RSC Advances
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2022
·Vol. 12
·期 8
·4615-4623
·
IF 4.036
Hao Lu,Xieming Xu,Guiqing Feng,Baoping Sun,Shuaihua Wang,Shaofan Wu
Radiographic screens are widely used in high energy physics, national defense, aviation, radiodynamic therapy and medical imaging due to their scintillation materials that can transform high-energy particles or rays into ultraviolet (UV) visible light or other signals. In recent years, lanthanide doped fluoride nanocrystals (NCs) have attracted much attention due to their excellent optical properties and stability. In this work, multiple lanthanide-doped LiLuF4 nanocrystal scintillation materials were synthesized by thermal decomposition. Among them, Tb-doped LiLuF4 nanocrystals have high X-ray sensitivity and low detection limit (36.31 nGy s−1), which is much lower than the requirement of medical imaging dose rate. After the irradiation of 42.29 mGy s−1 X-ray for 1 hour, the intensity of radioluminescence basically remained unchanged. Based on the good properties of our nanocrystals, we further prepared the flexible film of nanocomposites with epoxy resin. This kind of uniform, large area, high loaded flexible film exhibits excellent performance in X-ray imaging with a spatial resolution greater than 20 line pairs per millimeter (LP/mm).
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Nanoscale
·
2022
·Vol. 14
·期 11
·4263-4270
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IF 8.307
Kunlun Liu,Jun Zhao,Gencai Pan,Yaxian Zhu,Wenwu You,Huafang Zhang,Huiping Gao,Yanli Mao
Lead halide perovskite quantum dots (PQDs) are extremely unstable when exposed to oxygen, water and heat, especially red CsPbBrxI3−x (x = 0, 0.5, 1.2) PQDs. This seriously hinders their practical application. Here, red CsPbBrxI3−x (x = 0, 0.5, 1.2) PQDs have been successfully encapsulated in porous CaF2:Ce,Tb hierarchical nanospheres (HNSs), which not only greatly improved the stability of PQDs, benefitting from the protection of the CaF2 shell, but also maintained the high photoluminescence quantum yield (PLQY) of PQDs, benefitting from the sensitization of Tb3+ ions. More importantly, porous CaF2:Ce,Tb nanoarchitectures can prevent aggregation quenching and anion exchange of PQDs. Therefore, the CaF2:Ce,Tb&CsPbBrxI3−x (x = 0, 0.5, 1.2) composite powder can have high PLQY comparable to that of the PQD powder. In view of this, CaF2:Ce,Tb&CsPbBr1.2I1.8 composite based red light-emitting diodes (LEDs) are prepared, and they are very suitable as a supplementary light source for plant lighting. Furthermore, white LEDs are also prepared by coating the CaF2:Ce,Tb&CsPbBr3 and CaF2:Ce,Tb&CsPbBr1.2I1.8 composite on a 450 nm chip. The optimum luminous efficiency is 61.2 lm W−1, and the color rendering index is 91, which are comparable to the current highest values. This shows that the composite composed of PQDs has great potential in LED lighting.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 15
·5849-5855
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IF 8.067
Qiang Zhang,Minghui Jiang,Guijun Yan,Yaqing Feng,Bao Zhang
All-inorganic CsPbBr3 perovskite quantum dots (CsPbBr3 QDs) have become one of the most promising materials in the field of optoelectronics. However, the poor stability and low photoluminescence quantum yield (PLQY) of CsPbBr3 QDs hinder their further applications. Herein, fluorinated aromatic ammonium bromide (fluorophenethyl ammonium bromide, FPEABr) is introduced in the synthesis of CsPbBr3 QDs. The influence of the fluorination position (ortho, meta, and para) at the benzene ring on the optical properties and stability of CsPbBr3 is systematically evaluated. The results indicate that the short fluorinated aromatic alkyl ammonium chain has been successfully adsorbed onto the surface of CsPbBr3 QDs, and the bromine vacancy defects have been significantly reduced. Eventually, stable CsPbBr3 QDs with a high PLQY (>90%) are achieved with the use of pFPEABr. Furthermore, the short chains of the ligand improved the carrier transport in the CsPbBr3 QD film, and thus the surface treatment increases the maximum luminance of the corresponding perovskite quantum dot light-emitting diodes (QLEDs) from 531 to 1278 cd m−2. The surface ligand engineering strategy involving the FPEABr ligand, in particular pFPEABr, actually provides a new direction for the future development of high-performance QLEDs.
