ACS Sustainable Chemistry & Engineering
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2023
·
IF 8.4
Shiyao Lu,Jian Zhang,Hao Meng,Xiaoyuan Qin,Jianbin Huang,Yehao Liang,Feng-Shou Xiao
Dehydration of methyl lactate (ML) obtained from biomass is a sustainable route for the production of methyl acrylate (MA). Herein, we demonstrate that cesium-exchanged Al-rich Beta zeolite (Cs-Beta) is highly efficient for the dehydration of ML to MA, exhibiting full ML conversion with 87.4% MA yield at 340 °C. In situ FT-IR spectra and kinetic studies provide evidence that the ML dehydration on the Cs-Beta zeolite follows a forward ion-exchange/dehydration/reverse ion-exchange reaction pathway. Model experiments, DFT calculations, TG-DSC analysis, and FT-IR spectra showed that coke formation competes with the dehydration of ML to MA. Kinetic studies and theoretical simulations demonstrate that cesium cations in the micropores of Beta zeolite have a strong steric hindrance, suppressing the formation of oligomers and coke. These results offer new insights for developing highly selective and stable catalysts for the dehydration of ML to MA in the future.
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HYDROMETALLURGY
·
2022
·
IF 4.217
Wanlei Geng,Debin Wang,Yinfeng Liu,Jialing Zhang,Limei Zhong,Runxiong Lin,Li Ding,Lianying Wu,Dianquan Dong
Developing a stable and efficient adsorbent to recover Cs + from liquid resources or to remove radioactive Cs + from wastewater is challenging. In this study, the precursor Cs 2 Ti 6 O 13 (CTO) was synthesized by the solvothermal and solid-phase sintering methods for the first time, then it was acid-modified to synthesize a novel H-type titanium-based material (H-CTO nanosheets). A series of batch adsorption experiments was carried out. The adsorption of Cs + on H-CTO was evaluated under different experimental conditions, including contact time, temperature, initial Cs + concentration, pH, and interfering ions. Experiments show that H-CTO exhibits a larger adsorption capacity (329 mg/g) and better cycle performance than the currently reported titanium-based adsorbents. The cesium ions were easily eluted by the 0.2 M HCl solution; the adsorption capacity did not decrease significantly after five cycles. Furthermore, the adsorption behavior of Cs + on H-CTO can be described by the Langmuir isotherm and pseudo-second-order kinetic models. Characterization using IR and Raman spectroscopic analyses indicates that the adsorption mechanism of Cs + on H-CTO involves O H bond cleavage and O Cs bond formation. Thermodynamic studies showed that low temperatures are favorable for Cs + adsorption and are spontaneous. Overall, the results suggest that H-CTO nanosheets are promising for the recovery or removal of Cs + ions from Cs-containing liquid ores or radioactive wastewater .
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Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-12
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IF 26.6
Zhou Bo,Du Aixuan,Ding Dong,Liu Zexiang,Wang Ye,Zhong Haizhe,Li Henan,Hu Hanlin,Shi Yumeng
Abstract Single materials that exhibit efficient and stable white-light emission are highly desirable for lighting applications. This paper reports a novel zero-dimensional perovskite, Rb 4 CdCl 6 :Sn 2 + , Mn 2 + , which demonstrates exceptional white-light properties including adjustable correlated color temperature, high color rendering index of up to 85, and near-unity photoluminescence quantum yield of 99%. Using a co-doping strategy involving Sn 2+ and Mn 2+ , cyan-orange dual-band emission with complementary spectral ranges is activated by the self-trapped excitons and d-d transitions of the Sn 2+ and Mn 2+ centers in the Rb 4 CdCl 6 host, respectively. Intriguingly, although Mn 2+ ions doped in Rb 4 CdCl 6 are difficult to excite, efficient Mn 2+ emission can be realized through an ultra-high-efficient energy transfer