ACS Applied Nano Materials
·
2023
·
IF 5.9
Hao Hao,Hui-Ling Hu,Yi Liu,Feng-Lei Jiang
In this work, CdSe/ZnS core/shell quantum dots (QDs) were synthesized. Dilution of the as-synthesized QDs would lead to instability with photoluminescence (PL) quenching. It was found that the addition of tertiary phosphine and alkylthiol could recover the PL intensity of diluted QDs and make these QDs stable. Specifically, the recovery efficiency of tertiary phosphine was stronger than that of alkylthiol. Trioctylphosphine (TOP) and octanethiol (OT) were chosen as the representative ligands, respectively. Isothermal titration calorimetry (ITC) demonstrated that interactions between both TOP/OT and QDs were exothermic and spontaneous. The interaction between TOP and QDs was mainly driven by van der Waals forces due to the branched structure. This interaction had a negative entropy change, while the interaction between OT and QDs had a positive entropy change. There were about ∼12 TOP molecules and ∼17 OT molecules bound to a QD particle. The binding constants of TOP/OT to QDs were 1.6 × 103 and 12.8 × 103 M–1, respectively. The reaction rate between TOP and QDs was fast, and the addition of OT could slow the reaction rate constant from 0.081 to 0.024 min–1. PL decay indicated that TOP and OT could increase the radiative recombination of excitons. Furthermore, both TOP and OT could greatly improve the brightness of the QD films, which was a prerequisite for the efficient improvement of quantum dot light-emitting diodes. This work explicitly investigated the dilution process of QDs, explored the methods for keeping diluted QDs stable and bright, and highlighted the importance of surface ligands.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Xiao-Hang He,Yu-Lin Yin,Ge Tang,Yi Liu,Feng-Lei Jiang
Trioctylphosphine (TOP) is widely used in the synthetic process of colloidal quantum dots (QDs). However, its role has not been fully elucidated yet. Herein, the role of TOP was revealed by kinetic studies with spectroscopic methods. It was found that TOP suppressed the growth rate but increased the solubility; hence, it modulated QDs by controlling both. The extent of impact from TOP varied in the length of acids that was used in QD synthesis. In general, the impact from TOP to QDs synthesized by short acids was mainly the suppressing effect because shorter aliphatic acids had a higher diffusion rate, and they might suffer from TOP a lot. On the contrary, longer aliphatic acids diffused intrinsically slowly, so the reaction rate was rarely influenced by TOP, but the solubility was supposed to be considered at this time. This difference also led to the optimal amount of TOP used in the synthesis. These results pointed out that both the growth rate and solubility were time-dependent and should be considered to obtain high-quality QDs. In addition, the initial nucleation procedure was also seemingly suppressed by TOP. This work not only shed light on the underlying role of TOP and convinced the controllable synthesis of QDs but also provided a method to investigate the behavior of QD growth by considering several conditions synergistically and dynamically.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2021
·Vol. 33
·期 5
·055602
·
IF 3.874
Xinsu Zhang,Hao Lv,Weishuo Xing,Yanjun Li,Chong Geng,Shu Xu
Significant advance was realized on the economic synthesis of InP quantum dots (QDs) by using aminophosphines as phosphorus precursor. However, the low reaction activity and thermal degradation of aminophosphines bring severe difficulty for growth control of InP QDs. Here, we employed trioctylphosphine (TOP) as a surfactant to accelerate the growth of the InP QDs. The reaction mechanism study reveals that the TOP could form a reactive complex with indium halides that effectively accelerates the formation of InP monomer and reduces the demand for reaction temperature. On this basis, the effect of reaction temperature, precursors, and zinc halide additives on the growth of the TOP-InP QDs was explored. This strategy alleviates the difficulty in growth control of InP QDs and also benefits to the synthesis of luminescent InP/ZnS core–shell QDs within visible regime. A white-light emitting diode device was fabricated with the InP/ZnS QDs that demonstrates their application potential in light-emitting devices.