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 7
·2101944
·
IF 6.389
Qianli Xing,Wei Yan,Chuangyu Wei,Zuoxu Xiao,Zhicheng Jin,Xue Liu,Jianwei Ren,Yanli Chen,Xiyou Li
The multidimensional PtZn quasi-cubic nanodendrites (PtZn-ND) with tremendous amounts of defectively coarse branches, having both highly active high-index facets and short-range (100) and (110) terraces resisted to sulfate, are synthesized via facile oil phase route at first time. The growth process is found to start from Pt nano-cuboid seeds, then PtZn nanoclovers which are formed from epitaxial growth, and then the flower-like PtZn crystals and finally the novel PtZn-ND. The formation mechanism of PtZn-ND, in particular the effects of hexadecyltrimethyammonium bromide (CTAB) and oleic acid (OA) on the morphology, crystal shape and exposure lattice facets, have been comparatively and systematically studied. And it turns out that CTAB mainly controls depositing directions, while OA mainly controls the crystal shape/size. The combination effect results in unique PtZn-ND structures. The novel PtZn-ND also displays superior catalytic performance and anti-sulfate poisoning ability. In particular, the mass activity (MA) and specific activity (SA) are 5.72 and 7.55 times higher than those of commercial Pt/C, and still 2.91 and 5.09 times higher after accelerated durability tests in 0.5 m H 2 SO 4 for oxygen reduction reaction.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 14
·8303-8310
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IF 3.945
Ruirui Wu,Shunfa Gong,Lifang Wu,Hailong Yu,Qiuju Han,Wenzhi Wu
Benefiting from the easily adjustable optical properties of perovskite, CsPbBr3 nanocrystals (NCs) are considered to show their advantages in the field of display. Here, we report that a selective laser irradiation is used to induce CsPbBr3 nanostructural reshaping and then yielding a morphological change. Under 360 or 405 nm laser irradiation, a hierarchical crystal growth process occurs for the fabricated CsPbBr3 nanoplatelets (NPLs), which are first arranged in a side-by-side manner and reshaped into nanorods (NRs), and then NRs are arranged in the face-to-face manner to reshape into NCs. The entire process is monitored optically and microscopically, which showed that crystal growth relies on seeking a dynamic balance between heat dissipation and accumulation under laser irradiation. The heat on NPLs generated by laser irradiation dissipated with a low dissipation rate and thus led to temperature rising and lattice breaking, which turned out to be the driving force for the crystal growth in CsPbBr3 NPLs. This feasible laser irradiation-assisted method provides for crystal growth a reliable and scalable route toward the preparation of perovskite functional materials.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Pengfei Ma,Yixin Hou,Yifan Zheng,Jun Su,Luying Li,Nishuang Liu,Zhi Zhang,Yanan Ma,Yihua Gao
All-inorganic perovskite quantum dots (QDs) are very promising materials for their potential applications in water-related photoluminescence due to their sensitive properties to water. This work initiatively attempts to absorb Cs 4 PbBr 6 QDs into a super-hydrophobic polydivinylbenzene (PDB) porous framework. Under the protection of PDB, the non-luminescent Cs 4 PbBr 6 and luminescent CsPbBr 3 transform reversibly by alternate water treatment (excess or small amount) and removal of water. The extraction of CsBr by water and reinsertion of CsBr by evaporation from/into the QDs make up a reversible phase transformation process. The super-hydrophobic porous structure of PDB not only provides the confined space for dissolved CsBr but also inhibits the overflow of trapped CsBr, thereby reducing the adverse impact of excess water on reversible hydrochromism. This work provided a new perspective to understand the phase conversion between Cs 4 PbBr 6 and CsPbBr 3 . Furthermore, the Cs 4 PbBr 6 @PDB in waterborne luminescent inks by screen printing opens a way in the field of anti-counterfeiting owing to the excellent stability of encryption and decryption.