between Sn 2+ and Mn 2+ via the formation of adjacent exchange-coupled Sn–Mn pairs. Benefiting from this efficient Dexter energy transfer process, the dual emission shares the same optimal excitation wavelengths of the Sn 2+ centers and suppresses the non-radiative vibration relaxation significantly. Moreover, the relative intensities of the dual-emission components can be modulated flexibly by adjusting the fraction of the Sn 2+ ions to the Sn–Mn pairs. This co-doping approach involving short-range energy transfer represents a promising avenue for achieving high-quality white light within a single material.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 32
·11010-11016
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IF 6.4
Fan Chen,Xiao-Jun Wang,Wenhao Bai,Xuehu Zhang,Wen Hao,Changhua Zhang,Tongtong Xuan
Zero-dimensional (0D) lead-free halide perovskites are emerging as promising light-emitters, which can be applied as light conversion materials for illumination and display. Herein, we prepared a series of Sb3+:Rb2InCl5·H2O perovskites by a simple and efficient coprecipitation method. The Rb2InCl5·H2O perovskite gives no emission due to the parity-forbidden transition. When Sb3+ is doped into Rb2InCl5·H2O, radiative transition occurs. Under 365 nm excitation, the Sb3+:Rb2InCl5·H2O perovskites show an intense orange-red emission peak at 615 nm, ascribed to the 3P1 to 1S0 transition of Sb3+. The brightest luminescence of Sb3+:Rb2InCl5·H2O was achieved by doping 40%Sb3+, with a high photoluminescence quantum yield (PLQY) of 62.1% and an external quantum efficiency (EQE) of 30.2%. Furthermore, the prepared Sb3+:Rb2InCl5·H2O perovskite exhibits a distinguished thermal stability. At 150 °C, its PL intensity remains 68% of that measured at room temperature, with a high thermal activation energy of 0.184 eV. By combining Sb3+:Rb2InCl5·H2O with a blue-emitting Eu2+:BaMgAl10O17 (Eu2+:BAM) phosphor, bright warm-white light with a color rendering index of 88 and a correlated color temperature of 3242 K was achieved. To sum up, the prepared Sb3+:Rb2InCl5·H2O orange-red perovskites have the advantages of suitable excitation and emission peak positions, high emission intensity, high PLQY and EQE, excellent stability, and environmental friendliness, making them very attractive in the field of lighting and displays.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Yating Kan,Chenhua Han,Ying Ye,Xiao Zhang,Yuanfeng Huang,Liang Xing,Yifan Zhou,Huawei Qin
An all-solid-state ammonium ion-selective electrode, with silver/nano-silver wire as the substrate, polyaniline as transducer and poly (o-phenylenediamine) as sensitive membrane, is presented. The nano-silver was prepared by electrodeposition in 0.1 M AgNO 3 standard solution with the half-sine wave at amplitude of 500 mV, frequency of 50 HZ and action time of 1 min. The polyaniline and poly (o-phenylenediamine) were electropolymerized on the surface of the silver/nano-silver substrate by cyclic voltammetry with the scanning potential from 0 to 0.45 V in solutions of 1.0 M aniline hydrochloride and 0.08 M o-phenylenediamine hydrochloride, respectively. Under the SEM, poly (o-phenylenediamine) with 0.5-5 μm in size was evenly and firmly embedded on the surface of the PANI. This ammonium electrode exhibited low impedance of approximately 70 Ohm. It can detect as low as 1.2×10 -5 M of ammonium ion, with the slopes of 54.99-55.70 mV per decade (R 2 >0.99) within a linear range between 2×10 -5 M to 0.1 M. It responds as quickly as 0.5-2 s, as well as its lifespan extends to at least 147 days. The electrode showed a superior selectivity toward NH 4 + , and was successfully applied to detect the NH 4 + concentration in real samples. In addition, this electrode is miniature and convenient for package and assembly, which will enable in-situ measurement and long-term monitoring of NH 4 + concentration in rivers, lakes and industrial sewage.
