ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Dongyang Shen,Zhenwei Ren,Qinyi Li,Chengzhao Luo,Wenlin Xia,Zhishuai Zheng,Wenchen Ma,Jie Li,Yu Chen
Quasi-two-dimensional (quasi-2D) perovskite has exhibited great potential to be an ideal luminescent material for perovskite light-emitting diodes (PeLEDs). However, the low-order phases (especially n = 1 phase) and the inevitable defects result in massive nonradiative recombination and poor emission efficiency. Herein, a multifunctional molecule of tetrabutylammonium dihydrogen phosphate (TDP) is introduced to simultaneously suppress the low-n phase, passivate the defects, and increase the exciton binding energy of the quasi-2D perovskite for massive radiative recombination and thus high emission efficiency. The multifunctional roles of TDP are realized by the synergistic effects of tetrabutylammonium cation and dihydrogen phosphate anion, both of which show strong interaction with the lead bromide octahedron of the perovskite. As a result, the TDP-incorporated perovskite films show a great enhancement of the emission efficiency with a remarkable increase in photoluminescence quantum yield (PLQY) from 34.6 to 96.9% at the wavelength of 522 nm. The strengthened radiative recombination promotes efficient emission efficiency with over 2.5-fold improvement in external quantum efficiency (EQE) and current efficiency (CE) from 3.27% and 10.83 cd A–1 to 9.25% and 28.35 cd A–1, respectively, as well as high brightness with over 37% enhancement from 12713 to 17536 cd m–2. Consequently, this work contributes to an efficient approach to employ a multifunctional molecule for highly emissive quasi-2D perovskites and enhanced quasi-2D PeLED performances.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Junfeng Yang,Yuyang Wu,Yanhui Dong,Hao Cui,Chenyang Shi,Hang Sun,Shengyan Yin
Herein, a ternary Bi@H-TiO 2 /B-C 3 N 4 type II heterostructure is successfully designed and prepared via metal Bi as cocatalyst for photocatalytic H 2 generation. As expected, under λ > 300 nm light, the highest photocatalytic hydrogen production rate (HPR) of Bi@H-TiO 2 /B-C 3 N 4 is up to 223.08 μmol g −1 h −1 . Excitingly, under visible light (λ > 400 nm), the highest HPR of Bi@H-TiO 2 /B-C 3 N 4 is increased to 18.84 μmol g −1 h −1 , which is about 67.3 times, 37.7 times and 6.8 times as high as that of H-TiO 2 , B-C 3 N 4 and H-TiO 2 /B-C 3 N 4 under the same conditions, respectively. Moreover, the electrochemical impedance spectroscopy and transient photocurrent tests manifest that the interface resistance of Bi@H-TiO 2 /B-C 3 N 4 composite decreases and the photocurrent density increases after loading metal Bi. These results indicate that loading metal Bi as cocatalyst (providing more electron trapping sites) is beneficial to improve photocatalytic activity in the type II heterostructure composite. And the electron transfer directions (B-C 3 N 4 → H-TiO 2 → Bi or B-C 3 N 4 → Bi) are proved by ultraviolet photoelectron spectroscopy test. Therefore, the Bi@H-TiO 2 /B-C 3 N 4 photocatalyst with strong visible light absorption is expected to be a promising candidate in photocatalytic fields under visible light.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
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2022
·Vol. 223
·期 14
·2200038
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IF 2.996
Qiang Fu,Jiaqiang Rui,Jiaojiao Fang,Yaru Ni,Liang Fang,Chunhua Lu,Zhongzi Xu
Due to low penetration ability of ultraviolet (UV) light, UV-induced free radical reactions of polymers are limited to the preparation of thin-layer materials such as coatings and inks. Although upconversion (UC) nanomaterials that can be excited by near-infrared (NIR) light and emit UV light which is used to achieve polymerization or curing of monomers or prepolymers, low quantum efficiency and high excitation threshold limit their applications. Here, triplet-triplet annihilation up-conversion luminescent (TTA-UCL) chromophores of platinum (II) octaethylporphyrin (PtOEP) and 9,10-diphenylanthracene (DPA) are used to realize TTA-UCL-assisted photoinitiated polymerization of butyl acrylate (BA) and ethoxylated trimethylolpropane triacrylate (ETPTA) as well as photo curing of polyurethane acrylates (PUA) using visible light at 520 nm. The effects of chromophores concentrations and incident light power density on double-bond conversion rate are investigated. The results show that a mediate TTA-UCL chromophore concentration of 0.02% is beneficial for polymerization of ETPTA- co -BA with thickness of 25 mm within 15 min. Satisfied adhesion of colored plastic substrates using PUA prepolymers can be achieved after irradiation for 30 s when chromophore concentration of 0.1% is used. TTA-UCL assisted photoinitiated reactions show great potential in engineering aspects including quick repair of leaking tubes and photocuring of adhesives underwater.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuwei Ma,Guangtong Hai,Juming Liu,Jinxiao Bao,Yan Li,Ge Wang