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ACS Nano
·
2022
·
IF 18.027
Nuoya Li,Xujian Chen,Jin Wang,Xinmeng Liang,Lintao Ma,Xiaolang Jing,De-Li Chen,Zhengquan Li
Utilizing sunlight to convert CO2 into chemical fuels could simultaneously address the greenhouse effect and fossil fuel crisis. ZnSe nanocrystals are promising candidates for photocatalysis because of their low toxicity and excellent photoelectric properties. However, pristine ZnSe generally has low catalytic activities due to serious charge recombination and the lack of efficient catalytic sites for CO2 reduction. Herein, a ZnSe nanorods–CsSnCl3 perovskite (ZnSe–CsSnCl3) type II heterojunction composite is designed and prepared for photocatalytic CO2 reduction. The ZnSe–CsSnCl3 type II heterojunction composite exhibits enhanced photocatalytic activity for CO2 reduction with respect to pristine ZnSe nanorods. The experimental characterizations and theoretical calculations reveal that the efficient charge separation and lowered free energy of CO2 reduction facilitate the CO2 conversion on the ZnSe–CsSnCl3 heterojunction composite. This work presents a type II heterojunction composite photocatalyst based on ecofriendly metal chalcogenides and metal halide perovskites. Our study has also promoted the understanding of the CO2 reduction mechanisms on perovskite nanocrystals, which could be valuable for the development of metal halide perovskite photocatalysts.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Zhenyu Wang,Xinyu Shen,Chengyuan Tang,Xin Li,Junhua Hu,Jinyang Zhu,William W. Yu,Hongwei Song,Xue Bai
Oleylamine and oleic acid are common organic capping ligands used in the hot injection preparation of perovskite quantum dots (QDs). Their labile nature is responsible for the poor colloidal stability and conductivity that affect the performance of perovskite QD light-emitting diodes (LEDs). We introduced 4-trifluoro phenethylammonium iodide (CF3PEAI) directly in the synthesis and found that CF3PEAI efficiently modified the I– vacancy defects on the QD surface and partially substituted the surface capping ligand oleylamine. The strong electron pulling ability of F in CF3PEAI results in a more positive −NH3+ terminal compared to that of PEAI, which promotes tight bonding of CF3PEAI on the surface of CsPbI3 QDs. As a result, we achieved bright QDs with a photoluminescence quantum yield of 92% and efficient red LEDs. The maximal luminance was improved to 4550 cd m–2 for 685 nm red light, which was nearly 4.6-fold of the LEDs with plain CsPbI3 QDs. Additionally, the peak external quantum efficiency reached 12.5%.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jinling Yang,Xiang Li,Jianrong Zhang,Yang Zhou,Yuanyuan Wang
All-inorganic metal nanocrystals (NCs) offer an ideal platform for atomically precise surface design and show improved electrocatalytic activity compared to conventional NCs capped with organic ligands. Here, we show the possibility of obtaining colloidal all-inorganic Au NCs directly from magic-size clusters (MSCs) with the assistance of inorganic molecules, NOBF4 or Na2S2O8. The unique advantages of NOBF4 or Na2S2O8 as both oxidizing agents and stripping ligands are taken to tune the surface state of Au25(PET)18–TOA+ MSCs and assemble them to form either positively or negatively charged all-inorganic Au NCs. We show that positively charged all-inorganic Au NCs can be further modified with different functional groups, which provide the possibility to meet the target requirements. We found that the negatively charged NCs exhibit improved faradaic efficiency (FE = 92%) for the reduction of CO2 to CO at −0.369 V (vs RHE) and a 5-fold increase in current density compared to organic-capped Au NCs (FE = 67%). In addition, we extended this approach to other MSCs and formed all-inorganic metal NCs with different compositions and morphologies. The use of simple inorganic ligands to induce the conversion from MSCs to metal NCs enriches the current solution process of synthesizing all-inorganic NCs and can open up more opportunities for designing colloidal nanocrystal catalysts.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Shirong Qin,Hanlun Xu,Mengjuan Liu,Nasir Ali,Yansong Chen,Sihan Zhao,Huizhen Wu