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CHEMISTRY OF MATERIALS
·
2023
·
IF 8.6
Mengran Sun,Wenhao Xing,Shyong K. Chen,Chunxiao Li,Wenhao Liu,Ming-Hsien Lee,Jiyong Yao
Chalcogenides are promising candidates for exploring mid- and far-infrared nonlinear optical (NLO) materials. Nevertheless, although tellurides possess greater advantages in the above-mentioned spectral regions, the reports on telluride NLO materials are far fewer than those on sulfides and selenides. In this work, a new quaternary NLO-active telluride, KCd4Ga5Te12, was discovered, and its Rb and Cs analogues were successfully synthesized. They are crystallized in the trigonal R3 space group and the structure features a 3D diamond-like framework constructed by vertex-sharing asymmetric MTe4 tetrahedra (centered by disordered Cd and Ga) that are stacked along the c-axis. Moreover, a comprehensive study of their IR NLO properties, photoluminescence properties, and structural features was performed. These compounds exhibited large powder second-harmonic generation (SHG) intensities, about 2.1 (2.7, 4.4) times that of AgGaSe2 in the particle size range of 20–50 (125–150) μm and a wide transmission range (∼25 μm). The SHG-density analysis revealed that the largest component χ333(2) of KCd4Ga5Te12 originates from three types of Te in the crystal structure. More importantly, it is rare in literature to demonstrate the consistency of linear and NLO properties calculated using both ultrasoft pseudopotentials and norm-conservation pseudopotentials. Besides, the title compounds also exhibit strong luminescence emissions around 420 and 470 nm at 298 K. This work implies that title compounds are promising candidates in the IR NLO applications.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 47
·2305858
·
IF 19
Shuangyi Zhao,Zhenglin Jia,Yian Huang,Qingkai Qian,Qianqian Lin,Zhigang Zang
Lead-free metal halides have recently received sustained attention because of their nontoxicity, low-cost, as well as excellent stability and optoelectronic properties. However, most of the reported lead-free metal halides are synthesized via slow solution-processing at high temperature in toxic solvents, which may impede their commercial applications. Here, a solvent-free strategy is proposed to synthesize inorganic rubidium copper halides (Rb 2 CuX 3 , X = Cl, Br) at room temperature, which exhibit efficient violet emission dominated by a self-trapped excitons (STEs) mechanism and attractive stabilities against ultraviolet illumination and heating. Thus, Rb 2 CuX 3 powders are employed as emitters and scintillators applied in wireless light communication and X-ray imaging technologies. Under orthogonal frequency division multiplexing modulation, emitters demonstrate a broad −3 dB bandwidth of 26.3 MHz and a high received data rate of 205.1 Mbps. Additionally, flexible scintillation films based on as-prepared powders are fabricated and show outstanding X-ray scintillation properties, including a high spatial resolution of 18.1 lp mm −1 and a low detection limit of 104 nGy air s −1 , as well as promising imaging performance for irregular objects. These results suggest large-scale production of nontoxic Rb 2 CuX 3 and their potential commercialization in fields of high-speed light communication and X-ray radiography.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 39
·15067-15073
·
IF 4.569
Yi Huang,Junben Huang,Yong Zhang
Metal thiophosphates have aroused much research interest due to their structural chemistry and possible applications as infrared functional materials. In this study, five quaternary Sr-based alkali metal thiophosphates ASrPS4 (A = Li, Na, K, Rb, Cs) were obtained. Their structural comparison shows that their symmetry undergoes transformation from tetragonal (I41/acd) to monoclinic (P21/c) to orthorhombic (Pnma) system, which is induced by the cation size effects and coordination features of different alkali metal cations. The experimental and theoretical results demonstrate that the band gaps of all title compounds are large, namely 3.6–3.9 eV (experimental results) and 3.78–4.12 eV (HSE06). Theoretical analyses indicate that the [PS4] group could be regarded as a good unit for designing wide band gap compounds, and the birefringence of NaSrPS4 is 0.08 at the fundemental 1064 nm wavelength, which shows that it may be a potential infrared birefringent material.