研究领域:
材料科学
·
化学工程
·
纳米技术
✓ 已验证
DOI
高影响因子
Materials
·
2025
·Vol. 18
·期 7
·1518
·
IF 3.2
Chengqi Liu,Zahir Abdalla,Xiaoqian Wang,Manrui Liu,Yanhui Jiao,Zisheng Tang,Qi Zhang,Yong Liu
Metal halide perovskite nanorods hold great promise for optoelectronic applications. However, they tend to undergo phase transitions due to the instability of the crystal phase under environmental conditions, leading to a rapid decline in the fluorescence efficiency. Here, we report a method in which trioctylphosphine (TOP) directly serves as both the surface ligand and solvent to synthesize highly stable α-CsPbI3nanorods (NRs). This approach produces monodisperse α-phase NRs with controlled sizes (1 μm and 150 nm in length, and an aspect ratio of 10:1), as confirmed by high-resolution transmission electron microscopy (TEM) and X-ray diffraction. The optimized NRs exhibit a high photoluminescence quantum yield of around 80%, as well as excellent environmental stability; after 15 days of storage, the photoluminescence quantum yield (PLQY) retention is 90%. Transient absorption spectroscopy shows that the carrier lifetime is extended to 23.95 ns and 27.86 ns, attributed to the dual role of TOP in defect passivation and hydrolysis suppression. This work provides a scalable paradigm for stabilizing metastable perovskite nanostructures through rational ligand selection, paving the way for durable perovskite-based optoelectronics.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Yurou Shao,Yangyang Jiang,Dong Wang,Benshuai Guo,Jingyan Zhao,Zhibin Zhou,Jianqiu Chen,Ruixin Guo,Yuntao Lei,Lili Jin
Capturing and recovering carbon dioxide (CO 2 ) from the combustion of fossil fuels is an effective way to reduce carbon emissions, as CO 2 is not only a threat to the environment but also an important C1 feedstock. In the current work, a series of trioctylphosphine oxide (TOPO)-based azole deep eutectic solvents (DESs) have been synthesized for the efficient absorption of CO 2 . The solid–liquid phase diagrams of the DESs were projected using the prediction data from COSMO-RS, and the experimental melting temperature was found to be lower than that of the prediction. These DESs exhibit satisfactory physical properties, including low viscosities (20–60 mPa·s) and high thermal decomposition temperatures (up to 192.5 °C). Furthermore, the CO 2 uptake process was carried out at 35 °C and 0.1 MPa, and the results demonstrated that the CO 2 uptake capacity was positively influenced by hydrogen bond donors (HBDs), mole fraction of HBDs, temperatures, and humidity. Among the DESs, TOPO-imidazole (1:1) was notable for its high absorption capacity of 0.062 mol CO 2 /mol DES, as well as its excellent recyclability. There was no discernible decline in the CO 2 uptake capacity after four absorption–desorption cycles. In this work, NMR and FT-IR investigations indicated the physical absorption mechanism of this system. The designed DESs have the potential to be effective absorbents for efficient reversible CO 2 capture.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Ranran Hu,Fengkai He,Ruixue Hou,Zhenghui Wu,Xiangtong Zhang,Huaibin Shen
Low-toxicity InP-based quantum dots (QDs) exhibit potential for replacing Cd/Pb-containing QDs in the visible and near-infrared regions. Despite advancements, further improvement relies on synthesizing homogeneous InP QDs to achieve a high color purity. In a commonly employed two-step “seed-mediated” synthetic approach, we demonstrate the high sensitivity of InP seed sizes and size distribution to the quantities of trioctylphosphine (TOP) and tris(trimethylsilyl)phosphine [(TMS)3P], attributed to the process of “self-focusing of size distribution” and enhanced reactivity of In-oleate through coordination with TOP. During growth, the processes of size focusing and defocusing are modulated by the accumulation of oleic acid and TOP molecules, as well as the amount of (TMS)3P in the growth precursor, which may relate to the dissolution process of InP magic size clusters. Through precise control, the best valley/depth ratio of InP QDs was 0.52 at the first absorption peak at 571 nm, resulting in luminescence with a full width at half-maximum of 35 at 620 nm with an absolute photoluminescence quantum yield around 90% after heteroepitaxial growth with ZnSe and ZnS shells.