Ni-doped cadmium sulfide (CdS) nanospheres with nickel phosphide (Ni 2 P) loading (Ni 2 P@CdS-Ni) were successfully prepared via the two-step thermal treatment growth and chemical reduction method in this work. Firstly, the thermal treatment method was applied to introduce the Ni 2+ into the lattice of CdS and induce the Ni-precursor loaded on surface of the CdS intimately. Then, the Ni-precursor was reduced into Ni(OH) 2 by using the chemical reduction process. Furthermore, the Ni 2 P were loaded on the CdS via the second thermal phosphorization reaction. The loaded Ni 2 P would evidently accelerate the transfer of photo-generated electrons between CdS-Ni and Ni 2 P and meanwhile effectively decrease the charges recombination. Moreover, the results of UV–vis DR spectra and density functional theory (DFT) calculations confirmed that Ni cations doped in the lattice of CdS lead to a doping level at the bottom of the conduct band, which narrowed the bandgap. The work function indicated that doped Ni 2+ helps to enhance the migration and separation of the photo-induced charge. Based on the synergistic effects, 3.7% Ni 2 P@CdS-Ni-3 presented a relatively high hydrogen evolution rate of 176.6 mmol h −1 g −1 under visible light irradiation (λ ≥ 420 nm), which is 63 times of the common CdS.
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Signal Transduction and Targeted Therapy
·
2022
·Vol. 7
·期 1
·1-9
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IF 38.104
Cao Changyu,Zhang Tingbo,Yang Nan,Niu Xianghong,Zhou Zhaobo,Wang Jinlan,Yang Dongliang,Chen Peng,Zhong Liping,Dong Xiaochen,Zhao Yongxiang
The current feasibility of nanocatalysts in clinical anti-infection therapy, especially for drug-resistant bacteria infection is extremely restrained because of the insufficient reactive oxygen generation. Herein, a novel Ag/Bi 2 MoO 6 (Ag/BMO) nanozyme optimized by charge separation engineering with photoactivated sustainable peroxidase-mimicking activities and NIR-II photodynamic performance was synthesized by solvothermal reaction and photoreduction. The Ag/BMO nanozyme held satisfactory bactericidal performance against methicillin-resistant Staphylococcus aureus (MRSA) (~99.9%). The excellent antibacterial performance of Ag/BMO NPs was ascribed to the corporation of peroxidase-like activity, NIR-II photodynamic behavior, and acidity-enhanced release of Ag + . As revealed by theoretical calculations, the introduction of Ag to BMO made it easier to separate photo-triggered electron-hole pairs for ROS production. And the conduction and valence band potentials of Ag/BMO NPs were favorable for the reduction of O 2 to ·O 2 − . Under 1064 nm laser irradiation, the electron transfer to BMO was beneficial to the reversible change of Mo 5+ /Mo 6+ , further improving the peroxidase-like catalytic activity and NIR-II photodynamic performance based on the Russell mechanism. In vivo, the Ag/BMO NPs exhibited promising therapeutic effects towards MRSA-infected wounds. This study enriches the nanozyme research and proves that nanozymes can be rationally optimized by charge separation engineering strategy.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Xin Gao,Baodong Li,Shouwei Jian
The fabrication of visible-light-driven heterostructured photocatalysts has been regarded as a promising strategy to enhance the photocatalytic performance. Here, a wet chemical method was adopted to prepare step-scheme CeO 2 /CaIn 2 S 4 (CCIS) composites. The CeO 2 nanoparticles were deposited on the surface of CaIn 2 S 4 (CIS) to form a tight interface, namely, heterojunction , which was confirmed by the multiple characterization methods. The formed heterojunction between CeO 2 and CIS was advantageous to promoting the charge carrier separation and migration. The photocatalytic performance of the resulted CCIS composites were evaluated by the Cr(Ⅵ) reduction under visible light irradiation. The optimized CCIS-10 sample exhibited the highest photocatalytic Cr(Ⅵ) reduction activity with the efficiency of 95% within 105 min. The enhanced photocatalytic activity of CCIS was attributed to the construction of step-scheme heterojunction system, leading to the efficient charge separation and high redox potential . The proposed mechanism for the enhanced photocatalytic performance was fully discussed and confirmed. This work may provide a simple strategy to rationally design efficient photocatalyst for Cr(Ⅵ) removal.