Two-dimensional (2D) photodetectors based on semiconducting transitional metal chalcogenides (TMDs) have attracted much attention because of its unique mechanical and opto-electronic properties which can be integrated into nanoscale-sized opto-electronic devices and complex circuits. However, the photodetection range of 2D TMDs materials based detectors are generally limited within the visible range due to its intrinsic relatively large band-gap. In addition, 2D TMDs materials also suffers from weak light absorption inherited from their atomically thin layers, resulting in a photoresponsivity that can be further improved. Herein, by combining 2D MoS 2 with zero-dimensional (0D) PbSe quantum dots (QDs) and Au nanocrystals (NCs), a novel 2D-0D photodetector (i.e., MoS 2 /PbSe@Au) is fabricated. Our MoS 2 /PbSe@Au photodetector exploits the 2D MoS 2 as the conduction channels and PbSe@Au NCs as light sensitizer, which promote the absorption of the entire device and enable appreciable photodetection extending to the near-infrared (NIR). Prominently, the mixed-dimensional photodetector exhibits high responsivity of 1.22 A/W and detectivity of 1.56*10 9 Jones (cm·Hz 1/2 ·W −1 ) at NIR (e.g., 1064 nm) compared with the MoS 2 photodetector with PbSe QDs only, which are ascribed to the more efficient two-step charge transfer process between PbSe and MoS 2 with the presence of Au NCs. We further identify the new carrier multiplication mechanism when comparing the photoresponse of our photodetectors at 405 nm and 635 nm. We found the extremely high EQE of MoS 2 /PbSe@Au photodetector at the wavelength of 405 nm (268.1%) could be ascribed to the synergism of carrier multiplication (CM) in PbSe QDs and the photo-gating effect induced by Au nanoparticles. Our study demonstrates that the novel mixed-dimensional photodetectors based on CVD-grown MoS 2 may provide a new route for designing and realizing high-performance optoelectronic devices with harvesting merits of hybrid nanomaterials.
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Chemistry-An Asian Journal
·
2022
·Vol. 17
·期 6
·e202101343
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IF 4.839
Yao Xiao,Shuai Hou,Zhao Jin,Changpeng Liu,Junjie Ge,Wei Xing
Graphical The HER performance of non-precious metal catalysts Ni 2 P was greatly improved by coating with a ultrathin N-doped carbon shell. The relationship between the carbon shell structure and HER performance of Ni 2 P was studied in detail. Developing non-precious metal catalysts towards hydrogen evolution reaction (HER) is of both high scientific and technical importance for the widespread application of water electrolysis. Herein, Ni 2 P nanoparticles coated with a ultrathin N-doped carbon shell were prepared as a highly efficient HER catalyst. Ni 2 P@CN exhibits both enhanced catalytic activity and durability in comparison with the carbon-supported Ni 2 P counterpart, and represents 100% faradaic yield for HER in an acidic medium. The improved charge transfer of N-doped graphitic carbon shells contributes to the increase in activity. Meanwhile, the carbon shells suppress the aggregation and exfoliation of Ni 2 P nanoparticles. As a result, the synergistic role of the N-doped carbon layer confers the Ni 2 P cores with boosted activity and stability.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Wei Shen,Ye Yu,Wenzhu Zhang,Yanfeng Chen,Jianbin Zhang,Liu Yang,Jingting Feng,Gang Cheng,Lihui Liu,Shufen Chen
Exploitation of next-generation blue light-emitting diodes (LEDs) is the foundation of the revolution in lighting and display devices. Development of high-performance blue perovskite LEDs is still challenging. Herein, 4-aminobenzenesulfonic acid (SA) is introduced to passivate blue CsPbBr3 nanoplates (NPLs), reducing the ionic migration via a more stable Pb2+–SO3–– formation, and the trap state density of films shows a 50% reduction. The inevitable Br– vacancy defects after the multistep washing process can be suppressed by a suitable MABr treatment, which can boost the external quantum efficiency (EQE) performance. It should be noted that the coverage of NPL films is another key factor to realize reproducible pure blue electroluminescence (EL). Therefore, we proposed an alternate droplet/spin coating method to improve the coverage and thickness of NPL layer to prevent hole transport layer emission and increase the reproducibility of LED performance and spectra. Furthermore, we designed hole transport layers to decrease the hole transport barrier and improve the energy-level alignment. According to SA passivation, MABr treatment, alternate droplet/spin coating method, and device structure optimization, a CsPbBr3 NPL-based pure blue (0.138, 0.046) LED with 3.18% maximum EQE can be achieved, and the half-lifetime of EL can be enhanced 1.71 times as compared to that of the counterpart LED without SA. Both performance and stability of pure blue NPL LEDs can be greatly improved via ligand passivation, alternate droplet/spin coating method, and device structure optimization, which is a trend to promote the development of pure blue perovskite LEDs in future.
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