研究领域:
材料科学
·
纳米技术
·
光学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yan Zhao,Beili Pang,Shaojie Zheng,Xiangyu Kong,Mengyuan Zhao,Hongzhou Dong,Liyan Yu,Lifeng Dong
This study investigates the application of trioctylphosphine oxide (TOPO) and triphenylphosphine oxide (TPPO) as an additive to enhance the performance of all-inorganic CsPbBr3 perovskite solar cells (PSCs). The addition of TOPO and TPPO passivates surface defects, increases grain size, and reduces surface trap states, leading to better light absorption and accelerated carrier transport. These modifications lead to an optimized energy level distribution, resulting in a significant increase in power conversion efficiency from 5.14 to 9.21% with TOPO and from 5.14% to 7.28% with TPPO. Furthermore, the long alkyl chains in TOPO provide effective isolation from air and water, significantly enhancing device stability for over 2400 h without packaging. The findings demonstrate that oxygen phosphine additives with long alkane chains are more effective in improving PSCs than those with aromatic hydrocarbons, offering new insights for the use of passivators in perovskite solar cells.
研究领域:
材料科学
·
光伏技术
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry C
·
2021
·Vol. 9
·期 8
·2873-2881
·
IF 7.393
Dan Li,Yixuan Liu,Shuangshuang Shi,Yanjun Li,Chong Geng,Shu Xu
Lead halide perovskite nanocrystals (PNCs) are emerging as promising light-conversion materials for light-emitting diode (LED) display applications. However, the practical application of PNCs is hindered by their labile surface and dynamic ionic ligand binding. Here, we report a post-synthetic surface passivation strategy to stabilize the CsPbBr3 PNCs by zinc methacrylate (ZnMA) and trioctylphosphine oxide (TOPO) co-passivation. Surface analyses reveal that the ZnMA stabilizes the PNCs by replacing the surface ammonium ligands, and TOPO further coordinates to the ZnMA to provide a high photoluminescence quantum yield (PLQY) of the PNCs. Moreover, the ZnMA capping on the PNC surface could participate in the polymerization of MMA to form a crosslinked polymer shell around the PNCs. The resultant PNCs–PMMA film presents a PLQY of 74% and maintains a constant PL intensity under continuous UV irradiation in air, while the PNCs–PMMA film made of classical PNCs quickly degrades. The prepared PNCs–PMMA film was tested as the light down-conversion layer in LED backlighting and presented photostability comparable to classical CdSe/ZnS NCs–PMMA under continuous illumination. This surface passivation strategy avoids the use of ionic ligands for the surface passivation of PNCs in polymer matrices, and we expect related surface chemistry to promote the performance enhancement of diverse PNCs–polymer composites for LEDs and other optoelectronic applications.
研究领域:
材料科学
·
纳米技术
·
光电
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry C
·
2020
·Vol. 8
·期 29
·9861-9866
·
IF 7.059
Hanwen Zhu,Yu Tian,Supeng Yang,Yang Shen,Enze Xu,Jianxin Tang,Yang Jiang
Surface engineering and doping are common methods used to enhance the emission properties of perovskite quantum dot light-emitting diodes (PeQLEDs), and more effective methods need to be developed. Here, we introduce a spin-coated trioctylphosphine oxide (TOPO) layer that spontaneously forms concave–convex micro grid structures between the hole-transport layer (TFB) and the CsPbBr3 quantum dot (QD) layer. The unique concave–convex micro grid structures change with the concentration of TOPO solution and the type of solvent, which may be caused by the surface tension. Spectral measurements reveal that the TOPO layer passivates the surface defects between the perovskite QDs. The finite-difference-time-domain (FDTD) method proves that these concave–convex micro grid structures also increase light output from the quantum dot light-emitting diodes (QLEDs). As a result, green perovskite QD light emitting diodes (LEDs) of 514 nm with a Luminous Efficiency (LE) of 3975 cd m−2, Current Efficiency (CE) of 18.8 cd A−1 and External Quantum Efficiency (EQE) of 6.7% can be achieved, which are improved three-fold compared to the CsPbBr3 QLEDs without the TOPO layer. Our work suggests that the micro grid structures of the TOPO layer provide a novel and facile way to enhance the performance of the perovskite QLEDs.