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Materials
·
2022
·Vol. 15
·期 18
·6411
·
IF 3.748
Zhangyang Kang,Maogang He,Guangxuan Lu
In this study, the phase diagram of the NaCl+RbCl binary system was measured using differential scanning calorimetry, and the measured molar percentages of the binary mixture RbCl ranged from 12 to 97 mol%, updating and extending the experimental data for this binary system. The liquid phase of this system was thermodynamically modeled using a modified quasichemical model, and a computer optimization program for evaluation of the experimental data on phase equilibria and other thermodynamic data was developed based on this model. All thermodynamic models of the NaCl+RbCl binary system were constructed; calculations of the phase diagram, enthalpy of mixing, and activity coefficient of NaCl of the NaCl+RbCl binary system were completed using the obtained model parameters; and the calculated eutectic point positions werexRbCl= 0.567 and 550.2 °C. The calculated results were able to reproduce the various types of experimental data well, and the thermodynamic self-consistency between different types of experimental data was demonstrated.Keywords:differential scanning calorimetry;modified quasichemical model;phase diagram;thermodynamics;phase equilibria;activity coefficient
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Xinyu Shi,Zhilin Li,Mengyan Cao,Zhihui Rao,Xiujian Zhao,Xiao Gong
Due to the toxicity and instability issues of lead halide perovskites, lead-free perovskites have recently emerged as a viable alternative. However, significant optical band gaps of lead-free perovskites exert influence on their luminescent properties. Fortunately, the addition of dopants becomes an efficacious solution. The current widely utilized methods for synthesizing perovskites almost require high temperatures, a long period, and atmosphere protection, which cost more energy and resources. In this paper, we report that Rb2ZrCl6:xSb3+ perovskite phosphors can be easily prepared by a wet grinding approach at room temperature, which is a more efficient and facile process. Due to the self-trapped excitons of the host structure and Sb3+ ions, the produced samples display blue-white and orange fluorescence under UV lamp irradiation at 254 and 365 nm, respectively. In the photoluminescence spectrum, the doped perovskite exhibits an emission peak at 630 nm under excitation at 365 nm. Importantly, the prepared phosphors have tunable emissions related to the excitation wavelength. In addition, our produced powders show remarkable stability at room temperature, laying the foundations for this approach to be widely used in perovskite production.
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JOURNAL OF LUMINESCENCE
·
2022
·
IF 4.171
Fei Zhang,Zhipeng Chen,Zibin Liu,Mochen Jia,Xu Chen,Di Wu,Xinjian Li,Zhifeng Shi
In recent years, the lead-halide perovskite materials have shown great potential in lighting fields due to their excellent photoelectric properties . However, lead toxicity and instability severely limit their practical application and commercial development. In this work, zero-dimensional vacancy-ordered double perovskite Rb 2 ZrCl 6 microcrystal was synthesized by hydrothermal method for the first time. The Rb 2 ZrCl 6 microcrystals exhibit a blue-white light emission with high photoluminescence quantum yield of 60% and a large Stokes shift. The Rb 2 ZrCl 6 has a high exciton binding energy and a strong electron-phonon coupling, which supports the formation of self-trapped excitons under light excitation and the generation of broadband emission. In addition, the Rb 2 ZrCl 6 microcrystals show a remarkable stability against heat, ultraviolet light and environmental water/oxygen. Afterwards, we used the Rb 2 ZrCl 6 microcrystals as the phosphors to fabricate a white light-emitting diode (WLED). The device demonstrates a color coordinate of (0.30, 0.32), a high color rendering of 90.0, and a good working stability, with no emission degradation over continuous 10 h operation. Together with the eco-friendly features and low-cost solution processability, the nontoxic Rb 2 ZrCl 6 can therefore be deemed as a reliable light emitter for high-performance WLEDs.
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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2022
·
IF 4.966
Ting Xiong,Si-quan Ling,Jia-li Liu,Xin-nian Zeng
The red imported fire ant ( Solenopsis invicta ), a worldwide invasive and polyphagous pest, and often nests in residential areas. Finding an alternative pesticide that is both effective on S. invicta and environmentally friendly is urgent and crucial. Fluralaner, a novel isoxazoline insecticide, has been proven to possess selective toxicity for insects versus mammals and has been safe for mammals and non-target organisms, suggesting its potential in pest management. However, little toxicity information is available for the controlment of S. invicta. In this article, we studied the toxicity of fluralaner against S. invicta systematically, and the roles of metabolism-related enzymes in the metabolism process of fluralaner. The toxicity results showed that the topical application and feeding application were all effective for S. invicta . Moreover, fluralaner can be transmitted among workers by contacting and feeding which leads to a toxic reaction among nestmates. By exploring the biochemistry change, we found cytochrome P450 monooxygenase ( P450 ) may be involved in the detoxification of fluralaner as well as carboxylesterase ( CarE ), but not glutathione S-transferase ( GST ). Synergism assays gave solid evidence in which piperonyl butoxide , an activity inhibitor of P450, increased the toxicity of fluralaner to S. invicta . Importantly, with the RNAi treatment, four of S.invicta P450 genes were significantly inhibited and showed more sensitivity to fluralaner at LC 50 concentration. Our result indicated that fluralaner could be a potential alternative pesticide in S. invicta control . And CYP9AS16 , CYP6AS161 , CYP6SQ20 , and CYP336A45 genes were closely associated with the metabolism process of fluralaner.
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