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Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 12
·1647-1657
·
IF 8.683
Huanhuan Zhang,Lin Yang,Hao Chen,Wenqiang Ma,Rui Wang,Guozhong Cao
Lead-free metal halides have gained considerable attention due to their excellent optoelectronic properties; however, the direct synthesis of white light sources remains a challenge for developing high-performance white light-emitting diodes (WLEDs). Herein, we synthesized all-inorganic copper-based ternary halides using a microwave method. Through a strategy of controlling the amount of cuprous iodide (CuI), two highly efficient light emitters, blue-emissive Cs3Cu2I5 and yellow-emissive CsCu2I3, can be obtained. The large Stokes-shifted broadband emission with a relatively long radiative lifetime is ascribed to the self-trapped exciton (STE) formation. The unique negative thermal quenching suggests that carrier transfer from more deeply trapped states to shallowly trapped states is beneficial for enhancing the STE emission. Moreover, with an increased amount of CuI, the as-synthesized Cs3Cu2I5@CsCu2I3 composites exhibit a series of stable cold/warm white-light emissions. The bright WLEDs ranging from cold-white (12810 K) to pure-white (6109 K) and warm-white (4149 K) are displayed by placing the Cs3Cu2I5@CsCu2I3 composite directly onto a commercial ultraviolet chip (310 nm), and an ultra-high color-rendering index (CRI) of 92 is achieved. The results imply that highly emissive and color-tunable copper-based halide composites open the door to explore their potential applications in next-generation solid-state lightings.
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INORGANIC CHEMISTRY
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2022
·
IF 5.436
Xiaoxi Li,Weiwei Li,Mengling Xia,Chao Liu,Neng Li,Zuhao Shi,Yinsheng Xu,Xianghua Zhang
Lead-free double perovskites (DPs) have outstanding luminescent properties, which make them excellent candidates for wide use in optoelectronics. Herein, a solvent-free melting-crystallization technique, which can produce kilogram-scale DP microcrystals (DP-MCs) in one batch, is invented to synthesize the Cs2NaxAg1–xInCl6: Bi (x = 0, 0.2, 0.4, 0.6, 0.8, and 1) DP-MCs. The structure and composition analysis confirmed the products are pure Cs2NaxAg1–xInCl6 DP-MCs. Affected by Jahn–Teller distortion of AgCl6 octahedra, self-trapped excitons appear in the excited state, resulting in the broadband emission (400–850 nm) of Cs2Ag1–xNaxInCl6: Bi DP-MCs. The enhancement of the photoluminescence quantum yield can be realized by introducing Na+ to break the parity-forbidden transition in the Cs2AgInCl6 DP. Optimized Cs2Na0.4Ag0.6InCl6: Bi DP-MC phosphors combined with commercial blue and green phosphors were coated on ultraviolet chips (365 nm) to fabricate white light-emitting diodes (WLEDs) from warm white (2930 K) to cold white (6957 K). An ultrahigh color rendering index of 97.1 and a CCT of 5548 K as well as Commission Internationale de l’Eclairage color coordinates of (0.331, 0.339) have been demonstrated. This kilogram-scale synthesis technique could stimulate the industrial development of WLEDs for general lighting based on DP-MC phosphors.