研究领域:
材料科学
·
光电子学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2018
·
IF 3.789
Pan Sun,Kun Huang,Huizhou Liu
Understanding the essence of the specific salt effect on the enhancement of the transport of metal ions across the liquid/liquid interface during the process of solvent extraction is of crucial importance for the development of a new approach to extract and selectively separate various valuable metals from complex aqueous solutions. However, some abnormal experimental phenomena involved in the salt effect on the liquid/liquid solvent extraction could not be understood only from the conventional interpretation based on the salting-out ability of salt ions. The knowledge into the microscopic mechanism behind the specific salt effect was urgent. Herein, as an example, the effect of adding various salts on the extraction performance of rare earth ion Pr3+ using trioctylphosphine oxide (TOPO) as the organic extractant was investigated. It was revealed that the difference in the interface propensity of different salt anions enriched at the organic–aqueous two-phase interface played a crucial role in promoting the interaction of TOPO molecules with Pr3+ ions, despite the occurrence of the salting-out effect of those salt anions with the increase of their concentrations in aqueous solutions. The interfacial interaction mechanism obtained by molecular dynamics simulations revealed that both the interface propensity and the salting-out ability of the coexisting salt anions contributed to the enhancement in the extraction of Pr3+ into the TOPO organic phase. However, when the concentrations of coexisting salts in aqueous solutions were low enough, the extraction of Pr3+ was mainly dominated by the interface propensity of those added salt anions but not their salting-out ability. With the increase in the concentration of salts, the salting-out effect gradually became significant and, therefore, began to join with the interface propensity of salt anions to co-dominate the transport of Pr3+ ions across the liquid/liquid interface. The present study highlights the microscopic nature of the salt effect on promoting the extraction of rare earth ions and suggests that the interaction of organic extractant molecules with rare earth ions at liquid/liquid interface was dependent not only upon the salting-out ability of the coexisting salt ions but also their interface propensity.
研究领域:
化学
·
材料科学
·
环境科学
·
物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Optical Materials
·
2021
·Vol. 10
·期 3
·2102074
·
IF 9.926
Zi Chen,Dongdong Lu,Hangqing Xie,Xiaolei Yang,Yang Li,Chenhao Bao,Lei Lei,Shiqing Xu
The increasing demand for radiation detection in many applications has led to demanding requirements for scintillators. Realizing low-dose, pollution-free, and reliable X-ray detection has become a key technical challenge. Here, a triplet-enhanced lanthanide radioluminescence (RL) material Ga 3+ /Tb 3+ metallacrowns (Tb-1) is reported. This Tb-1 crystal emits bright green luminescence under ultraviolet light or X-ray excitation, and the emission intensity is 286 and 242 times that of Tb 3+ in inorganic salt, respectively. Tb-1 crystal is further passivated by trioctylphosphine oxide (TOPO), and the enhanced RL intensity is equivalent to that of commercial Tl-doped cesium iodide scintillator. In addition, RL of Tb-1–TOPO has an extremely narrow full width at half maximum and an excellent linear response to the X-ray dose rate. The detection limit is calculated to be 0.146 μGy s −1 , which is 38 times lower than typical medical imaging doses. Triplet-enhanced lanthanide RL provides new ideas for replacing scintillators that require high temperature synthesis processes such as inorganic phosphors and ceramics, and provides a new alternative scintillator material for flexible X-ray monitoring, bioimaging, radiotherapy, and other applications.
研究领域:
辐射检测
·
材料科学
·
医学成像
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lei-Tao Sha,Qiang Wu,Yi-Fan Zhang,Wei-Jia Wang,Fei Wu,Qing-Gang Huang,Ze-Yi Yan
The hydrophobic deep eutectic solvents (HDES) with low viscosity, density and environmental friendliness have been prepared and characterized based on trioctylphosphine oxide (TOPO) and N,N -dihexyl succinamic acid (DHSCA), which were used as both extractant and organic phase for highly efficient removal of radioactive elements of U(VI) and Th(IV) from rare earth (RE) leaching solution. The extraction efficiency of U(VI) and Th(IV) exceeded 99 % by a single stage extraction. Benefiting from the blocking effect of hydrogen bonding on P = O and the good affinity of DHSCA and TOPO for actinides, the present HDES exhibited the excellent extraction selectivity for U(VI) and Th(IV) over Fe(III), Al(III), Mg(II), Ca(II) and RE(III). Even after seven extraction-stripping cycles, the prepared HDES could still effectively remove radioactive U(VI) and Th(IV) from RE leaching solution. The co-extracted U(VI) and Th(IV) was further separated and enriched by two successive stripping steps. Using the slope analysis, 31 P NMR and FT-IR spectra, the stoichiometry of extracted species and the extraction mechanism of HDES to Th(IV) and U(VI) were evaluated. Due to the superior extraction efficiency, excellent environmental compatibility and sustainability, the present approach offers a practical alternative for removal of radioactive elements from rare earth minerals.
研究领域:
化学工程
·
环境科学
·
核化学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）