsorption experiments. Based on the Fourier transform infrared spectrum (FTIR) and X-ray photoelectron spectroscopy (XPS) and the density functional theory (DFT) calculations, the hydroxyl, carboxyl, amino, methoxyl, and dithiocarbamate groups are contributed to the binding with Pb 2+ , and density functional theory calculation further suggested dithiocarbamate and the carboxyl group are the primary active sites.
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高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Yang-Peng Lin,Xiao-Ying Huang,Ke-Zhao Du
Bromine is essential to scientific study and industrial application. However, the high toxicity, volatility and corrosivity of Br 2 increase the risk of leakage or explosion. Using solid materials to capture bromine gas can alleviate the leakage and explosion. Herein, X Br 3 ( X = Cs, C 8 H 20 N and C 16 H 36 N) polybromide compounds, were synthesized by the one-pot Br 2 -free solvothermal method. CsBr 3 can reversibly decompose and generate along with the release and capture of Br 2 gas, while Br 2 can be separated from aqueous solution in the form of Et 4 NBr 3 (Et = Ethyl) or Bu 4 NBr 3 (Bu = Butyl). CsBr 3 can release 42.89% Br 2 per molecular formula, which is the highest in reported crystalline materials so far. Bu 4 NBr can enrich Br 2 in water with approximately 73% yield through the hydrophilic-hydrophobic effect. Our study presents an alternative method for solidification and efficient recycle of Br 2 .
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