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JOURNAL OF RARE EARTHS
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2022
·
IF 4.632
Yangyang Sheng,Liyan Ming,Lin Liu,Peng Lin,Junpeng Shi,Liang Song,Yun Zhang
In recent years, white persistent luminescence materials have received extensive attention due to the potential application of white light in the field of plant growth lighting. The white persistent luminescence materials synthesized by traditional methods either have strict requirements on the concentration of doped ions or cannot produce white light continuously and stably due to different decay rates of various emission centers, which limits their further application. In our work, we successfully synthesized a novel Li + -doped MgLuGaO 4 phosphor with stable white-light emission and long persistent luminescence. The broadband emission of MgLuGaO 4 :Li + is mainly located at 350 – 650 nm, which has no change at different decay time, showing stable white-light emission. The persistent luminescence intensity is increased by 3.8 times and the persistent luminescence time is extended from 24 h to more than 36 h by doping Li + ions. Stable white-light and long persistent luminescence emission make it promising to be used in plant growth lighting.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Yinglin Qiu,Zhipeng Gong,Lei Xu,Qiaocan Huang,Zunxian Yang,Bingqing Ye,Yuliang Ye,Zongyi Meng,Zhiwei Zeng,Zihong Shen,Wenbo Wu,Yuanqing Zhou,Zeqian Hong,Zhiming Cheng,Songwei Ye,Hongyi Hong,Qianting Lan,Fushan Li,Tailiang Guo,Sheng Xu
CdSe-based quantum dots (QDs) have increasingly become important QDs for emerging display material because of their suitable bandgap, controllable size, and high PLQY. However, there are still many problems with CdSe QD films, including severe fluorescence quenching and low conductivity. Herein, we replace the long insulated oleic acid ligand with the shorter thiol ligand to enhance the mobility of charge carriers. It was found that the QDs with octanethiol in a quantum dot light-emitting diode (QLED) exhibited higher conductivity and lower turn-on voltage. Moreover, the defects on the surface of the QD layer were effectively passivated by adding a thin layer of cesium carbonate, and the radiation recombination of the quantum dot light-emitting layer was also significantly improved. It was evident that the performance of the optimized QLED device was improved with a peak luminance of 166 300–294 500 cd/m2 and a peak current efficiency of 10–32 cd/A. Thus, the current work provides two ways to optimize QD films and proposes a method to improve the performance of QLEDs.
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OPTICAL MATERIALS
·
2022
·
IF 3.754
Zehao Hu,Ting Chen,Zhixiang Xie,Chunxian Guo,Weihui Jiang,Yuanhong Chen,Yanqiao Xu
Microwave organic phase preparation of AgInS 2 quantum dots (QDs) is extremely essential to the large-scale, green and efficient preparation of AgInS 2 QDs. Here, commercial glycerol is used as the microwave absorber to prepare AgInS 2 QDs in nonpolar organic solvent octadecene at reaction temperature range of 100–180 °C. The AgInS 2 QDs can be obtained within 15 min and exhibit tunable photoluminescent properties. After decorating by ZnS layer, the prepared AgInS 2 @ZnS core/shell QDs emitted a bright orange-yellow light under ultraviolet light irradiation, and its quantum yield increased from 13.66% to 33.10%. Moreover, it exhibited excellent spectral tunability among the range of 608.0 nm–549.8 nm with the molar ratios of Zn/AgIn changed from 0 to 3. Finally, a WLED was fabricated by combining AgInS 2 @ZnS QDs and Y 3 Al 5-x Ga x O 12 :Ce 3+ phosphors with a blue chip, the color rendering index (CRI), correlated color temperature (CCT), and luminous efficiency (LE) of the device was 87.6, 3361 K, and 58.83 lm/W, respectively, indicating the great application prospect in illumination. The research explores a novel avenue for the fast and efficient synthesis of I–III–VI semiconductor QDs in nonpolar solvent via microwave method.
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ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Hongwei Yang,Yayun Wu,Hefei Ruan,Feng Guo,Yuxin Liang,Gege Qin,Xiaolong Liu,Zhen Zhang,Jinghe Yuan,Xiaohong Fang
Stimulated emission depletion (STED) nanoscopy is an emerging super-resolution imaging platform for the study of the cellular structure. Developing suitable fluorescent probes of small size, good photostability, and easy functionalization is still in demand. Herein, we introduce a new type of surface-engineered gold nanoclusters (Au NCs) that are ultrasmall (1.7 nm) and ultrabright (QY = 60%) for STED bioimaging. A rigid shell formed by l-arginine (l-Arg) and 6-aza-2-thiothymine (ATT) on the Au NC surface enables not only its strong fluorescence in aqueous solution but also its easy chemical modification for specific biomolecule labeling. Au NCs show remarkable performance as STED nanoprobes, including high depletion efficiency, good photobleaching resistance, and low saturation intensity. Super-resolution imaging has been achieved with these Au NCs, and targeted nanoscopic imaging of cellular tubulin has been demonstrated. Moreover, the circular structure of lysosomes in live cells has been revealed. As a Au NC is also an ideal probe for electron microscopy, dual imaging of Aβ42 aggregates with the single labeling probe of Au NCs has been realized in correlative light and electron microscopy (CLEM). This work reports, for the first time, the application of Au NCs as a novel probe in STED and CLEM imaging. With their excellent properties, Au NCs show promising potential for nanoscale bioimaging.
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